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Author Zalfani, M.; van der Schueren, B.; Hu, Z.-Y.; Rooke, J.C.; Bourguiga, R.; Wu, M.; Li, Y.; Van Tendeloo, G.; Su, B.-L.
Title Novel 3DOM BiVO4/TiO2nanocomposites for highly enhanced photocatalytic activity Type A1 Journal article
Year 2015 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 3 Issue 3 Pages 21244-21256
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Novel 3DOM BiVO4/TiO2 nanocomposites with intimate contact were for the first time synthesized by a hydrothermal method in order to elucidate their visible-light-driven photocatalytic performances. BiVO4 nanoparticles and 3DOM TiO2 inverse opal were fabricated respectively. These materials were characterized by XRD, XPS, SEM, TEM, N2 adsorption–desorption and UV-vis diffuse (UV-vis) and photoluminescence spectroscopies. As references for comparison, a physical mixture of BiVO4 nanoparticles and 3DOM TiO2 inverse opal powder (0.08 : 1), and a BiVO4/P25 TiO2 (0.08 : 1) nanocomposite made also by the hydrothermal method were prepared. The photocatalytic performance of all the prepared materials was evaluated by the degradation of rhodamine B (RhB) as a model pollutant molecule under visible light irradiation. The highly ordered 3D macroporous inverse opal structure can provide more active surface areas and increased mass transfer because of its highly accessible 3D porosity. The results show that 3DOM BiVO4/TiO2 nanocomposites possess a highly prolonged lifetime and increased separation of visible light generated charges and extraordinarily high photocatalytic activity. Owing to the intimate contact between BiVO4 and large surface area 3DOM TiO2, the photogenerated high energy charges can be easily transferred from BiVO4 to the 3DOM TiO2 support. BiVO4 nanoparticles in the 3DOM TiO2 inverse opal structure act thus as a sensitizer to absorb visible light and to transfer efficiently high energy electrons to TiO2 to ensure long lifetime of the photogenerated charges and keep them well separated, owing to the direct band gap of BiVO4 of 2.4 eV, favourably positioned band edges, very low recombination rate of electron–hole pairs and stability when coupled with photocatalysts, explaining the extraordinarily high photocatalytic performance of 3DOM BiVO4/TiO2 nanocomposites. It is found that larger the amount of BiVO4 in the nanocomposite, longer the duration of photogenerated charge separation and higher the photocatalytic activity. This work can shed light on the development of novel visible light responsive nanomaterials for efficient solar energy utilisation by the intimate combination of an inorganic light sensitizing nanoparticle with an inverse opal structure with high diffusion efficiency and high accessible surface area.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000363163200049 Publication Date 2015-09-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488;2050-7496; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 88 Open Access
Notes This work was realized with the financial support of the Belgian FNRS (Fonds National de la Recherche Scientifique). This research used resources of the Electron Microscopy Service located at the University of Namur. This Service is a member of the “Plateforme Technologique Morphologie – Imagerie”. The XPS analyses were made in the LISE, Department of Physics of the University of Namur thanks to Dr P. Louette. This work was also supported by Changjiang Scholars and the Innovative Research Team (IRT1169) of the Ministry of Education of the People's Republic of China. B. L. Su acknowledges the Chinese Central Government for an “Expert of the State” position in the Program of the “Thousand Talents” and a Clare Hall Life Membership at the Clare Hall and the financial support of the Department of Chemistry, University of Cambridge. G. Van Tendeloo and Z. Y. Hu acknowledge support from the EC Framework 7 program ESTEEM2 (Reference 312483).; esteem2_jra4 Approved (down) Most recent IF: 8.867; 2015 IF: 7.443
Call Number c:irua:129476 c:irua:129476 Serial 3951
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Author Lander, L.; Rousse, G.; Abakumov, A.M.; Sougrati, M.; Van Tendeloo, G.; Tarascon, J.-M.
Title Structural, electrochemical and magnetic properties of a novel KFeSO4F polymorph Type A1 Journal article
Year 2015 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 3 Issue 3 Pages 19754-19764
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract In the quest for sustainable and low-cost positive electrode materials for Li-ion batteries, we discovered, as reported herein, a new low temperature polymorph of KFeSO4F. Contrary to the high temperature phase crystallizing in a KTiOPO4-like structure, this new phase adopts a complex layer-like structure built on FeO4F2 octahedra and SO4 tetrahedra, with potassium cations located in between the layers, as solved using neutron and synchrotron diffraction experiments coupled with electron diffraction. The detailed analysis of the structure reveals an alternation of edge-and corner-shared FeO4F2 octahedra leading to a large monoclinic cell of 1771.774(7) angstrom(3). The potassium atoms are mobile within the structure as deduced by ionic conductivity measurements and confirmed by the bond valence energy landscape approach thus enabling a partial electrochemical removal of K+ and uptake of Li+ at an average potential of 3.7 V vs. Li+/Li-0. Finally, neutron diffraction experiments coupled with SQUID measurements reveal a long range antiferromagnetic ordering of the Fe2+ magnetic moments below 22 K with a possible magnetoelectric behavior.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000362041300018 Publication Date 2015-08-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488; 2050-7496 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 11 Open Access
Notes Approved (down) Most recent IF: 8.867; 2015 IF: 7.443
Call Number UA @ lucian @ c:irua:132566 Serial 4253
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Author Reynaud, M.; Rousse, G.; Abakumov, A.M.; Sougrati, M.T.; Van Tendeloo, G.; Chotard, J.-N.; Tarascon, J.-M.
Title Design of new electrode materials for Li-ion and Na-ion batteries from the bloedite mineral Na2Mg(SO4)2\cdot4H2O Type A1 Journal article
Year 2014 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 2 Issue 8 Pages 2671-2680
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Mineralogy offers a large database to search for Li- or Na-based compounds having suitable structural features for acting as electrode materials, LiFePO4 being one example. Here we further explore this avenue and report on the electrochemical properties of the bloedite type compounds Na2M(SO4)(2)center dot 4H(2)O (M = Mg, Fe, Co, Ni, Zn) and their dehydrated phases Na2M(SO4)(2) (M = Fe, Co), whose structures have been solved via complementary synchrotron X-ray diffraction, neutron powder diffraction and transmission electron microscopy. Among these compounds, the hydrated and anhydrous iron-based phases show electrochemical activity with the reversible release/uptake of 1 Na+ or 1 Li+ at high voltages of similar to 3.3 V vs. Na+/Na-0 and similar to 3.6 V vs. Li+/Li-0, respectively. Although the reversible capacities remain lower than 100 mA h g(-1), we hope this work will stress further the importance of mineralogy as a source of inspiration for designing eco-efficient electrode materials.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000331247500031 Publication Date 2013-11-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488;2050-7496; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 56 Open Access
Notes Approved (down) Most recent IF: 8.867; 2014 IF: 7.443
Call Number UA @ lucian @ c:irua:115807 Serial 659
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Author Neubert, S.; Mitoraj, D.; Shevlin, S.A.; Pulisova, P.; Heimann, M.; Du, Y.; Goh, G.K.L.; Pacia, M.; Kruczała, K.; Turner, S.; Macyk, W.; Guo, Z.X.; Hocking, R.K.; Beranek, R.;
Title Highly efficient rutile TiO2 photocatalysts with single Cu(II) and Fe(III) surface catalytic sites Type A1 Journal article
Year 2016 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 4 Issue 4 Pages 3127-3138
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Highly active photocatalysts were obtained by impregnation of nanocrystalline rutile TiO2 powders with small amounts of Cu(II) and Fe(III) ions, resulting in the enhancement of initial rates of photocatalytic degradation of 4-chlorophenol in water by factors of 7 and 4, compared to pristine rutile, respectively. Detailed structural analysis by EPR and X-ray absorption spectroscopy (EXAFS) revealed that Cu(II) and Fe(III) are present as single species on the rutile surface. The mechanism of the photoactivity enhancement was elucidated by a combination of DFT calculations and detailed experimental mechanistic studies including photoluminescence measurements, photocatalytic experiments using scavengers, OH radical detection, and photopotential transient measurements. The results demonstrate that the single Cu(II) and Fe(III) ions act as effective cocatalytic sites, enhancing the charge separation, catalyzing “dark” redox reactions at the interface, thus improving the normally very low quantum yields of UV light-activated TiO2 photocatalysts. The exact mechanism of the photoactivity enhancement differs depending on the nature of the cocatalyst. Cu(II)-decorated samples exhibit fast transfer of photogenerated electrons to Cu(II/I) sites, followed by enhanced catalysis of dioxygen reduction, resulting in improved charge separation and higher photocatalytic degradation rates. At Fe(III)-modified rutile the rate of dioxygen reduction is not improved and the photocatalytic enhancement is attributed to higher production of highly oxidizing hydroxyl radicals produced by alternative oxygen reduction pathways opened by the presence of catalytic Fe(III/II) sites. Importantly, it was demonstrated that excessive heat treatment (at 450 degrees C) of photocatalysts leads to loss of activity due to migration of Cu(II) and Fe(III) ions from TiO2 surface to the bulk, accompanied by formation of oxygen vacancies. The demonstrated variety of mechanisms of photoactivity enhancement at single site catalyst-modified photocatalysts holds promise for developing further tailored photocatalysts for various applications.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000371077300040 Publication Date 2015-12-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488; 2050-7496 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 44 Open Access
Notes Approved (down) Most recent IF: 8.867
Call Number UA @ lucian @ c:irua:132322 Serial 4191
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Author Naik, P.V.; Wee, L.H.; Meledina, M.; Turner, S.; Li, Y.; Van Tendeloo, G.; Martens, J.A.; Vankelecom, I.F.J.
Title PDMS membranes containing ZIF-coated mesoporous silica spheres for efficient ethanol recovery via pervaporation Type A1 Journal article
Year 2016 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 4 Issue 4 Pages 12790-12798
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The design of functional micro- and mesostructured composite materials is significantly important for separation processes. Mesoporous silica is an attractive material for fast diffusion, while microporous zeolitic imidazolate frameworks (ZIFs) are beneficial for selective adsorption and diffusion. In this work, ZIF-71 and ZIF-8 nanocrystals were grown on the surface of mesoporous silica spheres (MSS) via the seeding and regrowth approach in order to obtain monodispersed MSS-ZIF-71 and MSS-ZIF-8 spheres with a particle size of 2-3 mm. These MSS-ZIF spheres were uniformly dispersed into a polydimethylsiloxane (PDMS) matrix to prepare mixed matrix membranes (MMMs). These MMMs were evaluated for the separation of ethanol from water via pervaporation. The pervaporation results reveal that the MSS-ZIF filled MMMs substantially improve the ethanol recovery in both aspects viz. flux and separation factor. These MMMs outperforms the unfilled PDMS membranes and the conventional carbon and zeolite filled MMMs. As expected, the mesoporous silica core allows very fast flow of the permeating compound, while the hydrophobic ZIF coating enhances the ethanol selectivity through its specific pore structure, hydrophobicity and surface chemistry. It can be seen that ZIF-8 mainly has a positive impact on the selectivity, while ZIF-71 enhances fluxes more significantly.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000382015100012 Publication Date 2016-07-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488; 2050-7496 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 26 Open Access
Notes Approved (down) Most recent IF: 8.867
Call Number UA @ lucian @ c:irua:137188 Serial 4395
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Author Pulinthanathu Sree, S.; Dendooven, J.; Geerts, L.; Ramachandran, R.K.; Javon, E.; Ceyssens, F.; Breynaert, E.; Kirschhock, C.E.A.; Puers, R.; Altantzis, T.; Van Tendeloo, G.; Bals, S.; Detavernier, C.; Martens, J.A.
Title 3D porous nanostructured platinum prepared using atomic layer deposition Type A1 Journal article
Year 2017 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 5 Issue 5 Pages 19007-19016
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract A robust and easy to handle 3D porous platinum structure was created via replicating the 3D channel system

of an ordered mesoporous silica material using atomic layer deposition (ALD) over micrometer distances.

After ALD of Pt in the silica material, the host template was digested using hydrogen fluoride (HF). A fully

connected ordered Pt nanostructure was obtained with morphology and sizes corresponding to that of

the pores of the host matrix, as revealed with high-resolution scanning transmission electron

microscopy and electron tomography. The Pt nanostructure consisted of hexagonal Pt rods originating

from the straight mesopores (11 nm) of the host structure and linking features resulting from Pt

replication of the interconnecting mesopore segments (2–4 nm) present in the silica host structure.

Electron tomography of partial replicas, made by incomplete infilling of Zeotile-4 material with Pt,

provided insight in the connectivity and formation mechanism of the Pt nanostructure by ALD. The Pt

replica was evaluated for its potential use as electrocatalyst for the hydrogen evolution reaction, one of

the half-reactions of water electrolysis, and as microelectrode for biomedical sensing. The Pt replica

showed high activity for the hydrogen evolution reaction and electrochemical characterization revealed

a large impedance improvement in comparison with reference Pt electrodes.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000411232100010 Publication Date 2017-06-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 9 Open Access OpenAccess
Notes This work was supported by the Flemish government through long-term structural funding (Methusalem) to JAM and FWO for a research project (G0A5417N). JD, TA and FC acknowledge Flemish FWO for a post-doctoral fellowship. S. B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); saraecas; ECAS_Sara; Approved (down) Most recent IF: 8.867
Call Number EMAT @ emat @ c:irua:144624 c:irua:144624 c:irua:144624UA @ admin @ c:irua:144624 Serial 4634
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Author Ben Dkhil, S.; Pfannmöller, M.; Ata, I.; Duche, D.; Gaceur, M.; Koganezawa, T.; Yoshimoto, N.; Simon, J.-J.; Escoubas, L.; Videlot-Ackermann, C.; Margeat, O.; Bals, S.; Bauerle, P.; Ackermann, J.
Title Time evolution studies of dithieno[3,2-b:2 ',3 '-d] pyrrole-based A-D-A oligothiophene bulk heterojunctions during solvent vapor annealing towards optimization of photocurrent generation Type A1 Journal article
Year 2017 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume 5 Issue 5 Pages 1005-1013
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Solvent vapor annealing (SVA) is one of the main techniques to improve the morphology of bulk heterojunction solar cells using oligomeric donors. In this report, we study time evolution of nanoscale morphological changes in bulk heterojunctions based on a well-studied dithienopyrrole-based A-D-A oligothiophene (dithieno[3,2-b: 2',3'-d] pyrrole named here 1) blended with [6,6]-phenyl-C-71-butyric acid methyl ester (PC71BM) to increase photocurrent density by combining scanning transmission electron microscopy and low-energy-loss spectroscopy. Our results show that SVA transforms the morphology of 1 : PC71BM blends by a three-stage mechanism: highly intermixed phases evolve into nanostructured bilayers that correspond to an optimal blend morphology. Additional SVA leads to completely phaseseparated micrometer-sized domains. Optical spacers were used to increase light absorption inside optimized 1 : PC71BM blends leading to solar cells of 7.74% efficiency but a moderate photocurrent density of 12.3 mA cm (-2). Quantum efficiency analyses reveal that photocurrent density is mainly limited by losses inside the donor phase. Indeed, optimized 1 : PC71BM blends consist of large donor-enriched domains not optimal for exciton to photocurrent conversion. Shorter SVA times lead to smaller domains; however they are embedded in large mixed phases suggesting that introduction of stronger molecular packing may help us to better balance phase separation and domain size enabling more efficient bulk heterojunction solar cells.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000394430800018 Publication Date 2016-11-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488; 2050-7496 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 19 Open Access Not_Open_Access
Notes ; We acknowledge financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (Grant number: F1110019V/201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7, Grant number: 287594). The synchrotron radiation experiments were performed at BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2016A1568). We further acknowledge financial support via ERC Starting Grant Colouratoms (335078). ; Approved (down) Most recent IF: 8.867
Call Number UA @ lucian @ c:irua:142602UA @ admin @ c:irua:142602 Serial 4695
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Author Arenas-Vivo, A.; Rojas, S.; Ocaña, I.; Torres, A.; Liras, M.; Salles, F.; Arenas-Esteban, D.; Bals, S.; Ávila, D.; Horcajada, P.
Title Ultrafast reproducible synthesis of a Ag-nanocluster@MOF composite and its superior visible-photocatalytic activity in batch and in continuous flow Type A1 Journal article
Year 2021 Publication Journal Of Materials Chemistry A Abbreviated Journal J Mater Chem A
Volume 9 Issue 28 Pages 15704-15713
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The (photo)catalytic properties of metal–organic frameworks (MOFs) can be enhanced by post-synthetic inclusion of metallic species in their porosity. Due to their extraordinarily high surface area and well defined porous structure, MOFs can be used for the stabilization of metal nanoparticles with adjustable size within their porosity. Originally, we present here an optimized ultrafast photoreduction protocol for the<italic>in situ</italic>synthesis of tiny and monodisperse silver nanoclusters (AgNCs) homogeneously supported on a photoactive porous titanium carboxylate MIL-125-NH<sub>2</sub>MOF. The strong metal–framework interaction between –NH<sub>2</sub>and Ag atoms influences the AgNC growth, leading to the surfactant-free efficient catalyst AgNC@MIL-125-NH<sub>2</sub>with improved visible light absorption. The potential use of AgNC@MIL-125-NH<sub>2</sub>was further tested in challenging applications: (i) the photodegradation of the emerging organic contaminants (EOCs) methylene blue (MB-dye) and sulfamethazine (SMT-antibiotic) in water treatment, and (ii) the catalytic hydrogenation of<italic>p</italic>-nitroaniline (4-NA) to<italic>p</italic>-phenylenediamine (PPD) with industrial interest. It is noteworthy that compared with the pristine MIL-125-NH<sub>2</sub>, the composite presents an improved catalytic activity and stability, being able to photodegrade 92% of MB in 60 min and 96% of SMT in 30 min, and transform 100% of 4-NA to PPD in 30 min. Aside from these very good results, this study describes for the first time the use of a MOF in a visible light continuous flow reactor for wastewater treatment. With only 10 mg of AgNC@MIL-125-NH<sub>2</sub>, high SMT removal efficiency over 70% is maintained after >2 h under water flow conditions found in real wastewater treatment plants, signaling a future real application of MOFs in water remediation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000671839200001 Publication Date 2021-06-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 18 Open Access OpenAccess
Notes Comunidad de Madrid, CAM PEJD-2016/IND-2828 Talento Modality 2, 2017-T2/IND-5149 ; Secretaría de Estado de Investigación, Desarrollo e Innovación, Raphuel project (ENE2016-79608-C2-1-R) Retos Project MAT2017-84385-R ; Ministerio de Ciencia e Innovación, Juan de la Cierva Incorporación Fellowship (grant agreement no. IJC2019-038894-I) MOFSEIDON project (PID2019-104228RB-I00) Ramón y Cajal, Grant Agreements 2014-15039 and 2015-18677 ; Fundación BBVA, IN[17]CBBQUI_0197 ; H2020 European Research Council, ERC Consolidator Grant REALNANO 815128 Grant Agreement no. 731019 (EUSMI) ; sygmaSB; Approved (down) Most recent IF: 8.867
Call Number EMAT @ emat @c:irua:179791 Serial 6802
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Author Wang, L.; Li, Y.; Yang, X.-Y.; Zhang, B.-B.; Ninane, N.; Busscher, H.J.; Hu, Z.-Y.; Delneuville, C.; Jiang, N.; Xie, H.; Van Tendeloo, G.; Hasan, T.; Su, B.-L.
Title Single-cell yolk-shell nanoencapsulation for long-term viability with size-dependent permeability and molecular recognition Type A1 Journal article
Year 2021 Publication National Science Review Abbreviated Journal Natl Sci Rev
Volume 8 Issue 4 Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Like nanomaterials, bacteria have been unknowingly used for centuries. They hold significant economic potential for fuel and medicinal compound production. Their full exploitation, however, is impeded by low biological activity and stability in industrial reactors. Though cellular encapsulation addresses these limitations, cell survival is usually compromised due to shell-to-cell contacts and low permeability. Here, we report ordered packing of silica nanocolloids with organized, uniform and tunable nanoporosities for single cyanobacterium nanoencapsulation using protamine as an electrostatic template. A space between the capsule shell and the cell is created by controlled internalization of protamine, resulting in a highly ordered porous shell-void-cell structure formation. These unique yolk-shell nano structures provide long-term cell viability with superior photosynthetic activities and resistance in harsh environments. In addition, engineering the colloidal packing allows tunable shell-pore diameter for size-dependent permeability and introduction of new functionalities for specific molecular recognition. Our strategy could significantly enhance the activity and stability of cyanobacteria for various nanobiotechnological applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000651827200002 Publication Date 2020-05-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2095-5138 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.843 Times cited Open Access OpenAccess
Notes Approved (down) Most recent IF: 8.843
Call Number UA @ admin @ c:irua:179085 Serial 6885
Permanent link to this record
 
 
Author Bai, J.; Wang, J.T.-W.; Rubio, N.; Protti, A.; Heidari, H.; Elgogary, R.; Southern, P.; Al-Jamal, W.' T.; Sosabowski, J.; Shah, A.M.; Bals, S.; Pankhurst, Q.A.; Al-Jamal, K.T.
Title Triple-Modal Imaging of Magnetically-Targeted Nanocapsules in Solid TumoursIn Vivo Type A1 Journal article
Year 2016 Publication Theranostics Abbreviated Journal Theranostics
Volume 6 Issue 6 Pages 342-356
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Triple-modal imaging magnetic nanocapsules, encapsulating hydrophobic superparamagnetic iron oxide nanoparticles, are formulated and used to magnetically target solid tumours after intravenous administration in tumour-bearing mice. The engineered magnetic polymeric nanocapsules m-NCs are ~200 nm in size with negative Zeta potential and shown to be spherical in shape. The loading efficiency of superparamagnetic iron oxide nanoparticles in the m-NC was ~100%. Up to ~3- and ~2.2-fold increase in tumour uptake at 1 and 24 h was achieved, when a static magnetic field was applied to the tumour for 1 hour. m-NCs, with multiple imaging probes (e.g. indocyanine green, superparamagnetic iron oxide nanoparticles and indium-111), were capable of triple-modal imaging (fluorescence/magnetic resonance/nuclear imaging) in vivo. Using triple-modal imaging is to overcome the intrinsic limitations of single modality imaging and provides complementary information on the spatial distribution of the nanocarrier within the tumour. The significant findings of this study could open up new research perspectives in using novel magnetically-responsive nanomaterials in magnetic-drug targeting combined with multi-modal imaging.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000377797200005 Publication Date 2015-12-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1838-7640 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.712 Times cited 54 Open Access OpenAccess
Notes The authors would like to thank Prof Robert Hider (King's College London) for useful discussion on the chemical functionalization of the polymers, Mr William Luckhurst (King's College London) on the technical help of AFM measurements and Mr Andrew Cakebread (King's College London) on his technical help of ICP-MS measurements. J.B. acknowledges funding from King's-China Scholarship Council (CSC). J.W. and N.R. acknowledge funding from Biotechnology and Biological Sciences Research Council (BB/J008656/1) and Associated International Cancer Research (12-1054). K.T.AJ. acknowledges funding from EU FP7-ITN Marie-Curie Network programme RADDEL (290023). S.B. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant No. 335078 COLOURATOMS, and the Integrated Infrastructure Initiative No. 262348 European Soft Matter Infrastructure, ESMI.; ECAS_Sara; (ROMEO:green; preprint:; postprint:can ; pdfversion:can); Approved (down) Most recent IF: 8.712
Call Number c:irua:130058 Serial 3995
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Author Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J.
Title Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity Type A1 Journal Article
Year 2024 Publication Chemistry of Materials Abbreviated Journal Chem. Mater.
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide

fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure,

with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5%

H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 001174840900001 Publication Date 2024-02-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access Not_Open_Access
Notes Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; Approved (down) Most recent IF: 8.6; 2024 IF: 9.466
Call Number EMAT @ emat @c:irua:204354 Serial 8997
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Author van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D.
Title Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000959572100001 Publication Date 2023-03-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 2 Open Access OpenAccess
Notes H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number EMAT @ emat @c:irua:195894 Serial 7255
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Author Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W.
Title Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal Chem. Mater.
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001052093300001 Publication Date 2023-08-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number EMAT @ emat @c:irua:198151 Serial 8810
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Author Arenas Esteban, D.; Pacquets, L.; Choukroun, D.; Hoekx, S.; Kadu, A.A.; Schalck, J.; Daems, N.; Breugelmans, T.; Bals, S.
Title 3D characterization of the structural transformation undergone by Cu@Ag core-shell nanoparticles following CO₂ reduction reaction Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 17 Pages 6682-6691
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract The increasing use of metallic nanoparticles (NPs) is significantly advancing the field of electrocatalysis. In particular, Cu/Ag bimetallic interfaces are widely used to enhance the electrochemical CO2 reduction reaction (eCO(2)RR) toward CO and, more recently, C-2 products. However, drastic changes in the product distribution and performance when Cu@Ag core-shell configurations are used can often be observed under electrochemical reaction conditions, especially during the first few minutes of the reaction. Possible structural changes that generate these observations remain underexplored; therefore, the structure-property relationship is hardly understood. In this study, we use electron tomography to investigate the structural transformation mechanism of Cu@Ag core-shells NPs during the critical first minutes of the eCO(2)RR. In this manner, we found that the crystallinity of the Cu seed determines whether the formation of a complete and homogeneous Ag shell is possible. Moreover, by tracking the particles' transformations, we conclude that modifications of the Cu-Ag interface and Cu2O enrichment at the surface of the NPs are key factors contributing to the product generation changes. These insights provide a better understanding of how bimetallic core-shell NPs transform under electrochemical conditions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001061530700001 Publication Date 2023-08-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 1 Open Access OpenAccess
Notes L.P. was supported through a PhD fellowship for strategicbasic research (1S56920N) of the Research Foundation – Flanders(FWO). S.H. was supported through a PhD fellowship for strategic basicresearch (1S42623N) of the Research Foundation – Flanders (FWO).S.B., D.A.E., and A.A.K. acknowledge financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the researchcouncil of the University of Antwerp (BOF-GOA 33928). Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:199187 Serial 8825
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Author Mulder, J.T.T.; Jenkinson, K.; Toso, S.; Prato, M.; Evers, W.H.H.; Bals, S.; Manna, L.; Houtepen, A.J.J.
Title Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 14 Pages 5311-5321
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001021474500001 Publication Date 2023-07-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the large-scale limit of quantum mechanics). The authors thank Niranjan Saikumar for proof reading the manuscript. Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:197787 Serial 8907
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Author Mayda, S.; Monico, L.; Krishnan, D.; De Meyer, S.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Sandu, I.C.A.; Partoens, B.; Lamoen, D.; Romani, A.; Miliani, C.; Verbeeck, J.; Janssens, K.
Title A combined experimental and computational approach to understanding CdS pigment oxidation in a renowned early 20th century painting Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 24 Pages 10403-10415
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract Cadmium sulfide (CdS)-based yellow pigments have been used in a number of early 20th century artworks, including The Scream series painted by Edvard Munch. Some of these unique paintings are threatened by the discoloration of these CdS-based yellow oil paints because of the oxidation of the original sulfides to sulfates. The experimental data obtained here prove that moisture and cadmium chloride compounds play a key role in promoting such oxidation. To clarify how these two factors effectively prompt the process, we studied the band alignment between CdS, CdCl2, and Cd-(OH)Cl as well as the radicals center dot OH and H3O center dot by density functional theory (DFT) methods. Our results show that a stack of several layers of Cd-(OH)Cl creates a pocket of positive holes at the Cl-terminated surface and a pocket of electrons at the OH-terminated surface by leading in a difference in ionization energy at both surfaces. The resulting band alignment indicates that Cd-(OH)Cl can indeed play the role of an oxidative catalyst for CdS in a moist environment, thus providing an explanation for the experimental evidence.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001133000900001 Publication Date 2023-12-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access
Notes The experimental research on the cadmium yellow powders/paint mock-ups and The Scream (ca. 1910) was financially supported by the European Union, research projects IPERION-CH (H2020-INFRAIA-2014-2015, GA no. 654028) and IPERION-HS (H2020-INFRAIA-2019-1, GA no. 871034) and the project AMIS within the program Dipartimenti di Eccellenza 2018-2022 (funded by MUR and the University of Perugia). For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiments HG64 and HG95), the DESY-P06 beamline, a member of the Helmholtz Association HGF (experiments I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the GA no. 730872 from the E.U. Framework Programme for Research and Innovation Horizon 2020. All of the staff of the MUNCH Museum (Conservation Department) is acknowledged for their collaboration. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO – Vlaanderen and the Flemish Government, Department EWI. Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:202836 Serial 8999
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Author Shevchenko, V.A.; Glazkova, I.S.; Novichkov, D.A.; Skvortsova, I.; V. Sobolev, A.; Abakumov, A.M.; Presniakov, I.A.; Drozhzhin, O.A.; V. Antipov, E.
Title Competition between the Ni and Fe redox in the O3-NaNi1/3Fe1/3Mn1/3O2 cathode material for Na-ion batteries Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 10 Pages 4015-4025
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sodium-ion batteries are attracting great attention due to their low cost and abundance of sodium. The O3-type NaNi1/3Fe1/3Mn1/3O2 layered oxide material is a promising candidate for positive electrodes (cathodes) in Na-ion batteries. However, its stable electrochemical performance is restricted by the upper voltage limit of 4.0 V (vs Na/Na+), which allows for reversibly removing 0.5-0.55 Na+ per formula unit, corresponding to the capacity of 120-130 mAh.g(-1). Further reduction of sodium content inevitably accelerates capacity degradation, and this issue calls for a detailed study of the redox reactions that accompany the electrochemical (de)intercalation of a large amount of sodium. Here, we present operando and ex situ studies using powder X-ray diffraction and X-ray absorption spectroscopy combined with Fe-57 Mossbauer spectroscopy. Our approach reveals the sequence of the redox transitions that occur during the charge and discharge of O3-NaNi1/3Fe1/3Mn1/3O2. Our data show that in addition to nickel and iron cations oxidizing to M+4, a part of iron transforms into the “3 + delta” state owing to the fast electron exchange Fe3+ + Fe4+ <-> Fe4+ + Fe3+. This process freezes upon cooling the material to 35 K, producing Fe4+ cations, some of which occupy tetrahedral positions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000985970200001 Publication Date 2023-05-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited Open Access
Notes Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:197352 Serial 9013
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Author Manzaneda-Gonzalez, V.; Jenkinson, K.; Pena-Rodriguez, O.; Borrell-Grueiro, O.; Trivino-Sanchez, S.; Banares, L.; Junquera, E.; Espinosa, A.; Gonzalez-Rubio, G.; Bals, S.; Guerrero-Martinez, A.
Title From multi- to single-hollow trimetallic nanocrystals by ultrafast heating Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 22 Pages 9603-9612
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Metal nanocrystals (NCs) display unique physicochemical features that are highly dependent on nanoparticle dimensions, anisotropy, structure, and composition. The development of synthesis methodologies that allow us to tune such parameters finely emerges as crucial for the application of metal NCs in catalysis, optical materials, or biomedicine. Here, we describe a synthetic methodology to fabricate hollow multimetallic heterostructures using a combination of seed-mediated growth routes and femtosecond-pulsed laser irradiation. The envisaged methodology relies on the coreduction of Ag and Pd ions on gold nanorods (Au NRs) to form Au@PdAg core-shell nanostructures containing small cavities at the Au-PdAg interface. The excitation of Au@PdAg NRs with low fluence femtosecond pulses was employed to induce the coalescence and growth of large cavities, forming multihollow anisotropic Au@PdAg nanostructures. Moreover, single-hollow alloy AuPdAg could be achieved in high yield by increasing the irradiation energy. Advanced electron microscopy techniques, energy-dispersive X-ray spectroscopy (EDX) tomography, X-ray absorption near-edge structure (XANES) spectroscopy, and finite differences in the time domain (FDTD) simulations allowed us to characterize the morphology, structure, and elemental distribution of the irradiated NCs in detail. The ability of the reported synthesis route to fabricate multimetallic NCs with unprecedented hollow nanostructures offers attractive prospects for the fabrication of tailored high-entropy alloy nanoparticles.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001110623500001 Publication Date 2023-11-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 2 Open Access OpenAccess
Notes Approved (down) Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:202144 Serial 9040
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Author Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K.
Title Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments Type A1 Journal article
Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
Volume 32 Issue 7 Pages 2863-2873
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000526394000016 Publication Date 2020-04-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 8 Open Access OpenAccess
Notes Universiteit Antwerpen; Belgian Federal Science Policy Office; Approved (down) Most recent IF: 8.6; 2020 IF: 9.466
Call Number EMAT @ emat @c:irua:168819 Serial 6363
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Author Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L.
Title Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission Type A1 Journal article
Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
Volume 32 Issue Pages acs.chemmater.0c03825
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000603288800034 Publication Date 2020-12-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 44 Open Access OpenAccess
Notes European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma Approved (down) Most recent IF: 8.6; 2020 IF: 9.466
Call Number EMAT @ emat @c:irua:174004 Serial 6659
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Author De wael, A.; De Backer, A.; Jones, L.; Varambhia, A.; Nellist, P.D.; Van Aert, S.
Title Measuring Dynamic Structural Changes of Nanoparticles at the Atomic Scale Using Scanning Transmission Electron Microscopy Type A1 Journal article
Year 2020 Publication Physical Review Letters Abbreviated Journal Phys Rev Lett
Volume 124 Issue 10 Pages 106105
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We propose a new method to measure atomic scale dynamics of nanoparticles from experimental high-resolution annular dark field scanning transmission electron microscopy images. By using the so-called hidden Markov model, which explicitly models the possibility of structural changes, the number of atoms in each atomic column can be quantified over time. This newly proposed method outperforms the current atom-counting procedure and enables the determination of the probabilities and cross sections for surface diffusion. This method is therefore of great importance for revealing and quantifying the atomic structure when it evolves over time via adatom dynamics, surface diffusion, beam effects, or during in situ experiments.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000519718100015 Publication Date 2020-03-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0031-9007 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Grant Agreement No. 770887 and No. 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A.D.w. and A.D.B. and projects G.0502.18N and EOS 30489208. L.J. acknowledges the SFI AMBER Centre for support. A.V. and P.D.N. acknowledge the UK Engineering and Physical Sciences Council (EPSRC) for support (EP/K040375/1 and 1772738). A.V. also acknowledges Johnson-Matthey for support. We would like to thank Brian Theobald and Jonathan Sharman from JMTC Sonning for provision of the Pt sample. Approved (down) Most recent IF: 8.6; 2020 IF: 8.462
Call Number EMAT @ emat @c:irua:167148 Serial 6347
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Author Li, C.; Sanli, E.S.; Barragan-Yani, D.; Stange, H.; Heinemann, M.-D.; Greiner, D.; Sigle, W.; Mainz, R.; Albe, K.; Abou-Ras, D.; van Aken, P. A.
Title Secondary-Phase-Assisted Grain Boundary Migration in CuInSe2 Type A1 Journal article
Year 2020 Publication Physical Review Letters Abbreviated Journal Phys Rev Lett
Volume 124 Issue 9 Pages 095702
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Significant structural evolution occurs during the deposition of CuInSe2 solar materials when the Cu content increases. We use in situ heating in a scanning transmission electron microscope to directly observe how grain boundaries migrate during heating, causing nondefected grains to consume highly defected grains. Cu substitutes for In in the near grain boundary regions, turning them into a Cu-Se phase topotactic with the CuInSe2 grain interiors. Together with density functional theory and molecular dynamics calculations, we reveal how this Cu-Se phase makes the grain boundaries highly mobile.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000518464200009 Publication Date 2020-03-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0031-9007 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes Horizon 2020 Framework Programme, 823717—ESTEEM3 ; Max-Planck-Gesellschaft; Helmholtz Virtual Institute; Approved (down) Most recent IF: 8.6; 2020 IF: 8.462
Call Number UA @ lucian @c:irua:167699 Serial 6393
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Author Lieberman, C.M.; Filatov, A.S.; Wei, Z.; Rogachev, A.Y.; Abakumov, A.M.; Dikarev, E.V.
Title Mixed-valent, heteroleptic homometallic diketonates as templates for the design of volatile heterometallic precursors Type A1 Journal article
Year 2015 Publication Chemical science Abbreviated Journal Chem Sci
Volume 6 Issue 6 Pages 2835-2842
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A novel series of mixed-valent, heteroleptic transition metal diketonates that can be utilized as prospective single-source precursors for the low-temperature preparation of oxide materials are reported. The first mixed-valent iron beta-diketonates with different Fe-III/Fe-II ratios have been synthesized by applying the mixed-ligand approach. Based on nearly quantitative reaction yields and analysis of iron-oxygen bonds, these compounds were formulated as [Fe-III(acac)(3)][Fe-II(hfac)(2)] (1) and [Fe-II(hfac)(2)][Fe-III(acac)(3)][Fe-II(hfac)(2)] (2). In the above heteroleptic complexes, the Lewis acidic, coordinatively unsaturated Fe-II centers chelated by two hfac (hexafluoroacetylacetonate) ligands with electron-withdrawing substituents maintain bridging interactions with oxygen atoms of electron-donating acac (acetylacetonate) groups that chelate the neighboring Fe-III atoms. Switching the ligands on Fe-III and Fe-II atoms in starting reagents resulted in the instant ligand exchange between iron centers and in yet another polynuclear homometallic diketonate [Fe-II(hfac)(2)][Fe-III(acac)(2)(hfac)][Fe-II(hfac)(2)] (3) that adheres to the same bonding pattern as in complexes 1 and 2. The proposed synthetic methodology has been extended to design heterometallic diketonates with different M : M' ratios. Homometallic parent molecules have been used as templates to obtain heterometallic mixed-valent [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Ni-II(hfac)(2)] – [Fe-III(acac)(3)][Ni-II(hfac)(2)] (5) complexes. The combination of two different diketonate ligands with electron-donating and electron-withdrawing substituents was found to be crucial for maintaining the above mixed-valent heterometallic assemblies. Theoretical investigation of two possible “isomers”, [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Mn-III(acac)(3)][Fe-II(hfac)(2)] (40) provided an additional support for the metal site assignment giving a preference of 9.78 kcal mol(-1) for the molecule 4. Heterometallic complexes obtained in the course of this study have been found to act as effective single-source precursors for the synthesis of mixed-transition metal oxide materials MxM2-xO3 and MxMi-xO. The title highly volatile precursors can be used for the low-temperature preparation of both amorphous and crystalline heterometallic oxides in the form of thin films or nanosized particles that are known to operate as efficient catalysts in oxygen evolution reaction.
Address
Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000353223100021 Publication Date 2015-02-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520;2041-6539; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 13 Open Access
Notes Approved (down) Most recent IF: 8.668; 2015 IF: 9.211
Call Number c:irua:126031 Serial 2092
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Author Alaria, J.; Borisov, P.; Dyer, M.S.; Manning, T.D.; Lepadatu, S.; Cain, M.G.; Mishina, E.D.; Sherstyuk, N.E.; Ilyin, N.A.; Hadermann, J.; Lederman, D.; Claridge, J.B.; Rosseinsky, M.J.;
Title Engineered spatial inversion symmetry breaking in an oxide heterostructure built from isosymmetric room-temperature magnetically ordered components Type A1 Journal article
Year 2014 Publication Chemical science Abbreviated Journal Chem Sci
Volume 5 Issue 4 Pages 1599-1610
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
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Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000332467400044 Publication Date 2014-01-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520;2041-6539; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 24 Open Access
Notes Approved (down) Most recent IF: 8.668; 2014 IF: 9.211
Call Number UA @ lucian @ c:irua:117064 Serial 1045
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Author Yan, L.; Niu, H.J.; Duong, G.V.; Suchomel, M.R.; Bacsa, J.; Chalker, P.R.; Hadermann, J.; Van Tendeloo, G.; Rosseinsky, M.J.
Title Cation ordering within the perovskite block of a six-layer Ruddlesden-Popper oxide from layer-by-layer growth artificial interfaces in complex unit cells Type A1 Journal article
Year 2011 Publication Chemical science Abbreviated Journal Chem Sci
Volume 2 Issue 2 Pages 261-272
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The (AO)(ABO3)n Ruddlesden-Popper structure is an archetypal complex oxide consisting of two distinct structural units, an (AO) rock salt layer separating an n-octahedra thick perovskite block. Conventional high-temperature oxide synthesis methods cannot access members with n > 3, but low-temperature layer-by-layer thin film methods allow the preparation of materials with thicker perovskite blocks, exploiting high surface mobility and lattice matching with the substrate. This paper describes the growth of an n = 6 member CaO[(CSMO)2(LCMO)2 (CSMO)2] in which the six unit cell perovskite block is sub-divided into two central La0.67Ca0.33MnO3 (LCMO) and two terminal Ca0.85Sm0.15MnO3 (CSMO) layers to allow stabilization of the rock salt layer and variation of the transition metal charge.
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Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000286327600010 Publication Date 2010-11-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520;2041-6539; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 16 Open Access
Notes Approved (down) Most recent IF: 8.668; 2011 IF: 7.525
Call Number UA @ lucian @ c:irua:88652 Serial 300
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Author Yang, T.; Abakumov, A.M.; Hadermann, J.; Van Tendeloo, G.; Nowik, I.; Stephens, P.W.; Hamberger, J.; Tsirlin, A.A.; Ramanujachary, K.V.; Lofland, S.; Croft, M.; Ignatov, A.; Sun, J.; Greenblatt, M.
Title _BiMnFe2O6, a polysynthetically twinned hcp MO structure Type A1 Journal article
Year 2010 Publication Chemical science Abbreviated Journal Chem Sci
Volume 1 Issue 6 Pages 751-762
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The most efficient use of spatial volume and the lowest potential energies in the metal oxide structures are based on cubic close packing (ccp) or hexagonal close packing (hcp) of anions with cations occupying the interstices. A promising way to tune the composition of close packed oxides and design new compounds is related to fragmenting the parent structure into modules by periodically spaced planar interfaces, such as twin planes at the unit cell scale. The unique crystal chemistry properties of cations with a lone electron pair, such as Bi3+ or Pb2+, when located at interfaces, enables them to act as chemical scissors, to help relieve configurational strain. With this approach, we synthesized a new oxide, BiMnFe2O6, where fragments of the hypothetical hcp oxygen-based MO structure (the NiAs structure type), for the first time, serve as the building modules in a complex transition metal oxide. Mn3+ and Fe3+ ions are randomly distributed in two crystallographically independent sites (M1 and M2). The structure consists of quasi two-dimensional blocks of the 2H hexagonal close packed MO structure cut along the (114) crystal plane of the hcp lattice and stacked along the c axis. The blocks are related by a mirror operation that allows BiMnFe2O6 to be considered as a polysynthetically twinned 2H hcp MO structure. The transition to an AFM state with an incommensurate spin configuration at [similar] 212 K is established by 57Fe Mössbauer spectroscopy, magnetic susceptibility, specific heat and low temperature powder neutron diffraction.
Address
Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000283939200013 Publication Date 2010-10-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520;2041-6539; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 12 Open Access
Notes Approved (down) Most recent IF: 8.668; 2010 IF: NA
Call Number UA @ lucian @ c:irua:85823 Serial 3517
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Author Bueken, B.; Van Velthoven, N.; Willhammar, T.; Stassin, T.; Stassen, I.; Keen, D.A.; Baron, G.V.; Denayer, J.F.M.; Ameloot, R.; Bals, S.; De Vos, D.; Bennett, T.D.
Title Gel-based morphological design of zirconium metal-organic frameworks Type A1 Journal article
Year 2017 Publication Chemical science Abbreviated Journal Chem Sci
Volume 8 Issue 8 Pages 3939-3948
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X – H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.
Address
Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000400553000077 Publication Date 2017-03-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 168 Open Access OpenAccess
Notes ; B. B., T. S. and I. S. acknowledge the FWO Flanders (doctoral and post-doctoral grants). T. W. acknowledges a post-doctoral grant from the Swedish Research Council. T. D. B. acknowledges the Royal Society (University Research Fellowship) and Trinity Hall (University of Cambridge) for funding. S. B. and D. D. V. are grateful for funding by Belspo (IAP 7/05 P6/27) and by the FWO Flanders. D. D. V. further acknowledges funding from the European Research Council (project H-CCAT). S. B. acknowledges financial support from the European Research Council (ERC Starting Grant #335078-COLOURATOMS). The authors acknowledge Arnau Carne and Shuhei Furukawa for assistance with supercritical CO<INF>2</INF> extraction, and Charles Ghesquiere for assistance in synthesis. ; Ecas_Sara Approved (down) Most recent IF: 8.668
Call Number UA @ lucian @ c:irua:152643UA @ admin @ c:irua:152643 Serial 5143
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Author Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E.
Title Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation Type A1 Journal article
Year 2019 Publication Chemical science Abbreviated Journal Chem Sci
Volume 10 Issue 10 Pages 3616-3622
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000463759100017 Publication Date 2019-02-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-6520 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.668 Times cited 68 Open Access OpenAccess
Notes ; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; Approved (down) Most recent IF: 8.668
Call Number UA @ admin @ c:irua:159403 Serial 5259
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Author Wang, Y.; Belén Serrano, A.; Sentosun, K.; Bals, S.; Liz-Marzán, L.M.
Title Stabilization and encapsulation of gold nanostars mediated by dithiols Type A1 Journal article
Year 2015 Publication Small Abbreviated Journal Small
Volume 11 Issue 11 Pages 4314-4320
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Surface chemistry plays a pivotal role in regulating the morphology of nanoparticles, maintaining colloidal stability, and mediating the interaction with target analytes toward practical applications such as surface-enhanced Raman scattering (SERS)-based sensing and imaging. The use of a binary ligand mixture composed of 1,4-benzenedithiol (BDT) and hexadecyltrimethylammonium chloride (CTAC) to provide gold nanostars with long-term stability is reported. This is despite BDT being a bifunctional ligand, which usually leads to bridging and loss of colloidal stability. It is found however that neither BDT nor CTAC alone are able to provide sufficient colloidal and chemical stability. BDT-coated Au nanostars are additionally used as seeds to direct the encapsulation with a gold outer shell, leading to the formation of unusual nanostructures including semishell-coated gold nanostars, which are characterized by high-resolution electron microscopy and electron tomography. Finally, BDT is exploited as a probe to reveal the enhanced local electric fields in the different nanostructures, showing that the semishell configuration provides significantly high SERS signals as compared to other coreshell configurations obtained during seeded growth, including full shells.
Address
Corporate Author Thesis
Publisher Place of Publication Weinheim Editor
Language Wos 000360852900009 Publication Date 2015-06-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1613-6810; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.643 Times cited 36 Open Access OpenAccess
Notes 267867 Plasmaquo; 335078 Colouratom; 262348 Esmi; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved (down) Most recent IF: 8.643; 2015 IF: 8.368
Call Number c:irua:127571 Serial 3136
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Author Rehor, I.; Slegerova, J.; Kucka, J.; Proks, V.; Petrakova, V.; Adam, M.P.; Treussart, F.; Turner, S.; Bals, S.; Sacha, P.; Ledvina, M.; Wen, A.M.; Steinmetz, N.F.; Cigler, P.;
Title Fluorescent nanodiamonds embedded in biocompatible translucent shells Type A1 Journal article
Year 2014 Publication Small Abbreviated Journal Small
Volume 10 Issue 6 Pages 1106-1115
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract High pressure high temperature (HPHT) nanodiamonds (NDs) represent extremely promising materials for construction of fluorescent nanoprobes and nanosensors. However, some properties of bare NDs limit their direct use in these applications: they precipitate in biological solutions, only a limited set of bio-orthogonal conjugation techniques is available and the accessible material is greatly polydisperse in shape. In this work, we encapsulate bright 30-nm fluorescent nanodiamonds (FNDs) in 1020-nm thick translucent (i.e., not altering FND fluorescence) silica shells, yielding monodisperse near-spherical particles of mean diameter 66 nm. High yield modification of the shells with PEG chains stabilizes the particles in ionic solutions, making them applicable in biological environments. We further modify the opposite ends of PEG chains with fluorescent dyes or vectoring peptide using click chemistry. High conversion of this bio-orthogonal coupling yielded circa 2000 dye or peptide molecules on a single FND. We demonstrate the superior properties of these particles by in vitro interaction with human prostate cancer cells: while bare nanodiamonds strongly aggregate in the buffer and adsorb onto the cell membrane, the shell encapsulated NDs do not adsorb nonspecifically and they penetrate inside the cells.
Address
Corporate Author Thesis
Publisher Place of Publication Weinheim Editor
Language Wos 000333538000012 Publication Date 2014-02-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1613-6810; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.643 Times cited 79 Open Access Not_Open_Access
Notes 262348 ESMI; Hercules; FWO Approved (down) Most recent IF: 8.643; 2014 IF: 8.368
Call Number UA @ lucian @ c:irua:115566 Serial 1234
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