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Author |
Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials. |
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Wos |
000878324400001 |
Publication Date |
2022-10-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
17 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. |
Approved |
Most recent IF: 17.1 |
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Call Number |
EMAT @ emat @c:irua:191815 |
Serial |
7116 |
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Permanent link to this record |
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Author |
Chen, H.; Xu, J.; Wang, Y.; Wang, D.; Ferrer-Espada, R.; Wang, Y.; Zhou, J.; Pedrazo-Tardajos, A.; Yang, M.; Tan, J.-H.; Yang, X.; Zhang, L.; Sychugov, I.; Chen, S.; Bals, S.; Paulsson, J.; Yang, Z. |
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Title |
Color-switchable nanosilicon fluorescent probes |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
9 |
Pages |
15450-15459 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Fluorescent probes are vital to cell imaging by allowing specific parts of cells to be visualized and quantified. Color-switchable probes (CSPs), with tunable emission wavelength upon contact with specific targets, are particularly powerful because they not only eliminate the need to wash away all unbound probe but also allow for internal controls of probe concentrations, thereby facilitating quantification. Several such CSPs exist and have proven very useful, but not for all key cellular targets. Here we report a pioneering CSP for in situ cell imaging using aldehydefunctionalized silicon nanocrystals (SiNCs) that switch their intrinsic photoluminescence from red to blue quickly when interacting with amino acids in live cells. Though conventional probes often work better in cell-free extracts than in live cells, the SiNCs display the opposite behavior and function well and fast in universal cell lines at 37 ? while requiring much higher temperature in extracts. Furthermore, the SiNCs only disperse in cytoplasm not nucleus, and their fluorescence intensity correlated linearly with the concentration of fed amino acids. We believe these nanosilicon probes will be promising tools to visualize distribution of amino acids and potentially quantify amino acid related processes in live cells. |
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Wos |
000861080700001 |
Publication Date |
2022-09-15 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
1 |
Open Access |
Not_Open_Access |
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Notes |
Z.Y. and H.C. acknowledge the funding support from the National Natural Science Foundation of China (21905316, 22175201) , the Science and Technology Planning Project of Guangdong Province (2019A050510018) , the Pearl River Recruitment Program of Talent (2019QN01C108) , the EU Infrastructure Project EUSMI (Grant No. E190700310) , and Sun Yat-sen University. S.C. acknowledge the funding support from the National Natural Science Foundation of China (32171192) . D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant No. 894254 SuprAtom) . S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of the grant agreement No. 731019 (EUSMI) and the ERC Consolidator Grant No. 815128 (REALNANO) . J.Z. acknowledged the funding support from the China Scholarship Council (CSC) . L.Z and J.X. thank Huzhou Li-in Biotechnology Co., Ltd. for the instrumentational and financial support. J.X. and R.F.-E. appreciate fruitful discussion with Dr. Emanuele Leoncini and Dr. Noah Olsman. J.X. and R.F.-E. also thank Mr. Daniel Eaton and Mr. Carlos Sanchez for their help with microscope setups. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:191574 |
Serial |
7288 |
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Permanent link to this record |
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Author |
Yao, Y.; Ugras, T.J.; Meyer, T.; Dykes, M.; Wang, D.; Arbe, A.; Bals, S.; Kahr, B.; Robinson, R.D. |
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Title |
Extracting pure circular dichroism from hierarchically structured CdS magic cluster films |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
12 |
Pages |
20457-20469 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiroptically active, hierarchically structured materials are difficult to accurately characterize due to linear anisotropic contributions (i.e., linear dichroism (LD) and linear birefringence (LB)) and parasitic ellipticities that produce artifactual circular dichroism (CD) signals, in addition to chiral analyte contributions ranging from molecular-scale clusters to micron-sized assemblies. Recently, we have shown that CdS magic-sized clusters (MSC) can self-assemble into ordered films that have a hierarchical structure spanning seven orders of length-scale. These films have a strong CD response, but the chiral origins are obfuscated by the hierarchical architecture and LDLB contributions. Here, we derive and demonstrate a method for extracting the “pure” CD signal (CD generated by structural dissymmetry) from hierarchical MSC films and identified the chiral origin. The theory behind the method is derived using Mueller matrix and Stokes vector conventions and verified experimentally before being applied to hierarchical MSC and nanoparticle films with varying macroscopic orderings. Each film's extracted “true CD” shares a bisignate profile aligned with the exciton peak, indicating the assemblies adopt a chiral arrangement and form an exciton coupled system. Interestingly, the linearly aligned MSC film possesses one of the highest g-factors (0.05) among semiconducting nanostructures reported. Additionally, we find that films with similar electronic transition dipole alignment can possess greatly different g-factors, indicating chirality change rather than anisotropy is the cause of the difference in the CD signal. The difference in g-factor is controllable via film evaporation geometry. This study provides a simple means to measure “true” CD and presents an example of experimentally understanding chiroptic interactions in hierarchical nanostructures. |
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Wos |
000888219600001 |
Publication Date |
2022-11-17 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
8 |
Open Access |
Not_Open_Access |
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Notes |
This work was supported in part by the National Science Foundation (NSF) under Award Nos. DMR-2003431 and CHE-2003586. This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC program (DMR-1719875). This work is partly supported by Grant PID2021-123438NB-I00 (MCIN/AEI/10.13039/501100011033 and “ERDF vA way of making Europe”) and Grant IT1566-22 (Eusko Jaurlaritza). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon 2020 program (Grant 894254 SuprAtom). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. B.K. acknowledges NSF award DMR-2003968. We would like to thank Dr. Mark August Pfeifer for help with circular dichroism measurements. Additionally, we would like to thank Professor Luis M. Liz-Marzan for invaluable discussions on chirality. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:192070 |
Serial |
7305 |
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Permanent link to this record |
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Author |
Parzyszek, S.; Tessarolo, J.; Pedrazo-Tardajos, A.; Ortuno, A.M.; Baginski, M.; Bals, S.; Clever, G.H.; Lewandowski, W. |
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Title |
Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
11 |
Pages |
18472-18482 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Circularly polarized luminescent (CPL) films with high dissymmetry factors hold great potential for optoelectronic applications. Herei n , we propose a strategy for achieving strongly dissymetric CPL in nanocomposite films based on chira l i t y induction and energy transfer to semiconductor nanocrystals. First, focusing on a purely organic system, aggregation-induced emission (AIE) and CPL activity of organic liquid crystals (LCs) forming helical nanofilaments was detected, featuring green emission with high dissymmetry factors g(lum) similar to 10(-2). The handedness of helical filaments, and thus the sign of CPL, was controlled via minute amounts of a small chiral organic dopant. Second, nanocomposite films were fabricated by incorporating InP/ZnS semi-conductor quantum dots (QDs) into the LC matri x , which induced the chiral assembly of QDs and endowed them with chiroptical properties. Due to the spectral matching of the components, energy transfer (ET) from LC to QDs was possible enabling a convenient way of tuning CPL wavelengths by varying the LC/QD ratio. As obtained, composite films exhibited absolute glum values up to similar to 10(-2) and thermally on/off switchable luminescence. Overall, we demonstrate the induction of chiroptical properties by the assembly of nonchiral building QDs on the chiral organic template and energy transfer from organic films to QDs, representing a simple and versatile approach to tune the CPL activity of organic materials. |
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Wos |
000883943600001 |
Publication Date |
2022-11-07 |
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Abbreviated Series Title |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
W.L., S.P., and M.B. acknowledge support from the National Science Center Poland under the OPUS Grant UMO-2019/35/B/ST5/04488. J.T. and G.H.C. acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy, Grant EXC 2033-390677874-RESOLV. W.L. acknowledges financial support from the European Commission under the Horizon 2020 Programme by Grant E210400529. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by Grant 731019 (EUSMI) and ERC Consolidator Grant 815128 (REALNANO). We thank Elie Benchimol for his help with the CPL measurements. We thank Damian Pociecha for his help in the determination of phase sequences of organic compounds. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:192101 |
Serial |
7345 |
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Permanent link to this record |
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Author |
Chen, B.; Gauquelin, N.; Strkalj, N.; Huang, S.; Halisdemir, U.; Nguyen, M.D.; Jannis, D.; Sarott, M.F.; Eltes, F.; Abel, S.; Spreitzer, M.; Fiebig, M.; Trassin, M.; Fompeyrine, J.; Verbeeck, J.; Huijben, M.; Rijnders, G.; Koster, G. |
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Title |
Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
13 |
Issue |
1 |
Pages |
265 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO<sub>3</sub>/BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize<italic>c</italic>-axis oriented BaTiO<sub>3</sub>layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO<sub>3</sub>single film and conventional BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO<sub>3</sub>as the thickness of BaTiO<sub>3</sub>increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities. |
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Wos |
000741852200073 |
Publication Date |
2022-01-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 823717—ESTEEM3. B.C. is sponsored by Shanghai Sailing Program 21YF1410700. J.V. and N.G. acknowledge funding through the GOA project “Solarpaint” of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from FWO Project G093417N from the Flemish fund for scientific research. M.T., N.S., M.F.S. and M.F. acknowledge the financial support by the EU European Research Council (Advanced Grant 694955—INSEETO). M.T. acknowledges the Swiss National Science Foundation under Project No. 200021-188414. N.S. acknowledges support under the Swiss National Science Foundation under Project No. P2EZP2-199913. M.S. acknowledges funding from Slovenian Research Agency (Grants No. J2-2510, N2-0149 and P2-0091). B.C. acknowledges Prof. C.D.; Prof. F.Y.; Prof. B.T. and Dr. K.J. for valuable discussions.; esteem3reported; esteem3TA |
Approved |
Most recent IF: 16.6 |
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Call Number |
EMAT @ emat @c:irua:185179 |
Serial |
6902 |
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Permanent link to this record |
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Author |
Otero-Martinez, C.; Imran, M.; Schrenker, N.J.; Ye, J.; Ji, K.; Rao, A.; Stranks, S.D.; Hoye, R.L.Z.; Bals, S.; Manna, L.; Perez-Juste, J.; Polavarapu, L. |
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Title |
Fast A-site cation cross-exchange at room temperature : single-to double- and triple-cation halide perovskite nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
61 |
Issue |
34 |
Pages |
e202205617-11 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We report here fast A-site cation cross-exchange between APbX(3) perovskite nanocrystals (NCs) made of different A-cations (Cs (cesium), FA (formamidinium), and MA (methylammonium)) at room temperature. Surprisingly, the A-cation cross-exchange proceeds as fast as the halide (X=Cl, Br, or I) exchange with the help of free A-oleate complexes present in the freshly prepared colloidal perovskite NC solutions. This enabled the preparation of double (MACs, MAFA, CsFA)- and triple (MACsFA)-cation perovskite NCs with an optical band gap that is finely tunable by their A-site composition. The optical spectroscopy together with structural analysis using XRD and atomically resolved high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and integrated differential phase contrast (iDPC) STEM indicates the homogeneous distribution of different cations in the mixed perovskite NC lattice. Unlike halide ions, the A-cations do not phase-segregate under light illumination. |
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Place of Publication |
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Wos |
000823857300001 |
Publication Date |
2022-06-24 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
28 |
Open Access |
OpenAccess |
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Notes |
L.P. acknowledges the support from the Spanish Ministerio de Ciencia e Innovacion through Ramon y Cajal grant (RYC2018-026103-I) and the Spanish State Research Agency (Grant No. PID2020-117371RA-I00), the grant from the Xunta de Galicia (ED431F2021/05). N.J.S. acknowledges financial support from the Research Foundation-Flanders via a postdoctoral fellowship (FWO Grant No. 1238622N). S.B. thanks the financial support of the European Research Council (ERC-CoG-2019815128) and of the European Commission (EUSMI, Grant 731019). R.L.Z.H. thanks the Royal Academy of Engineering through the Research Fellowships scheme (No.: RF\201718\1701). S.D.S. and K.J. acknowledge the Royal Society for funding. S.D.S. acknowledges the Royal Society and Tata Group (UF150033). The work has received funding from the European Research Council under the European Union's Horizon 2020 research and innovation programme (HYPERION -grant agreement no. 756962). The authors acknowledge the Engineering and Physical Sciences Research Council (EPSRC) for funding (EP/R023980/1). M.I. and L.M. acknowledge financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for Self-Powered Gas Sensors” (PeroGaS). The authors acknowledge the Universidade de Vigo/CISUG for open access funding. |
Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:189675 |
Serial |
7083 |
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Permanent link to this record |
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Author |
Toso, S.; Imran, M.; Mugnaioli, E.; Moliterni, A.; Caliandro, R.; Schrenker, N.J.; Pianetti, A.; Zito, J.; Zaccaria, F.; Wu, Y.; Gemmi, M.; Giannini, C.; Brovelli, S.; Infante, I.; Bals, S.; Manna, L. |
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Title |
Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
13 |
Issue |
1 |
Pages |
3976-10 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2. |
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Wos |
000825867200003 |
Publication Date |
2022-07-08 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
15 |
Open Access |
OpenAccess |
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Notes |
The authors would like to acknowledge Dr. Joka Buha for the help with preliminary tests preceding this project, and Dr. B. M. Aresta and Dr. L. Cassano for their administrative support. The authors acknowledge financial support from the Research Foundation Flanders (FWO) through a postdoctoral fellowship to N.J.S. (FWO Grant No. 1238622N, N.J.S). S.B. acknowledges financial support from the European Commission by ERC Consolidator grant REALNANO (No. 815128, S.B.). L.M. acknowledges financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for SelfPowered Gas Sensors” (PeroGaS, L.M.). The access to the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC0298CH10886 (NSLS-II Proposal Number 307441). |
Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:189684 |
Serial |
7085 |
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Permanent link to this record |
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Author |
Wang, D.; Hermes, M.; Najmr, S.; Tasios, N.; Grau-Carbonell, A.; Liu, Y.; Bals, S.; Dijkstra, M.; Murray, C.B.; van Blaaderen, A. |
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Title |
Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
13 |
Issue |
1 |
Pages |
6001-6012 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000867312100031 |
Publication Date |
2022-10-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
|
|
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
7 |
Open Access |
OpenAccess |
|
|
Notes |
We thank A. Kadu, M. Chiappini, F. Rabouw, S. Paliwal, X. Xie, C. Xia and Z. Wang for fruitful discussions. D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Y.L. acknowledges the Sustainability project between the faculties of Science and Geosciences of Utrecht University. M.D. acknowledges financial support from European Research Council (Grant No. ERC-2019-ADV-H2020 884902 SoftML). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. C.B.M. acknowledges support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge the EM square center at Utrecht University for the access to the microscopes. |
Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:191387 |
Serial |
7214 |
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Permanent link to this record |
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Author |
Cai, J.; Griffin, E.; Guarochico-Moreira, V.H.; Barry, D.; Xin, B.; Yagmurcukardes, M.; Zhang, S.; Geim, A.K.; Peeters, F.M.; Lozada-Hidalgo, M. |
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Title |
Wien effect in interfacial water dissociation through proton-permeable graphene electrodes |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
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Volume |
13 |
Issue |
1 |
Pages |
5776-5777 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Strong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 10(7) V m(-1), sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O reversible arrow H+ + OH-) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 10(8) V m(-1). The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager's theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000862552600012 |
Publication Date |
2022-10-01 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
14 |
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:191575 |
Serial |
7228 |
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Permanent link to this record |
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Author |
Zhou, Z.; Tan, Y.; Yang, Q.; Bera, A.; Xiong, Z.; Yagmurcukardes, M.; Kim, M.; Zou, Y.; Wang, G.; Mishchenko, A.; Timokhin, I.; Wang, C.; Wang, H.; Yang, C.; Lu, Y.; Boya, R.; Liao, H.; Haigh, S.; Liu, H.; Peeters, F.M.; Li, Y.; Geim, A.K.; Hu, S. |
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Title |
Gas permeation through graphdiyne-based nanoporous membranes |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
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Volume |
13 |
Issue |
1 |
Pages |
4031-4036 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeance. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of similar to 0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000918423100001 |
Publication Date |
2022-07-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
|
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ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
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Impact Factor |
16.6 |
Times cited |
21 |
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:194402 |
Serial |
7308 |
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Permanent link to this record |
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Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
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Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
|
|
Volume |
442 |
Issue |
|
Pages |
136268 |
|
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000797716700002 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit |
Approved |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7052 |
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Permanent link to this record |
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Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
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Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
442 |
Issue |
|
Pages |
136268 |
|
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
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Abstract |
CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000797716700002 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. We also thank R. De Meyer, K. Leyssens and S. Defossé for performing the charcoal characterizations. |
Approved |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7053 |
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Permanent link to this record |
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Author |
Van Alphen, S.; Ahmadi Eshtehardi, H.; O'Modhrain, C.; Bogaerts, J.; Van Poyer, H.; Creel, J.; Delplancke, M.-P.; Snyders, R.; Bogaerts, A. |
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Title |
Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
443 |
Issue |
|
Pages |
136529 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the performance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas temperature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000800010600003 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. |
Approved |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188283 |
Serial |
7057 |
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Permanent link to this record |
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Author |
Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. |
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Title |
Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
450 |
Issue |
|
Pages |
137860 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000830813300004 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. |
Approved |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:189502 |
Serial |
7100 |
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Permanent link to this record |
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Author |
Lang, X.; Ouyang, Y.; Vandewalle, L.A.; Goshayeshi, B.; Chen, S.; Madanikashani, S.; Perreault, P.; Van Geem, K.M.; van Geem, K.M. |
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Title |
Gas-solid hydrodynamics in a stator-rotor vortex chamber reactor |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
446 |
Issue |
5 |
Pages |
137323-12 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
The gas-solid vortex reactor (GSVR) has enormous process intensification potential. However the huge gas consumption can be a serious disadvantage for the GSVR in some applications such as fast pyrolysis. In this work, we demonstrate a recent novel design, where a stator-rotor vortex chamber (STARVOC) is driven by the fluid's kinetic energy, to decouple the solids bed rotation and gas. Gas-solid fluidization by using air and monosized aluminum balls was performed to investigate the hydrodynamics. A constructed fluidization flow regime map for a fixed solids loading of 100 g shows that the bed can only be fluidized for a rotation speed between 200 and 400 RPM. Below 200 RPM, particles settle down on the bottom plate and cannot form a stable bed due to inertia and friction. Above 400 RPM, the bed cannot be fluidized with superficial velocities up to 1.8 m/s (air flow rate of 90 Nm(3)/h). The bed thickness shows some non-uniformities, being smaller at the top of the bed than at the bottom counterpart. However by increasing the air flow rate or rotation speed the axial nonuniformity can be resolved. The bed pressure drop first increases with increasing gas flow rate and then levels off, showing similar characteristics as conventional fluidized beds. Theoretical pressure drops calculated from mathematical models such as Kao et al. model agree well with experimental measurements. Particle velocity discrepancies between the top and bottom particles reveal that the impact of gravity cannot be completely neglected. Design guidelines and possible applications for further development of STARVOC concept are proposed based on fundamental data provided in this work. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000833418100006 |
Publication Date |
2022-06-01 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 15.1 |
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Call Number |
UA @ admin @ c:irua:189283 |
Serial |
7167 |
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Permanent link to this record |
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Author |
Ying, J.; Lenaerts, S.; Symes, M.D.; Yang, X.-Y. |
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Title |
Hierarchical design in nanoporous metals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Advanced Science |
Abbreviated Journal |
Adv Sci |
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Volume |
9 |
Issue |
27 |
Pages |
2106117-2106120 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Hierarchically porous metals possess intriguing high accessibility of matter molecules and unique continuous metallic frameworks, as well as a high level of exposed active atoms. High rates of diffusion and fast energy transfer have been important and challenging goals of hierarchical design and porosity control with nanostructured metals. This review aims to summarize recent important progress toward the development of hierarchically porous metals, with special emphasis on synthetic strategies, hierarchical design in structure-function and corresponding applications. The current challenges and future prospects in this field are also discussed. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000831201000001 |
Publication Date |
2022-07-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2198-3844 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 15.1 |
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Call Number |
UA @ admin @ c:irua:189646 |
Serial |
7170 |
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Permanent link to this record |
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|
Author |
Brienza, F.; Van Aelst, K.; Devred, F.; Magnin, D.; Tschulkow, M.; Nimmegeers, P.; Van Passel, S.; Sels, B.F.; Gerin, P.; Debecker, D.P.; Cybulska, I. |
|
|
Title |
Unleashing lignin potential through the dithionite-assisted organosolv fractionation of lignocellulosic biomass |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
|
|
Volume |
450 |
Issue |
3 |
Pages |
138179-14 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
|
|
Abstract |
The development of biomass pretreatment approaches that, next to (hemi)cellulose valorization, aim at the conversion of lignin to chemicals is essential for the long-term success of a biorefinery. Herein, we discuss a dithionite-assisted organosolv fractionation (DAOF) of lignocellulose in n-butanol and water to produce cellulosic pulp and mono-/oligo-aromatics. The study frames the technicalities of this biorefinery process and relates them to the features of the obtained product streams. We comprehensively identify and quantify all products of interest: solid pulp (acid hydrolysis-HPLC, ATR-FTIR, XRD, SEM, enzymatic hydrolysis-HPLC), lignin derivatives (GPC, GC-MS/FID, 1H-13C HSQC NMR, ICP-AES), and carbohydrate derivatives (HPLC). These results were used for inspecting the economic feasibility of DAOF. In the best process configuration, a high yield of monophenolics was reached (~20%, based on acid insoluble lignin in birch sawdust). Various other lignocellulosic feedstocks were also explored, showing that DAOF is particularly effective on hardwood and herbaceous biomass. Overall, this study demonstrates that DAOF is a viable fractionation method for the sustainable upgrading of lignocellulosic biomass. |
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Address |
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Corporate Author |
|
Thesis |
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Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000888204900005 |
Publication Date |
2022-07-20 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
1385-8947; 1873-3212 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 15.1 |
|
|
Call Number |
UA @ admin @ c:irua:189322 |
Serial |
7373 |
|
Permanent link to this record |
|
|
|
|
Author |
Lopez-Garcia, C.; Canossa, S.; Hadermann, J.; Gorni, G.; Oropeza, F.E.; de la Pena O'Shea, V.A.; Iglesias, M.; Monge, M.A.; Gutierrez-Puebla, E.; Gandara, F. |
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|
Title |
Heterometallic molecular complexes act as messenger building units to encode desired metal-atom combinations to multivariate metal-organic frameworks |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
|
|
Volume |
144 |
Issue |
36 |
Pages |
16262-16266 |
|
|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
|
Abstract |
A novel synthetic approach is described for the targeted preparation of multivariate metal-organic frameworks (MTV-MOFs) with specific combinations of metal elements. This methodology is based on the use of molecular complexes that already comprise desired metal-atom combinations, as building units for the MTV-MOF synthesis. These units are transformed into the MOF structural constituents through a ligand/linker exchange process that involves structural modifications while preserving their origina l l y encoded atomic combination. Thus, through the use of heterometalli c ring-shaped molecules combining gallium and nickel or cobalt, we have obtained MOFs with identical combinations of the metal elements, now incorporated in the rod-shaped secondary building unit, as confirmed with a combination of X-ray and electron diffraction, electron microscopy, and X-ray absorption spectroscopy techniques. |
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Address |
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Corporate Author |
|
Thesis |
|
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Publisher |
|
Place of Publication |
|
Editor |
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|
|
Language |
|
Wos |
000841435900001 |
Publication Date |
2022-08-12 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0002-7863 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
15 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 15 |
|
|
Call Number |
UA @ admin @ c:irua:190023 |
Serial |
7169 |
|
Permanent link to this record |
|
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|
|
Author |
Watanabe, Y.; Hyeon-Deuk, K.; Yamamoto, T.; Yabuuchi, M.; Karakulina, O.M.; Noda, Y.; Kurihara, T.; Chang, I.-Y.; Higashi, M.; Tomita, O.; Tassel, C.; Kato, D.; Xia, J.; Goto, T.; Brown, C.M.; Shimoyama, Y.; Ogiwara, N.; Hadermann, J.; Abakumov, A.M.; Uchida, S.; Abe, R.; Kageyama, H. |
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Title |
Polyoxocationic antimony oxide cluster with acidic protons |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Science Advances |
Abbreviated Journal |
|
|
|
Volume |
8 |
Issue |
24 |
Pages |
eabm5379-8 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
|
Abstract |
The success and continued expansion of research on metal-oxo clusters owe largely to their structural richness and wide range of functions. However, while most of them known to date are negatively charged polyoxometalates, there is only a handful of cationic ones, much less functional ones. Here, we show an all-inorganic hydroxyiodide [H(10.)7Sb(32.1)O(44)][H2.1Sb2.1I8O6][Sb0.76I6](2)center dot 25H(2)O (HSbOI), forming a face-centered cubic structure with cationic Sb32O44 clusters and two types of anionic clusters in its interstitial spaces. Although it is submicrometer in size, electron diffraction tomography of HSbOI allowed the construction of the initial structural model, followed by powder Rietveld refinement to reach the final structure. The cationic cluster is characterized by the presence of acidic protons on its surface due to substantial Sb3+ deficiencies, which enables HSbOI to serve as an excellent solid acid catalyst. These results open up a frontier for the exploration and functionalization of cationic metal-oxo clusters containing heavy main group elements. |
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Address |
|
|
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Corporate Author |
|
Thesis |
|
|
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Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000812533800008 |
Publication Date |
2022-06-17 |
|
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2375-2548 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
13.6 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 13.6 |
|
|
Call Number |
UA @ admin @ c:irua:189689 |
Serial |
7091 |
|
Permanent link to this record |
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Author |
Marchetti, A.; Beltran, V.; Nuyts, G.; Borondics, F.; De Meyer, S.; Van Bos, M.; Jaroszewicz, J.; Otten, E.; Debulpaep, M.; De Wael, K. |
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Title |
Novel optical photothermal infrared (O-PTIR) spectroscopy for the noninvasive characterization of heritage glass-metal objects |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Science Advances |
Abbreviated Journal |
|
|
|
Volume |
8 |
Issue |
9 |
Pages |
eabl6769-9 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab); Antwerp X-ray Imaging and Spectroscopy (AXIS) |
|
|
Abstract |
Optical photothermal infrared (O-PTIR) is a recently developed molecular spectroscopy technique that allows to noninvasively obtain chemical information on organic and inorganic samples at a submicrometric scale. The high spatial resolution (approximate to 450 nm), lack of sample preparation, and comparability of the spectral results to traditional Fourier transform infrared spectroscopy make it a promising candidate for the analysis of cultural heritage. In this work, the potential of O-PTIR for the noninvasive characterization of small heritage objects (few cubic centimeters) is demonstrated on a series of degraded 16th century brass and glass decorative elements. These small and challenging samples, typically encountering limitations with existing noninvasive methods such as macroscopic x-ray powder diffraction and mu Raman, were successfully characterized by O-PTIR, ultimately identifying the markers of glass-induced metal corrosion processes. The results clearly demonstrate how O-PTIR can be easily implemented in a noninvasive multianalytical strategy for the study of heritage materials, making it a fundamental tool for cultural heritage analyses. |
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Address |
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Corporate Author |
|
Thesis |
|
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Publisher |
|
Place of Publication |
|
Editor |
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|
Language |
|
Wos |
000790020300013 |
Publication Date |
2022-03-04 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2375-2548 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
13.6 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 13.6 |
|
|
Call Number |
UA @ admin @ c:irua:188642 |
Serial |
7184 |
|
Permanent link to this record |
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Author |
De Keyser, N.; Broers, F.; Vanmeert, F.; De Meyer, S.; Gabrieli, F.; Hermens, E.; van der Snickt, G.; Janssens, K.; Keune, K. |
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|
Title |
Reviving degraded colors of yellow flowers in 17th century still life paintings with macro- and microscale chemical imaging |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Science Advances |
Abbreviated Journal |
|
|
|
Volume |
8 |
Issue |
23 |
Pages |
1-12 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Art; Antwerp Cultural Heritage Sciences (ARCHES); Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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|
Abstract |
Over time, artist pigments are prone to degradation, which can decrease the readability of the artwork or notably change the artist's intention. In this article, the visual implication of secondary degradation products in a degraded yellow rose in a still life painting by A. Mignon is discussed as a case study. A multimodal combination of chemical and optical imaging techniques, including noninvasive macroscopic x-ray powder diffraction (MA-XRPD) and macroscopic x-ray fluorescence imaging, allowed us to gain a 3D understanding of the transformation of the original intended appearance of the rose into its current degraded state. MA-XRPD enabled us to precisely correlate in situ formed products with what is optically visible on the surface and demonstrated that the precipitated lead arsenates and arsenolite from the yellow pigment orpiment and the light-induced fading of an organic yellow lake irreversibly changed the artist's intentional light-shadow modeling. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
|
Editor |
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|
Language |
|
Wos |
000811556500011 |
Publication Date |
2022-06-08 |
|
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2375-2548 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
13.6 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 13.6 |
|
|
Call Number |
UA @ admin @ c:irua:189657 |
Serial |
7205 |
|
Permanent link to this record |
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Author |
Thomassen, G.; Dewulf, J.; Van Passel, S. |
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Title |
Prospective material and substance flow analysis of the end-of-life phase of crystalline silicon-based PV modules |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Resources Conservation And Recycling |
Abbreviated Journal |
Resour Conserv Recy |
|
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Volume |
176 |
Issue |
|
Pages |
105917 |
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|
Keywords |
A1 Journal article; Engineering Management (ENM) |
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|
Abstract |
The approaching end-of life phase of early installed PV modules gave rise to a variety of potential end-of-life strategies, ranging from basic generic waste management strategies to advanced case-specific recycling options. However, no comprehensive assessment on the full range of technological possibilities is available and only limited attention was given to the material recovery rates of these different technologies in light of circular economy. In addition, current material recovery rates are indifferent towards the material value and the value of their secondary applications. Based on an extensive literature review, ten end-of-life scenarios with potential learning effects are identified and their material flows are quantified using a combined material and substance flow analysis. Subsequently, material recovery rates from a mass, economic value and embodied energy perspective are calculated, incorporating the differences in secondary applications. The differences in the mass-based recovery rates of the seven end-of-life scenarios that did not have landfill or municipal waste incineration as the main destination were minimal, as 73-79% of the mass was recovered for the best-case learning scenario. For the economic value recovery rate (9-66%) and the embodied energy recovery rate (18-45%), more profound differences were found. The collection rate was identified as most crucial parameter for all end-of-life scenarios, learning scenarios and recycling indicators. The mass-based recovery rate might favor end-of-life scenarios that lead to dissipation of valuable materials in non-functional secondary applications. Additional targets are required to avoid cascading of valuable materials and to avoid the economic cost and environmental burden of virgin materials. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
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Editor |
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Language |
|
Wos |
000708339400003 |
Publication Date |
2021-10-08 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0921-3449 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
13.2 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 13.2 |
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|
Call Number |
UA @ admin @ c:irua:182462 |
Serial |
6939 |
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Permanent link to this record |
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Author |
Spiller, M.; Moretti, M.; De Paepe, J.; Vlaeminck, S.E. |
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Title |
Environmental and economic sustainability of the nitrogen recovery paradigm : evidence from a structured literature review |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Resources, conservation and recycling |
Abbreviated Journal |
Resour Conserv Recy |
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Volume |
184 |
Issue |
|
Pages |
106406-106413 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Our economy drives on reactive nitrogen (Nr); while Nr emissions to the environment surpass the planetary boundary. Increasingly, it is advocated to recover Nr contained in waste streams and to reuse it ‘directly’ in the agri-food chain. Alternatively, Nr in waste streams may be removed as N2 and refixed via the Haber-Bosch process in an ‘indirect’ reuse loop. As a systematic sustainability analysis of ‘direct’ Nr reuse and its comparison to the ‘indirect’ reuse loop is lacking, this structured review aimed to analyze literature determining the environmental and economic sustainability of Nr recovery technologies. Bibliometric records were queried from 2000 to 2020 using Boolean search strings, and manual text coding. In total, 63 studies were selected for the review. Results suggest that ‘direct’ Nr reuse using Nr recovery technologies is the preferred paradigm as the majority of studies concluded that it is sustainable or that it can be sustainable depending on technological assumptions and other scenario variables. Only 17 studies compared the ‘direct’ with the ‘indirect’ Nr reuse route, therefore a system perspective in Nr recovery sustainability assessments should be more widely adopted. Furthermore, Nr reuse should also be analyzed in the context of a ‘new Nr economy’ that relies on decentralized Nr production from renewable energy. It is also recommended that on-par technology readiness level comparisons should be carried out, making use of technology development and technology learning methodologies. Finally, by-products of Nr recovery are important to be accounted for as they are reducing the environmental burdens through avoided impacts. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
|
Wos |
000804938100001 |
Publication Date |
2022-05-18 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0921-3449 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
13.2 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
|
Approved |
Most recent IF: 13.2 |
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Call Number |
UA @ admin @ c:irua:188873 |
Serial |
7156 |
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Permanent link to this record |
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Author |
De Weerdt, L.; De Jaeger, S.; Compernolle, T.; Van Passel, S. |
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Title |
How an incineration tax changes waste management practices among firms |
Type |
A1 Journal Article |
|
Year |
2022 |
Publication |
Resources Conservation And Recycling |
Abbreviated Journal |
Resour Conserv Recy |
|
|
Volume |
180 |
Issue |
|
Pages |
106172 |
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|
Keywords |
A1 Journal Article; Engineering Management (ENM) ; |
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Abstract |
Sustainable management of industrial plastic waste is crucial in the transition to a circular economy. Today, most industrial plastic waste is incinerated, whereas it could be recycled. As a consequence, governments increasingly make use of incineration taxes to improve current waste management practices. This paper presents an econometric panel analysis that studies the effects of an incineration tax on industrial plastic waste in Flanders (Belgium). Not only is this study the first econometric analysis on industrial plastic waste management in which firm heterogeneity is explicitly taken into account by including firm-specific characteristics, but this study also provides policymakers with insights into the effectiveness of an incineration tax to change current waste management practices. Empirical estimates imply that heterogeneous firms generate industrial plastic waste in different ways and that heterogeneous firms reduce their waste generation in different ways after the incineration tax rate increases. The estimates also show that the unique decrease of the incineration tax in 2007, did not change waste management practices. These estimates show that firms do not disinvest or indicate that loss aversion theory, i.e. a preference for avoiding losses over acquiring equivalent gains, might apply to firms that are faced with environmental taxation in a waste management context. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
|
Publication Date |
2022-01-19 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0921-3449 |
ISBN |
|
Additional Links |
|
|
|
Impact Factor |
13.2 |
Times cited |
|
Open Access |
Not_Open_Access |
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|
Notes |
|
Approved |
Most recent IF: 13.2 |
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|
Call Number |
ENM @ enm @ |
Serial |
7256 |
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Permanent link to this record |
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Author |
Nematollahi, P.; Barbiellini, B.; Bansil, A.; Lamoen, D.; Qingying, J.; Mukerjee, S.; Neyts, E.C. |
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Title |
Identification of a Robust and Durable FeN4CxCatalyst for ORR in PEM Fuel Cells and the Role of the Fifth Ligand |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
|
Issue |
|
Pages |
7541-7549 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Although recent studies have advanced the understanding of pyrolyzed
Fe−N−C materials as oxygen reduction reaction (ORR) catalysts, the atomic and
electronic structures of the active sites and their detailed reaction mechanisms still remain unknown. Here, based on first-principles density functional theory (DFT) computations, we discuss the electronic structures of three FeN4 catalytic centers with different local topologies of the surrounding C atoms with a focus on unraveling the mechanism of their ORR activity in acidic electrolytes. Our study brings back a forgotten, synthesized pyridinic Fe−N coordinate to the community’s attention, demonstrating that this catalyst can exhibit excellent activity for promoting direct four-electron ORR through the addition of a fifth ligand such as −NH2, −OH, and −SO4. We also identify sites with good stability properties through the combined use of our DFT calculations and Mössbauer spectroscopy data. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
|
Wos |
000823193100001 |
Publication Date |
2022-06-10 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS full record; WoS citing articles |
|
|
Impact Factor |
12.9 |
Times cited |
|
Open Access |
OpenAccess |
|
|
Notes |
Basic Energy Sciences, DE-FG02-07ER46352 ; Fonds Wetenschappelijk Onderzoek, 1261721N ; Opetus- ja Kulttuuriministeri?; Department of Energy, DE-EE0008416 ; |
Approved |
Most recent IF: 12.9 |
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|
Call Number |
EMAT @ emat @c:irua:189000 |
Serial |
7073 |
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Permanent link to this record |
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Author |
Cui, Z.; Meng, S.; Yi, Y.; Jafarzadeh, A.; Li, S.; Neyts, E.C.; Hao, Y.; Li, L.; Zhang, X.; Wang, X.; Bogaerts, A. |
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Title |
Plasma-catalytic methanol synthesis from CO₂ hydrogenation over a supported Cu cluster catalyst : insights into the reaction mechanism |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
|
|
Volume |
12 |
Issue |
2 |
Pages |
1326-1337 |
|
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma-catalytic CO, hydrogenation for methanol production is gaining increasing interest, but our understanding of its reaction mechanism remains primitive. We present a combined experimental/computational study on plasma-catalytic CO, hydrogenation to CH3OH over a size-selected Cu/gamma-Al2O3 catalyst. Our experiments demonstrate a synergistic effect between the Cu/gamma-Al2O3 catalyst and the CO2/H-2 plasma, achieving a CO2 conversion of 10% at 4 wt % Cu loading and a CH3OH selectivity near 50% further rising to 65% with H2O addition (for a H2O/CO2 ratio of 1). Furthermore, the energy consumption for CH3OH production was more than 20 times lower than with plasma only. We carried out density functional theory calculations over a Cu-13/gamma-Al2O3 model, which reveal that the interfacial sites of the Cu-13 cluster and gamma-Al2O3 support show a bifunctional effect: they not only activate the CO2 molecules but also strongly adsorb key intermediates to promote their hydrogenation further. Reactive plasma species can regulate the catalyst surface reactions via the Eley-Rideal (E-R) mechanism, which accelerates the hydrogenation process and promotes the generation of the key intermediates. H2O can promote the CH3OH desorption by competitive adsorption over the Cu-13/gamma-Al2O3 surface. This study provides new insights into CO2 hydrogenation through plasma catalysis, and it provides inspiration for the conversion of some other small molecules (CH4, N-2, CO, etc.) by plasma catalysis using supported-metal clusters. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
|
Wos |
000742735600001 |
Publication Date |
2022-01-07 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
12.9 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 12.9 |
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Call Number |
UA @ admin @ c:irua:186416 |
Serial |
7192 |
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Permanent link to this record |
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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
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Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
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Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
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Permanent link to this record |
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Author |
De Backer, A.; Zhang, Z.; van den Bos, K.H.W.; Bladt, E.; Sánchez‐Iglesias, A.; Liz‐Marzán, L.M.; Nellist, P.D.; Bals, S.; Van Aert, S. |
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Title |
Element Specific Atom Counting at the Atomic Scale by Combining High Angle Annular Dark Field Scanning Transmission Electron Microscopy and Energy Dispersive X‐ray Spectroscopy |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Small methods |
Abbreviated Journal |
Small Methods |
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Volume |
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Issue |
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Pages |
2200875 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
A new methodology is presented to count the number of atoms in multimetallic nanocrystals by combining energy dispersive X-ray spectroscopy (EDX) and high angle annular dark field scanning transmission electron microscopy (HAADF STEM). For this purpose, the existence of a linear relationship between the incoherent HAADF STEM and EDX images is exploited. Next to the number of atoms for each element in the atomic columns, the method also allows quantification of the error in the obtained number of atoms, which is of importance given the noisy nature of the acquired EDX signals. Using experimental images of an Au@Ag core–shell nanorod, it is demonstrated that 3D structural information can be extracted at the atomic scale. Furthermore, simulated data of an Au@Pt core–shell nanorod show the prospect to characterize heterogeneous nanostructures with adjacent atomic numbers. |
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Place of Publication |
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Wos |
000862072700001 |
Publication Date |
2022-09-30 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2366-9608 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.4 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S.V.A., Grant 815128 REALNANO to S.B., and Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0267.18N, G.0502.18N, G.0346.21N) and a postdoctoral grant to A.D.B.; esteem3reported; esteem3JRA |
Approved |
Most recent IF: 12.4 |
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Call Number |
EMAT @ emat @c:irua:191570 |
Serial |
7109 |
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Permanent link to this record |
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Author |
Van Schoubroeck, S.; Vermeyen, V.; Alaerts, L.; Van Acker, K.; Van Passel, S. |
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Title |
How to monitor the progress towards a circular food economy : a Delphi study |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Sustainable Production and Consumption |
Abbreviated Journal |
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Volume |
32 |
Issue |
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Pages |
457-467 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM) |
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Abstract |
Within the food sector, the implementation of a circular economy (CE) can reduce resource consumption and emissions to the environment by moving away from a linear and unsustainable system. This necessitates a clear vision on what circularity for food means, which will provide a much-needed foundation to develop a mon-itoring tool that reveals insights into the progress being made towards a CE, and to expose the bottlenecks and opportunities. This research study contributes to the development of a shared vision for circularity within the food system, and defines and prioritizes a set of indicator themes to monitor a circular food economy (CFE). A two-round Delphi study was performed, including a brainstorming session with experts and the construction of a consensus ranking of indicator themes, considering the production and processing and the consumption stage. The Delphi results provide a shared vision on a CFE, and a blueprint for researchers and policy-makers on its monitoring, which will stimulate the progression from a linear to a circular system.(c) 2022 Published by Elsevier Ltd on behalf of Institution of Chemical Engineers. |
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Place of Publication |
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Wos |
000806368300009 |
Publication Date |
2022-05-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2352-5509 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 12.1 |
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Call Number |
UA @ admin @ c:irua:189513 |
Serial |
7360 |
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Permanent link to this record |
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Author |
Batuk, M.; Vandemeulebroucke, D.; Ceretti, M.; Paulus, W.; Hadermann, J. |
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Title |
Topotactic redox cycling in SrFeO2.5+δ explored by 3D electron diffraction in different gas atmospheres |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Journal of materials chemistry A : materials for energy and sustainability |
Abbreviated Journal |
J Mater Chem A |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
For oxygen conducting materials applied in solid oxide fuel cells and chemical-looping processes, the understanding of the oxygen diffusion mechanism and the materials’ crystal structure at different stages of the redox reactions is a key parameter to control their performance. In this paper we report the first ever in situ 3D ED experiment in a gas environment and with it uncover the structure evolution of SrFeO2.5 as notably different from that reported from in situ X-ray and in situ neutron powder diffraction studies in gas environments. Using in situ 3D ED on submicron sized single crystals obtained from a high quality monodomain SrFeO2.5 single crystal , we observe the transformation under O2 flow of SrFeO2.5 with an intra- and interlayer ordering of the left and right twisted (FeO4) tetrahedral chains (space group Pcmb) into consecutively SrFeO2.75 with space group Cmmm (at 350°C, 33% O2) and SrFeO3-δ with space group Pm3 ̅m (at 400°C, 100% O2). Upon reduction in H2 flow, the crystals return to the brownmillerite structure with intralayer order, but without regaining the interlayer order of the pristine crystals. Therefore, redox cycling of SrFeO2.5 crystals in O2 and H2 introduces stacking faults into the structure, resulting in an I2/m(0βγ)0s symmetry with variable β. |
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Thesis |
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Place of Publication |
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Wos |
000891928400001 |
Publication Date |
0000-00-00 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-7488 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.9 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Financial support is acknowledged from the FWO-Hercules fund I003218N ‘Infrastructure for imaging nanoscale processes in gas/vapor or liquid environments’, from the University of Antwerp through grant BOF TOP 38689. This work was supported by the European Commission Horizon 2020 NanED grant number 956099. Financial support from the French National Research Agency (ANR) through the project “Structural induced Electronic Complexity controlled by low temperature Topotactic Reaction” (SECTOR No. ANR-14-CE36- 0006-01) is gratefully acknowledged. |
Approved |
Most recent IF: 11.9 |
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Call Number |
EMAT @ emat @c:irua:192325 |
Serial |
7229 |
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Permanent link to this record |