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Author De Backer, A.; Jones, L.; Lobato, I.; Altantzis, T.; Goris, B.; Nellist, P.D.; Bals, S.; Van Aert, S.
Title Three-dimensional atomic models from a single projection using Z-contrast imaging: verification by electron tomography and opportunities Type A1 Journal article
Year 2017 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 9 Issue 9 Pages 8791-8798
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract In order to fully exploit structure–property relations of nanomaterials, three-dimensional (3D) characterization at the atomic scale is often required. In recent years, the resolution of electron tomography has reached the atomic scale. However, such tomography typically requires several projection images demanding substantial electron dose. A newly developed alternative circumvents this by counting the number of atoms across a single projection. These atom counts can be used to create an initial atomic model with which an energy minimization can be applied to obtain a relaxed 3D reconstruction of the nanoparticle. Here, we compare, at the atomic scale, this single projection reconstruction approach with tomography and find an excellent agreement. This new approach allows for the characterization of beam-sensitive materials or where the acquisition of a tilt series is impossible. As an example, the utility is illustrated by the 3D atomic scale characterization of a nanodumbbell on an in situ heating holder of limited tilt range.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000404614700031 Publication Date 2017-06-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 33 Open Access OpenAccess
Notes The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0374.13N, G.0369.15N, G.0368.15N, and WO.010.16N) and postdoctoral grants to T. Altantzis, A. De Backer, and B. Goris. S. Bals acknowledges financial support from the European Research Council (Starting Grant No. COLOURATOM 335078). Funding from the European Union Seventh Framework Programme under Grant Agreement 312483 – ESTEEM2 (Integrated Infrastructure Initiatieve-I3) is acknowledged. The authors would also like to thank Luis Liz-Marzán, Marek Grzelczak, and Ana Sánchez-Iglesias for sample provision. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 7.367
Call Number EMAT @ emat @ c:irua:144436UA @ admin @ c:irua:144436 Serial 4617
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Author Schnepf, M.J.; Mayer, M.; Kuttner, C.; Tebbe, M.; Wolf, D.; Dulle, M.; Altantzis, T.; Formanek, P.; Förster, S.; Bals, S.; König, T.A.F.; Fery, A.
Title Nanorattles with tailored electric field enhancement Type A1 Journal article
Year 2017 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 9 Issue 9 Pages 9376-9385
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Nanorattles are metallic core–shell particles with core and shell separated by a dielectric spacer. These

nanorattles have been identified as a promising class of nanoparticles, due to their extraordinary high

electric-field enhancement inside the cavity. Limiting factors are reproducibility and loss of axial symmetry

owing to the movable metal core; movement of the core results in fluctuation of the nanocavity dimensions

and commensurate variations in enhancement factor. We present a novel synthetic approach for

the robust fixation of the central gold rod within a well-defined box, which results in an axisymmetric

nanorattle. We determine the structure of the resulting axisymmetric nanorattles by advanced transmission

electron microscopy (TEM) and small-angle X-ray scattering (SAXS). Optical absorption and scattering

cross-sections obtained from UV-vis-NIR spectroscopy quantitatively agree with finite-difference

time-domain (FDTD) simulations based on the structural model derived from SAXS. The predictions of

high and homogenous field enhancement are evidenced by scanning TEM electron energy loss spectroscopy

(STEM-EELS) measurement on single-particle level. Thus, comprehensive understanding of

structural and optical properties is achieved for this class of nanoparticles, paving the way for photonic

applications where a defined and robust unit cell is crucial.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000405387100015 Publication Date 2017-06-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 69 Open Access OpenAccess
Notes This study was funded by the European Research Council under grant Template-assisted assembly of METAmaterials using MECHanical instabilities (METAMECH) ERC-2012-StG 306686. This work was also supported by the Deutsche Forschungsgemeinschaft (DFG) within the Cluster of Excellence ‘Center for Advancing Electronics Dresden’ (cfaed). M. T. wants to acknowledge funding by the Elite Network of Bavaria, the Bavarian Ministry of State according to the Bavarian elite promotion act (BayEFG), as well as the Alexander von Humboldt Foundation for a Feodor-Lynen Research Fellowship. S. B. acknowledges financial support from the European Research Council (Starting Grant No. COLOURATOM 335078) and T. A. acknowledges funding from the Research Foundation Flanders (FWO, Belgium) through a postdoctoral grant. We thank Ken Harris from the National Research Council Canada for valuable discussion of the manuscript. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 7.367
Call Number EMAT @ emat @ c:irua:144797UA @ admin @ c:irua:144797 Serial 4631
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Author Zheng, G.; Chen, Z.; Sentosun, K.; Pérez-Juste, I.; Bals, S.; Liz-Marzán, L.M.; Pastoriza-Santos, I.; Pérez-Juste, J.; Hong, M.
Title Shape control in ZIF-8 nanocrystals and metal nanoparticles@ZIF-8 heterostructures Type A1 Journal article
Year 2017 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 9 Issue 9 Pages 16645-16651
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Shape control in metal-organic frameworks still remains a challenge. We propose a strategy based on the capping agent modulator method to control the shape of ZIF-8 nanocrystals. This approach requires the use of a surfactant, cetyltrimethylammonium bromide (CTAB), and a second capping agent, tris(hydroxymethyl)aminomethane (TRIS), to obtain ZIF-8 nanocrystals with morphology control in aqueous media. Semiempirical computational simulations suggest that both shape-inducing agents adsorb onto different surface facets of ZIF-8, thereby slowing down their crystal growth rates. While CTAB molecules preferentially adsorb onto the {100} facets, leading to ZIF-8 particles with cubic morphology, TRIS preferentially stabilizes the {111} facets, inducing the formation of octahedral crystals. Interestingly, the presence of both capping agents leads to nanocrystals with irregular shapes and higher index facets, such as hexapods and burr puzzles. Additionally, the combination of ZIF-8 nanocrystals with other materials is expected to impart additional properties due to the hybrid nature of the resulting nanocomposites. In the present case, the presence of CTAB and TRIS molecules as capping agents facilitates the synthesis of metal nanoparticle@ZIF-8 nanocomposites, due to synergistic effects which could be of use in a number of applications such as catalysis, gas sensing and storage.
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Publisher Place of Publication Editor
Language Wos 000414960900015 Publication Date 2017-07-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 109 Open Access OpenAccess
Notes This work was supported by the Ministerio de Economía y Competitividad (MINECO, Spain), under the Grants MAT2013- 45168-R and MAT2016-77809-R. This study was also funded by the Xunta de Galicia/FEDER (ED431C 2016-048). We are grateful to the financial support from National Natural Science Foundation of China (21671010), Guangdong Science and Technology Program (2013A061401002), and Shenzhen Strategic Emerging Industries (KQCX2015032709315529, CXZZ20140419131807788). Approved Most recent IF: 7.367
Call Number EMAT @ emat @c:irua:145827UA @ admin @ c:irua:145827 Serial 4705
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Author Pramanik, G.; Humpolickova, J.; Valenta, J.; Kundu, P.; Bals, S.; Bour, P.; Dracinsky, M.; Cigler, P.
Title Gold nanoclusters with bright near-infrared photoluminescence Type A1 Journal article
Year 2018 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 10 Issue 10 Pages 3792-3798
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The increase in nonradiative pathways with decreasing emission energy reduces the luminescence quantum yield (QY) of near-infrared photoluminescent (NIR PL) metal nanoclusters. Efficient surface ligand chemistry can significantly improve the luminescence QY of NIR PL metal nanoclusters. In contrast to the widely reported but modestly effective thiolate ligand-to-metal core charge transfer, we show that metal-to-ligand charge transfer (MLCT) can be used to greatly enhance the luminescence QY of NIR PL gold nanoclusters (AuNCs). We synthesized water-soluble and colloidally stable NIR PL AuNCs with unprecedentedly high QY (similar to 25%) upon introduction of triphenylphosphonium moieties into the surface capping layer. By using a combination of spectroscopic and theoretical methods, we provide evidence for gold core-to-ligand charge transfer occurring in AuNCs. We envision that this work can stimulate the development of these unusually bright AuNCs for promising optoelectronic, bioimaging, and other applications.
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Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000426148500026 Publication Date 2018-01-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 97 Open Access OpenAccess
Notes ; The authors acknowledge support from the GACR project Nr. 18-12533S. J. V. acknowledges funding from the Ministry of Education, Youth and Sports of the Czech Republic via the V4+Japan project No. 8F15001 (cofinanced by the International Visegrad Fund). P. B. acknowledges GACR project No. 16-05935S and Ministry of Education, Youth and Sports of the Czech Republic project No. LTC17012. ; Approved Most recent IF: 7.367
Call Number UA @ lucian @ c:irua:149901UA @ admin @ c:irua:149901 Serial 4935
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Author Rizzo, F.; Augieri, A.; Kursumovic, A.; Bianchetti, M.; Opherden, L.; Sieger, M.; Huehne, R.; Haenisch, J.; Meledin, A.; Van Tendeloo, G.; MacManus-Driscoll, J.L.; Celentano, G.
Title Pushing the limits of applicability of REBCO coated conductor films through fine chemical tuning and nanoengineering of inclusions Type A1 Journal article
Year 2018 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 10 Issue 17 Pages 8187-8195
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract An outstanding current carrying performance (namely critical current density, J(c)) over a broad temperature range of 10-77 K for magnetic fields up to 12 T is reported for films of YBa2Cu3O7-x with Ba2Y(Nb,Ta)O-6 inclusion pinning centres (YBCO-BYNTO) and thicknesses in the range of 220-500 nm. J(c) values of 10 MA cm(-2) were measured at 30 K – 5 T and 10 K – 9 T with a corresponding maximum of the pinning force density at 10 K close to 1 TN m(-3). The system is very flexible regarding properties and microstructure tuning, and the growth window for achieving a particular microstructure is wide, which is very important for industrial processing. Hence, the dependence of J(c) on the magnetic field angle was readily controlled by fine tuning the pinning microstructure. Transmission electron microscopy (TEM) analysis highlighted that higher growth rates induce more splayed and denser BYNTO nanocolumns with a matching field as high as 5.2 T. Correspondingly, a strong peak at the B||c-axis is noticed when the density of vortices is lower than the nanocolumn density. YBCO-BYNTO is a very robust and reproducible composite system for high-current coated conductors over an extended range of magnetic fields and temperatures.
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Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000432261400037 Publication Date 2018-03-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 9 Open Access OpenAccess
Notes ; This work was partially financially supported by EUROTAPES, a collaborative project funded by the European Commission's Seventh Framework Program (FP7/ 2007-2013) under Grant Agreement No. 280432. This work has been partially carried out within the framework of the EUROfusion Consortium and has received funding from the Euratom research and training programme 2014-2018 under grant agreement no. 633053. The views and opinions expressed herein do not necessarily reflect those of the European Commission. ; Approved Most recent IF: 7.367
Call Number UA @ lucian @ c:irua:151520 Serial 5038
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Author Claes, N.; Asapu, R.; Blommaerts, N.; Verbruggen, S.W.; Lenaerts, S.; Bals, S.
Title Characterization of silver-polymer core–shell nanoparticles using electron microscopy Type A1 Journal article
Year 2018 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 10 Issue 10 Pages 9186-9191
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract Silver-polymer core–shell nanoparticles show interesting optical properties, making them widely applicable in the field of plasmonics. The uniformity, thickness and homogeneity of the polymer shell will affect the properties of the system which makes a thorough structural characterization of these core–shell silver-polymer nanoparticles of great importance. However, visualizing the shell and the particle simultaneously is far from straightforward due to the sensitivity of the polymer shell towards the electron beam. In this study, we use different 2D and 3D electron microscopy techniques to investigate different structural aspects of the polymer coating.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000437007700028 Publication Date 2018-04-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 11 Open Access OpenAccess
Notes N. C. and S. B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS) and from the FWO through project funding (G038116N). R. A. and S. L. acknowledge the Research Foundation Flanders (FWO) for financial support. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ECAS_Sara Approved Most recent IF: 7.367
Call Number EMAT @ emat @c:irua:151290UA @ admin @ c:irua:151290 Serial 4959
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Author Ata, I.; Ben Dkhil, S.; Pfannmoeller, M.; Bals, S.; Duche, D.; Simon, J.-J.; Koganezawa, T.; Yoshimoto, N.; Videlot-Ackermann, C.; Margeat, O.; Ackermann, J.; Baeuerle, P.
Title The influence of branched alkyl side chains in A-D-A oligothiophenes on the photovoltaic performance and morphology of solution-processed bulk-heterojunction solar cells Type A1 Journal article
Year 2017 Publication Organic chemistry frontiers : an international journal of organic chemistry Abbreviated Journal Org Chem Front
Volume 4 Issue 4 Pages 1561-1573
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Besides providing sufficient solubility, branched alkyl chains also affect the film-forming and packing properties of organic semiconductors. In order to avoid steric hindrance as it is present in wide-spread alkyl chains comprising a branching point position at the C2-position, i.e., 2-ethylhexyl, the branching point can be moved away from the pi-conjugated backbone. In this report, we study the influence of the modification of the branching point position from the C2-position in 2-hexyldecylamine (1) to the C4-position in 4-hexyldecylamine (2) connected to the central dithieno[3,2-b: 2', 3'-d] pyrrole (DTP) moiety in a well-studied A-D-A oligothiophene on the optoelectronic properties and photovoltaic performance in solution- processed bulk heterojunction solar cells (BHJSCs) with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as the acceptor material. Post-treatment of the photoactive layers is performed via solvent vapor annealing (SVA) in order to improve the film microstructure of the bulk heterojunction. The time evolution of nanoscale morphological changes is followed by combining scanning transmission electron microscopy with low-energy-loss spectroscopic imaging (STEM-SI), solid-state absorption spectroscopy, and two-dimensional grazing incidence X-ray diffraction (2D-GIXRD). Our results show an improvement of the photovoltaic performance that is dependent on the branching point position in the donor oligomer. Optical spacers are utilized to increase light absorption inside the co-oligomer 2-based BHJSCs leading to increased power conversion efficiencies (PCEs) of 8.2% when compared to the corresponding co-oligomer 1-based devices. A STEM-SI analysis of the respective device cross-sections of active layers containing 1 and 2 as donor materials indeed reveals significant differences in their respective active layer morphologies.
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Publisher RSC Publishing Place of Publication London Editor
Language Wos 000406374800013 Publication Date 2017-05-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2052-4129 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.955 Times cited 24 Open Access OpenAccess
Notes ; We acknowledge financial support by the European Commission under the project “SUNFLOWER” (FP7-ICT-2011-7, grant number: 287594) and S.B. acknowledges the ERC Starting Grant Colouratoms (335078). ; Approved Most recent IF: 4.955
Call Number UA @ lucian @ c:irua:145176UA @ admin @ c:irua:145176 Serial 4727
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Author Ulu Okudur, F.; D'Haen, J.; Vranken, T.; De Sloovere, D.; Verheijen, M.; Karakulina, O.M.; Abakumov, A.M.; Hadermann, J.; Van Bael, M.K.; Hardy, A.
Title Ti surface doping of LiNi0.5Mn1.5O4−δpositive electrodes for lithium ion batteries Type A1 Journal article
Year 2018 Publication RSC advances Abbreviated Journal Rsc Adv
Volume 8 Issue 13 Pages 7287-7300
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The particle surface of LiNi0.5Mn1.5O4−δ (LNMO), a Li-ion battery cathode material, has been modified by Ti cation doping through a hydrolysis–condensation reaction followed by annealing in oxygen. The effect of different annealing temperatures (500–850 °C) on the Ti distribution and electrochemical performance of the surface modified LNMO was investigated. Ti cations diffuse from the preformed amorphous ‘TiOx’ layer into the LNMO surface during annealing at 500 °C. This results in a 2–4 nm thick Ti-rich spinel surface having lower Mn and Ni content compared to the core of the LNMO particles, which was observed with scanning transmission electron microscopy coupled with compositional EDX mapping. An increase in the annealing temperature promotes the formation of a Ti bulk doped LiNi(0.5−w)Mn(1.5+w)−tTitO4 phase and Ti-rich LiNi0.5Mn1.5−yTiyO4 segregates above 750 °C. Fourier-transform infrared spectrometry indicates increasing Ni–Mn ordering with annealing temperature, for both bare and surface modified LNMO. Ti surface modified LNMO annealed at 500 °C shows a superior cyclic stability, coulombic efficiency and rate performance compared to bare LNMO annealed at 500 °C when cycled at 3.4–4.9 V vs. Li/Li+. The improvements are probably due to suppressed Ni and Mn dissolution with Ti surface doping.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000425508900064 Publication Date 2018-02-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2046-2069 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.108 Times cited 9 Open Access OpenAccess
Notes This research is supported by the Research Foundation Flanders (FWO Vlaanderen, grant number G040116N). This project receives the support of the European Union, the European Regional Development Fund ERDF, Flanders Innovation & Entrepreneurship and the Province of Limburg (project 936). Greet Cuyvers and Gilles Bonneux (UHasselt) are acknowledged for the ICP-AES sample preparation and measurements. Vera Meynen and Karen Leyssens (Antwerp University, Belgium) are acknowledged for the BET measurements. Special thanks to Bart Ruttens (UHasselt) for XRD measurements and discussions on the refinements. Approved Most recent IF: 3.108
Call Number EMAT @ emat @c:irua:149513 Serial 4905
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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.
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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 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 Serrano-Sevillano, J.; Reynaud, M.; Saracibar, A.; Altantzis, T.; Bals, S.; van Tendeloo, G.; Casas-Cabanas, M.
Title Enhanced electrochemical performance of Li-rich cathode materials through microstructural control Type A1 Journal article
Year 2018 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 20 Issue 20 Pages 23112-23122
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The microstructural complexity of Li-rich cathode materials has so far hampered understanding the critical link between size, morphology and structural defects with both capacity and voltage fadings that this family of materials exhibits. Li2MnO3 is used here as a model material to extract reliable structure–property

relationships that can be further exploited for the development of high-performing and long-lasting Li-rich oxides. A series of samples with microstructural variability have been prepared and thoroughly characterized using the FAULTS software, which allows quantification of planar defects and extraction of

average crystallite sizes. Together with transmission electron microscopy (TEM) and density functional theory (DFT) results, the successful application of FAULTS analysis to Li2MnO3 has allowed rationalizing the synthesis conditions and identifying the individual impact of concurrent microstructural features on

both voltage and capacity fadings, a necessary step for the development of high-capacity Li-ion cathode materials with enhanced cycle life.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000445220500071 Publication Date 2018-08-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 36 Open Access OpenAccess
Notes This work was supported by the Spanish Ministerio de la Economı´a y de la Competitividad through the project IONSTORE (MINECO ref. ENE2016-81020-R). The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement 312483 – ESTEEM2 (Integrated Infrastructure Initiative-I3). JSS and AS are grateful for computing time provided by the Spanish i2Basque Centers. MR acknowledges the Spanish State for its financial support through her post-doctoral grant Juan de la Cierva – Formacio´n (MINECO ref. FJCI-2014-19990) and her international mobility grant Jose´ Castillejos (MECD ref. CAS15/00354). S. B. acknowledges funding from the European Research Council (ERC starting grant #335078 Colouratom) and T. A. a postdoctoral grant from the Research Foundation Flanders (FWO). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ecas_sara Approved Most recent IF: 4.123
Call Number EMAT @ emat @c:irua:154782UA @ admin @ c:irua:154782 Serial 5062
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Author Mefford, J.T.; Kurilovich, A.A.; Saunders, J.; Hardin, W.G.; Abakumov, A.M.; Forslund, R.P.; Bonnefont, A.; Dai, S.; Johnston, K.P.; Stevenson, K.J.
Title Decoupling the roles of carbon and metal oxides on the electrocatalytic reduction of oxygen on La1-xSrxCoO3-\delta perovskite composite electrodes Type A1 Journal article
Year 2019 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 21 Issue 6 Pages 3327-3338
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Perovskite oxides are active room-temperature bifunctional oxygen electrocatalysts in alkaline media, capable of performing the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with lower combined overpotentials relative to their precious metal counterparts. However, their semiconducting nature necessitates the use of activated carbons as conductive supports to generate applicably relevant current densities. In efforts to advance the performance and theory of oxide electrocatalysts, the chemical and physical properties of the oxide material often take precedence over contributions from the conductive additive. In this work, we find that carbon plays an important synergistic role in improving the performance of La1-xSrxCoO3- (0 x 1) electrocatalysts through the activation of O-2 and spillover of radical oxygen intermediates, HO2- and O-2(-), which is further reduced through chemical decomposition of HO2- on the perovskite surface. Through a combination of thin-film rotating disk electrochemical characterization of the hydrogen peroxide intermediate reactions (hydrogen peroxide reduction reaction (HPRR), hydrogen peroxide oxidation reaction (HPOR)) and oxygen reduction reaction (ORR), surface chemical analysis, HR-TEM, and microkinetic modeling on La1-xSrxCoO3- (0 x 1)/carbon (with nitrogen and non-nitrogen doped carbons) composite electrocatalysts, we deconvolute the mechanistic aspects and contributions to reactivity of the oxide and carbon support.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000459584900049 Publication Date 2019-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076; 1463-9084 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 5 Open Access OpenAccess
Notes ; Financial support for this work was provided by the R. A. Welch Foundation (grants F-1529 and F-1319). S. D. was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. ; Approved Most recent IF: 4.123
Call Number UA @ admin @ c:irua:158625 Serial 5244
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Author Hasanli, N.; Gauquelin, N.; Verbeeck, J.; Hadermann, J.; Hayward, M.A.
Title Small-moment paramagnetism and extensive twinning in the topochemically reduced phase Sr2ReLiO5.5 Type A1 Journal article
Year 2018 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T
Volume 47 Issue 44 Pages 15783-15790
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Reaction of the cation-ordered double perovskite Sr2ReLiO6 with dilute hydrogen at 475 degrees C leads to the topochemical deintercalation of oxide ions from the host lattice and the formation of a phase of composition Sr2ReLiO5.5, as confirmed by thermogravimetric and EELS data. A combination of neutron and electron diffraction data reveals the reduction process converts the -Sr2O2-ReLiO4-Sr2O2-ReLiO4- stacking sequence of the parent phase into a -Sr2O2-ReLiO3-Sr2O2-ReLiO4-, partially anion-vacant ordered sequence. Furthermore a combination of electron diffraction and imaging reveals Sr2ReLiO5.5 exhibits extensive twinning – a feature which can be attributed to the large, anisotropic volume expansion of the material on reduction. Magnetisation data reveal a strongly reduced moment of (eff) = 0.505(B) for the d(1) Re6+ centres in the phase, suggesting there remains a large orbital component to the magnetism of the rhenium centres, despite their location in low symmetry coordination environments.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000450208000019 Publication Date 2018-10-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1477-9226 ISBN Additional Links UA library record; WoS full record
Impact Factor 4.029 Times cited Open Access Not_Open_Access
Notes Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE13284). Experiments at the ISIS pulsed neutron facility were supported by a beam time allocation from the STFC. NH acknowledges funding from the “State Programme on Education of Azerbaijani Youth Abroad in 2007-2015” by the Ministry of Education of Azerbaijan. 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. Approved Most recent IF: 4.029
Call Number EMAT @ emat @c:irua:155771 Serial 5137
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Author Barreca, D.; Gri, F.; Gasparotto, A.; Carraro, G.; Bigiani, L.; Altantzis, T.; Žener, B.; Lavrenčič Štangar, U.; Alessi, B.; Padmanaban, D.B.; Mariotti, D.; Maccato, C.
Title Multi-functional MnO2nanomaterials for photo-activated applications by a plasma-assisted fabrication route Type A1 Journal article
Year 2019 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 11 Issue 1 Pages 98-108
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Supported MnO2-based nanomaterials were fabricated on fluorine-doped tin oxide substrates by plasma enhanced-chemical vapor deposition (PE-CVD) between 100 °C and 400 °C, starting from a fluorinated Mn(II) diamine diketonate precursor. Growth experiments yielded -MnO2 nanosystems with hierarchical morphology tuneable from dendritic structures to quasi-1D nanosystems as a function of growth temperature, whose variation enabled also a concomitant tailoring of the system fluorine content, and of the optical absorption and band gap. Preliminary photocatalytic tests were aimed at the investigation of photoinduced hydrophilic (PH) and solid phase photocatalytic (PC) performances of the present nanomaterials, as well as at the photodegradation of Plasmocorinth B azo-dye aqueous solutions. The obtained findings highlighted an attractive system photoactivity even under visible light, finely tailored by fluorine content, morphological organization and optical properties of the prepared nanostructures. The results indicate that the synthesized MnO2 nanosystems have potential applications as advanced smart materials for anti-fogging/self-cleaning end uses and water purification.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000454327500037 Publication Date 2018-10-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 7 Open Access OpenAccess
Notes Padova University DOR 2016–2017, P-DiSC #03BIRD2016-UNIPD projects, HERALD Cost Action MP1402 – 37831 and ACTION post-doc fellowship are acknowledged for financial support. T.A. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO). Thanks are also due to Prof. Sara Bals (EMAT, University of Antwerp, Belgium), Prof. Romana Cerc Korošec and to Dr. Lev Matoh (University of Ljubljana, Slovenia), and to Prof. Elza Bontempi (Brescia University, Italy). The work was also supported by EPSRC (award EP/R008841/1, EP/M024938/1). Approved Most recent IF: 7.367
Call Number EMAT @ emat @UA @ admin @ c:irua:156388 Serial 5148
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Author Vanrompay, H.; Bladt, E.; Albrecht, W.; Béché, A.; Zakhozheva, M.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Bals, S.
Title 3D characterization of heat-induced morphological changes of Au nanostars by fast in situ electron tomography Type A1 Journal article
Year 2018 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 10 Issue 10 Pages 22792-22801
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract A thorough understanding of the thermal stability and potential reshaping of anisotropic gold nanostars is required for various potential applications. Combination of a tomographic heating holder with fast tilt series acquisition has been used to monitor temperature-induced morphological changes of Au nanostars. The outcome of our 3D investigations can be used as an input for boundary element method simulations, enabling us to investigate the influence of reshaping on the nanostars’ plasmonic properties. Our work leads to a better understanding of the mechanism behind thermal reshaping. In addition, the approach presented here is generic and can hence be applied to a wide variety of nanoparticles made of different materials and with arbitrary morphology.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000453248100010 Publication Date 2018-11-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 55 Open Access OpenAccess
Notes H.V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020. The authors acknowledge funding from European Commission Grant (EUSMI 731019 to S.B., L.M.L.-M. and M.Z. and MUMMERING 765604 to S.B. and M.Z.). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #335078- COLOURATOMS).; Ecas_sara Approved Most recent IF: 7.367
Call Number EMAT @ emat @c:irua:155718UA @ admin @ c:irua:155718 Serial 5071
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Author Tonkikh, A.A.; Tsebro, V.I.; Obraztsova, E.A.; Rybkovskiy, D.V.; Orekhov, A.S.; Kondrashov, I.I.; Kauppinen, E.I.; Chuvilin, A.L.; Obraztsova, E.D.
Title Films of filled single-wall carbon nanotubes as a new material for high-performance air-sustainable transparent conductive electrodes operating in a wide spectral range Type A1 Journal article
Year 2019 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 11 Issue 14 Pages 6755-6765
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract In this paper we show the advantages of transparent high conductive films based on filled single-wall carbon nanotubes. The nanotubes with internal channels filled with acceptor molecules (copper chloride or iodine) form networks demonstrating significantly improved characteristics. Due to the charge transfer between the nanotubes and filler, the doped-nanotube films exhibit a drop in electrical sheet resistance of an order of magnitude together with a noticeable increase of film transparency in the visible and near-infrared spectral range. The thermoelectric power measurements show a significant improvement of air-stability of the nanotube network in the course of the filling procedure. For the nanotube films with an initial transparency of 87% at 514 nm and electrical sheet resistance of 862 Ohm sq(-1) we observed an improvement of transparency up to 91% and a decrease of sheet resistance down to 98 Ohm sq(-1). The combination of the nanotube synthesis technique and molecules for encapsulation has been optimized for applications in optoelectronics.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000464454400024 Publication Date 2019-03-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 2 Open Access Not_Open_Access: Available from 06.09.2019
Notes ; The work was supported by the RFBR project 18-29-19113-mk, grant no. 311533 of Academy of Finland, Russian Federation President Program for young scientist MK-3140.2018.2. Also, the reported study was funded by RFBR and Moscow city Government according to the research project no. 19-32-70004. TEM measurements were performed with financial support from the Ministry of Science and Higher Education of the Russian Federation within the state assignment for the Federal Scientific Research Centre “Crystallography and Photonics” of the Russian Academy of Sciences. ; Approved Most recent IF: 7.367
Call Number UA @ admin @ c:irua:159339 Serial 5249
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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.
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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 Most recent IF: 8.668
Call Number UA @ admin @ c:irua:159403 Serial 5259
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Author Mourdikoudis, S.; Montes-Garcia, V.; Rodal-Cedeira, S.; Winckelmans, N.; Perez-Juste, I.; Wu, H.; Bals, S.; Perez-Juste, J.; Pastoriza-Santos, I.
Title Highly porous palladium nanodendrites : wet-chemical synthesis, electron tomography and catalytic activity Type A1 Journal article
Year 2019 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal
Volume 48 Issue 48 Pages 3758-3767
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A simple procedure to obtain highly porous hydrophilic palladium nanodendrites in one-step is described. The synthetic strategy is based on the thermal reduction of a Pd precursor in the presence of a positively charged polyelectrolyte such as polyethylenimine (PEI). Advanced electron microscopy techniques combined with X-ray diffraction (XRD), thermogravimetry and BET analysis demonstrate the polycrystalline nature of the nanodendrites as well as their high porosity and active surface area, facilitating a better understanding of their unique morphology. Besides, catalytic studies performed using Raman scattering and UV-Vis spectroscopies revealed that the nanodendrites exhibit a superior performance as recyclable catalysts towards hydrogenation reaction compared to other noble metal nanoparticles.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000461088700027 Publication Date 2019-02-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0300-9246; 1477-9226; 1472-7773 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 23 Open Access OpenAccess
Notes ; This work was supported by the Ministerio de Economia y Competitividad (MINECO, Spain) under the Grant MAT2016-77809-R, Xunta de Galicia (GRC ED431C 2016-048 and Centro Singular de Investigacion de Galicia (ED431G/02)) and Fundacion Ramon Areces (SERSforSafety). S. M. acknowledges funding from the General Secretariat for Research and Technology in Greece (Project PE4 (1546)). S. B. and N. W. acknowledge financial support by the European Research Council (ERC Starting Grant #335078-COLOURATOMS). We thank the EPSRC CNIE Research Facility (EPSRC Award, EP/K038656/1) at the University College London for the collection of the BET data. Authors thank J. Millos for the XRD measurements. ; Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:158530 Serial 5251
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Author Yu, S.; Sankaran, K.J.; Korneychuk, S.; Verbeeck, J.; Haenen, K.; Jiang, X.; Yang, N.
Title High-performance supercabatteries using graphite@diamond nano-needle capacitor electrodes and redox electrolytes Type A1 Journal article
Year 2019 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 11 Issue 38 Pages 17939-17946
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Supercabatteries have the characteristics of supercapacitors and batteries, namely high power and energy densities as well as long cycle life. To construct them, capacitor electrodes with wide potential windows and/or redox electrolytes are required. Herein, graphite@diamond nano-needles and an aqueous solution of Fe(CN)(6)(3-/4-) are utilized as the capacitor electrode and the electrolyte, respectively. This diamond capacitor electrode has a nitrogen-doped diamond core and a nano-graphitic shell. In 0.05 M Fe(CN)(6)(3-/4-) + 1.0 M Na2SO4 aqueous solution, the fabricated supercabattery has a capacitance of 66.65 mF cm(-2) at a scan rate of 10 mV s(-1). It is stable over 10 000 charge/discharge cycles. The symmetric supercabattery device assembled using a two-electrode system possesses energy and power densities of 10.40 W h kg(-1) and 6.96 kW kg(-1), respectively. These values are comparable to those of other energy storage devices. Therefore, diamond supercabatteries are promising for many industrial applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000489646900036 Publication Date 2019-09-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 26 Open Access
Notes ; S. Yu and K. J. Sankaran contributed equally to this work. N. Yang acknowledges funding from the German Science Foundation under the project of YA344/1-1. J. Verbeeck and S. Korneychuk acknowledge the funding from the GOA project “Solarpaint” of the University of Antwerp. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. K. J. Sankaran and K. Haenen like to acknowledge the financial support of the Methusalem “NANO” network. S. Yu likes to acknowledge the financial support from fundamental research funds for the central universities (Grant No. SWU019001). ; Approved Most recent IF: 7.367
Call Number UA @ admin @ c:irua:163723 Serial 5388
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Author Daems, N.; De Mot, B.; Choukroun, D.; Van Daele, K.; Li, C.; Hubin, A.; Bals, S.; Hereijgers, J.; Breugelmans, T.
Title Nickel-containing N-doped carbon as effective electrocatalysts for the reduction of CO2 to CO in a continuous-flow electrolyzer Type A1 Journal article
Year 2019 Publication Sustainable energy & fuels Abbreviated Journal
Volume 4 Issue 4 Pages 1296-1311
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Nickel-containing N-doped carbons were synthesized for the electrochemical reduction of CO2 to CO, which is a promising approach to reduce the atmospheric CO2 levels and its negative impact on the environment. Unfortunately, poor performance (activity, selectivity and/or stability) is still a major hurdle for the economical implementation of this type of materials. The electrocatalysts were prepared through an easily up-scalable and easily tunable method based on the pyrolysis of Ni-containing N-doped carbons. Ni–N–AC–B1 synthesized with a high relative amount of nitrogen and nickel with respect to carbon, was identified as the most promising candidate for this reaction based on its partial CO current density (4.2 mA cm−2), its overpotential (0.57 V) and its faradaic efficiency to CO (>99%). This results in unprecedented values for the current density per g active sites (690 A g−1 active sites). Combined with its decent stability and its high performance in an actual electrolyzer setup, this makes it a promising candidate for the electrochemical reduction of CO2 to CO on a larger scale. Finally, the evaluation of this kind of material in a flow-cell setup has been limited and to the best of our knowledge never included an evaluation of several crucial parameters (e.g. electrolyte type, anode composition and membrane type) and is an essential investigation in the move towards up-scaling and ultimately industrial application of this technique. This study resulted in an optimal cell configuration, consisting of Pt as an anode, Fumatech® as the membrane and 1 M KHCO3 and 2 M KOH as catholyte and anolyte, respectively. In conclusion, this research offers a unique combination of electrocatalyst development and reactor optimization.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000518690900030 Publication Date 2019-12-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 14 Open Access OpenAccess
Notes ; The authors acknowledge sponsoring from the research foundation of Flanders (FWO) in the frame of a post-doctoral grant (12Y3919N – ND). J. Hereijgers was supported through a postdoctoral fellowship (28761) of the Research Foundation Flanders (FWO). This project was co-funded by the Interreg 2 Seas-Program 2014-2020, co-.nanced by the European Fund for Regional Development in the frame of subsidiary contract nr 2S03-019. This work was further performed in the framework of the Catalisti cluster SBO project CO2PERATE (“All renewable CCU based on formic acid integrated in an industrial microgrid”), with the.nancial support of VLAIO (Flemish Agency for Innovation and Entrepreneurship). This project.nally received funding from the European Research Council (ERC Consolidator Grant 815128, REALNANO). We thank Karen Leyssens for helping with the N<INF>2</INF> physisorption measurements and Kitty Baert (VUB) for analyzing the samples with XPS and Raman. ; sygma Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:165482 Serial 6311
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Author Spreitzer, M.; Klement, D.; Egoavil, R.; Verbeeck, J.; Kovac, J.; Zaloznik, A.; Koster, G.; Van Tendeloo, G.; Suvorov, D.; Rijnders, G.
Title Growth mechanism of epitaxial SrTiO3 on a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface Type A1 Journal article
Year 2020 Publication Journal Of Materials Chemistry C Abbreviated Journal J Mater Chem C
Volume 8 Issue 2 Pages 518-527
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sub-monolayer control over the growth at silicon-oxide interfaces is a prerequisite for epitaxial integration of complex oxides with the Si platform, enriching it with a variety of functionalities. However, the control over this integration is hindered by the intense reaction of the constituents. The most suitable buffer material for Si passivation is metallic strontium. When it is overgrown with a layer of SrTiO3 (STO) it can serve as a pseudo-substrate for the integration with functional oxides. In our study we determined a mechanism for epitaxial integration of STO with a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface using all-pulsed laser deposition (PLD) technology. A detailed analysis of the initial deposition parameters was performed, which enabled us to develop a complete protocol for integration, taking into account the peculiarities of the PLD growth, STO critical thickness, and process thermal budget, in order to kinetically trap the reaction between STO and Si and thus to minimize the thickness of the interface layer. The as-prepared oxide layer exhibits STO(001)8Si(001) out-of-plane and STO[110]8Si[100] in-plane orientation and together with recent advances in large-scale PLD tools these results represent a new technological solution for the implementation of oxide electronics on demand.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000506852400036 Publication Date 2019-10-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7526; 2050-7534 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited 12 Open Access OpenAccess
Notes ; The research was financially supported by the Slovenian Research Agency (Project No. P2-0091, J2-9237) and Ministry of Education, Science and Sport of the Republic of Slovenia (SIOX projects). This work was also funded by the European Union Council under the 7th Framework Program grant no. NMP3-LA-2010-246102 IFOX. J. V. and G. V. T. acknowledge funding from the Fund for Scientific Research Flanders under project no. G.0044.13N. ; Approved Most recent IF: 6.4; 2020 IF: 5.256
Call Number UA @ admin @ c:irua:165672 Serial 6298
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Author Sanchis-Gual, R.; Susic, I.; Torres-Cavanillas, R.; Arenas-Esteban, D.; Bals, S.; Mallah, T.; Coronado-Puchau, M.; Coronado, E.
Title The design of magneto-plasmonic nanostructures formed by magnetic Prussian Blue-type nanocrystals decorated with Au nanoparticles Type A1 Journal article
Year 2021 Publication Chemical Communications Abbreviated Journal Chem Commun
Volume 57 Issue 15 Pages 1903-1906
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We have developed a general protocol for the preparation of hybrid nanostructures formed by nanoparticles (NPs) of molecule-based magnets based on Prussian Blue Analogues (PBAs) decorated with plasmonic Au NPs of different shapes. By adjusting the pH, Au NPs can be attached preferentially along the edges of the PBA or randomly on the surface. The protocol allows tuning the plasmonic properties of the hybrids in the whole visible spectrum.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000620719300011 Publication Date 2021-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-7345 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.319 Times cited 5 Open Access OpenAccess
Notes European Commission, COST Action MOLSPIN CA15128 ERC Advanced Grant Mol-2D 788222 ERC Consolidator Grant REALNANO 815128 Grant Agreement No. 731019 (EUSMI) ; Ministry of Education and Science of the Russian Federation, No. 14.W03.31.0001 ; Ministerio de Ciencia, Innovación y Universidades, Maria de Maeztu CEX2019-000919-M Project MAT2017-89993-R ; Generalitat Valenciana, PROMETEO/2017/066 iDiFEDER/2018/061 ; sygma; Approved Most recent IF: 6.319
Call Number EMAT @ emat @c:irua:176542 Serial 6702
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Author Mazzeo, P.P.; Canossa, S.; Carraro, C.; Pelagatti, P.; Bacchi, A.
Title Systematic coformer contribution to cocrystal stabilization: energy and packing trends Type A1 Journal article
Year 2020 Publication Crystengcomm Abbreviated Journal Crystengcomm
Volume 22 Issue 43 Pages 7341-7349
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Polycyclic aromatic compounds such as acridine and phenazine are popular molecular partners used in cocrystal synthesis. The intermolecular interactions occurring between coformers and their molecular partners dominate the cocrystal packing energy, but coformer self-interactions might participate with a constant non-negligible contribution to the overall packing energy stabilization. Two new acridine-based cocrystals have been mechanochemically synthesized, then fully characterized<italic>via</italic>DSC and SCXRD analyses. A statistical analysis in the CSD has been performed to evaluate the recurrent π–π stacking orientation of polycyclic coformers in all deposited acridine-based cocrystals, then extended to phenazine-base analogs. Packing energy calculations were performed on a selected cocrystal subset to quantify the contribution of the π–π interaction to the overall stabilization energy.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000589506600017 Publication Date 2020-03-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1466-8033 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.1 Times cited Open Access OpenAccess
Notes European Cooperation in Science and Technology, CA18112 ; Ministero delle Politiche Agricole Alimentari e Forestali, PAC/Packaging Attivo Cristallino ; Approved Most recent IF: 3.1; 2020 IF: 3.474
Call Number EMAT @ emat @c:irua:174262 Serial 6661
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Author Paulus, A.; Hendrickx, M.; Bercx, M.; Karakulina, O.M.; Kirsanova, M.A.; Lamoen, D.; Hadermann, J.; Abakumov, A.M.; Van Bael, M.K.; Hardy, A.
Title An in-depth study of Sn substitution in Li-rich/Mn-rich NMC as a cathode material for Li-ion batteries Type A1 Journal article
Year 2020 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal
Volume 49 Issue 30 Pages 10486-10497
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Layered Li-rich/Mn-rich NMC (LMR-NMC) is characterized by high initial specific capacities of more than 250 mA h g(-1), lower cost due to a lower Co content and higher thermal stability than LiCoO2. However, its commercialisation is currently still hampered by significant voltage fade, which is caused by irreversible transition metal ion migration to emptied Li positionsviatetrahedral interstices upon electrochemical cycling. This structural change is strongly correlated with anionic redox chemistry of the oxygen sublattice and has a detrimental effect on electrochemical performance. In a fully charged state, up to 4.8 Vvs.Li/Li+, Mn4+ is prone to migrate to the Li layer. The replacement of Mn4+ for an isovalent cation such as Sn4+ which does not tend to adopt tetrahedral coordination and shows a higher metal-oxygen bond strength is considered to be a viable strategy to stabilize the layered structure upon extended electrochemical cycling, hereby decreasing voltage fade. The influence of Sn4+ on the voltage fade in partially charged LMR-NMC is not yet reported in the literature, and therefore, we have investigated the structure and the corresponding electrochemical properties of LMR-NMC with different Sn concentrations. We determined the substitution limit of Sn4+ in Li1.2Ni0.13Co0.13Mn0.54-xSnxO2 by powder X-ray diffraction and transmission electron microscopy to be x approximate to 0.045. The limited solubility of Sn is subsequently confirmed by density functional theory calculations. Voltage fade for x= 0 andx= 0.027 has been comparatively assessed within the 3.00 V-4.55 V (vs.Li/Li+) potential window, from which it is concluded that replacing Mn4+ by Sn4+ cannot be considered as a viable strategy to inhibit voltage fade within this window, at least with the given restricted doping level.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000555330900018 Publication Date 2020-07-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0300-9246; 1477-9226; 1472-7773 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4 Times cited Open Access OpenAccess
Notes ; The authors acknowledge Research Foundation Flanders (FWO) project number G040116N for funding. The authors are grateful to Dr Ken Elen and Greet Cuyvers (imo-imomec, UHasselt and imec) for respectively preliminary PXRD measurements and performing ICP-AES on the monometal precursors. Dr Dmitry Rupasov (Skolkovo Institute of Science and Technology) is acknowledged for performing TGA measurements on the metal sulfate precursors. 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 Most recent IF: 4; 2020 IF: 4.029
Call Number UA @ admin @ c:irua:171149 Serial 6450
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Author Reguera, J.; Flora, T.; Winckelmans, N.; Rodriguez-Cabello, J.C.; Bals, S.
Title Self-assembly of Janus Au:Fe₃O₄ branched nanoparticles. From organized clusters to stimuli-responsive nanogel suprastructures Type A1 Journal article
Year 2020 Publication Nanoscale Advances Abbreviated Journal
Volume 2 Issue 6 Pages 2525-2530
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Janus nanoparticles offer enormous possibilities through a binary selective functionalization and dual properties. Their self-assembly has attracted strong interest due to their potential as building blocks to obtain molecular colloids, supracrystals and well-organized nanostructures that can lead to new functionalities. However, this self-assembly has been focused on relatively simple symmetrical morphologies, while for complex nanostructures this process has been unexplored. Here, we study the assembly of plasmonic-magnetic Janus nanoparticles with a branched (nanostar) – sphere morphology. The branched morphology enhances their plasmonic properties in the near-infrared region and therefore their applicability, but at the same time constrains their self-assembly capabilities to obtain more organized or functional suprastructures. We describe the self-assembly of these nanoparticles after amphiphilic functionalization. The role of the nanoparticle branching, as well as the size of the polymer-coating, is explored. We show how the use of large molecular weight stabilizing polymers can overcome the anisotropy of the nanoparticles producing a change in the morphology from small clusters to larger quasi-cylindrical nanostructures. Finally, the Janus nanoparticles are functionalized with a thermo-responsive elastin-like recombinamer. These nanoparticles undergo reversible self-assembly in the presence of free polymer giving rise to nanoparticle-stabilized nanogel-like structures with controlled size, providing the possibility to expand their applicability to multi-stimuli controlled self-assembly.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000543283200032 Publication Date 2020-04-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2516-0230 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.7 Times cited 10 Open Access OpenAccess
Notes ; J. R. acknowledges the.nancial support of Basque Country Elkartek-KK-2019/ 00101. T. F. and J. C. R-C acknowledge the funding from the European Commission (NMP-2014-646075), the Spanish Government (PCIN-2015-010 (FunBioPlas), MAT2016-78903-R), Junta de Castilla y Leon (VA317P18) and Centro en Red de Medicina Regenerativa y Terapia Celular de Castilla y Leon. ; Approved Most recent IF: 4.7; 2020 IF: NA
Call Number UA @ admin @ c:irua:170773 Serial 6600
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Author Payne, L.M.; Albrecht, W.; Langbein, W.; Borri, P.
Title The optical nanosizer – quantitative size and shape analysis of individual nanoparticles by high-throughput widefield extinction microscopy Type A1 Journal article
Year 2020 Publication Nanoscale Abbreviated Journal Nanoscale
Volume Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Nanoparticles are widely utilised for a range of applications, from catalysis to medicine, requiring accurate knowledge of their size and shape. Current techniques for particle characterisation are either not very accurate or time consuming and expensive. Here we demonstrate a rapid and quantitative method for particle analysis based on measuring the polarisation-resolved optical extinction cross-section of hundreds of individual nanoparticles using wide-field microscopy, and determining the particle size and shape from the optical properties. We show measurements on three samples consisting of nominally spherical gold nanoparticles of 20 nm and 30 nm diameter, and gold nanorods of 30 nm length and 10 nm diameter. Nanoparticle sizes and shapes in three dimensions are deduced from the measured optical cross-sections at different wavelengths and light polarisation, by solving the inverse problem, using an ellipsoid model of the particle polarisability in the dipole limit. The sensitivity of the method depends on the experimental noise and the choice of wavelengths. We show an uncertainty down to about 1 nm in mean diameter, and 10% in aspect ratio when using two or three color channels, for a noise of about 50 nm<sup>2</sup>in the measured cross-section. The results are in good agreement with transmission electron microscopy, both 2D projection and tomography, of the same sample batches. Owing to its combination of experimental simplicity, ease of access to statistics over many particles, accuracy, and geometrical particle characterisation in 3D, this “optical nanosizer” method has the potential to become the technique of choice for quality control in next-generation particle manufacturing.
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Language Wos 000558928800022 Publication Date 2020-07-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited Open Access OpenAccess
Notes This work was supported by a Welsh Government Life Sciences Bridging Fund (grant LSBF/R6-005) and by the UK EPSRC (grant no. EP/I005072/1 and EP/M028313/1). PB acknowledges the Royal Society for her Wolfson research merit award (grant WM140077). The authors acknowledge funding from the European Commission (Grant EUSMI E191000350). WA acknowledges an Individual Fellowship from the Marie Sklodowska-Curie actions (MSCA) under the EU’s Horizon 2020 program (Grant 797153, SOPMEN), and Sara Bals for supporting the STEM measurements. The bright-field TEM was performed by Thomas Davies at Cardiff University. We acknowledge Attilio Zilli for helpful discussions and contributions in calculating the relative field strengths in the illumination and finite-element simulation of cross-sections shown in the ESI.† We acknowledge Iestyn Pope for technical support of the optical equipment. Approved Most recent IF: 6.7; 2020 IF: 7.367
Call Number UA @ lucian @c:irua:170485 Serial 6397
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Author Geerts, L.; Geerts-Claes, H.; Skorikov, A.; Vermeersch, J.; Vanbutsele, G.; Galvita, V.; Constales, D.; Chandran, C.V.; Radhakrishnan, S.; Seo, J.W.; Breynaert, E.; Bals, S.; Sree, S.P.; Martens, J.A.
Title Spherical core–shell alumina support particles for model platinum catalysts Type A1 Journal article
Year 2021 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 13 Issue 7 Pages 4221-4232
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract γ- and δ-alumina are popular catalyst support materials. Using a hydrothermal synthesis method starting from aluminum nitrate and urea in diluted solution, spherical core–shell particles with a uniform particle size of about 1 μm were synthesized. Upon calcination at 1000 °C, the particles adopted a core–shell structure with a γ-alumina core and δ-alumina shell as evidenced by 2D and 3D electron microscopy and<sup>27</sup>Al magic angle spinning nuclear magnetic resonance spectroscopy. The spherical alumina particles were loaded with Pt nanoparticles with an average size below 1 nm using the strong electrostatic adsorption method. Electron microscopy and energy dispersive X-ray spectroscopy revealed a homogeneous platinum dispersion over the alumina surface. These platinum loaded alumina spheres were used as a model catalyst for bifunctional catalysis. Physical mixtures of Pt/alumina spheres and spherical zeolite particles are equivalent to catalysts with platinum deposited on the zeolite itself facilitating the investigation of the catalyst components individually. The spherical alumina particles are very convenient supports for obtaining a homogeneous distribution of highly dispersed platinum nanoparticles. Obtaining such a small Pt particle size is challenging on other support materials such as zeolites. The here reported and well-characterized Pt/alumina spheres can be combined with any zeolite and used as a bifunctional model catalyst. This is an interesting strategy for the examination of the acid catalytic function without the interference of the supported platinum metal on the investigated acid material.
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Publisher Place of Publication Editor
Language Wos 000621767000026 Publication Date 2021-01-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 3 Open Access OpenAccess
Notes Fonds Wetenschappelijk Onderzoek, G0A5417N G038116N ; Vlaamse regering, Methusalem ; Hercules Foundation, AKUL/13/19 ; Approved Most recent IF: 7.367
Call Number EMAT @ emat @c:irua:176021 Serial 6679
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Author Liu, P.; Arslan Irmak, E.; De Backer, A.; De wael, A.; Lobato, I.; Béché, A.; Van Aert, S.; Bals, S.
Title Three-dimensional atomic structure of supported Au nanoparticles at high temperature Type A1 Journal article
Year 2021 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 13 Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Au nanoparticles (NPs) deposited on CeO2 are extensively used as thermal catalysts since the morphology of the NPs is expected to be stable at elevated temperatures. Although it is well known that the activity of Au NPs depends on their size and surface structure, their three-dimensional (3D) structure at the atomic scale has not been completely characterized as a function of temperature. In this paper, we overcome the limitations of conventional electron tomography by combining atom counting applied to aberration-corrected scanning transmission electron microscopy images and molecular dynamics relaxation. In this manner, we are able to perform an atomic resolution 3D investigation of supported Au NPs. Our results enable us to characterize the 3D equilibrium structure of single NPs as a function of temperature. Moreover, the dynamic 3D structural evolution of the NPs at high temperatures, including surface layer jumping and crystalline transformations, has been studied.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000612999200029 Publication Date 2020-12-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 13 Open Access OpenAccess
Notes This work was supported by the European Research Council (Grant 815128 REALNANO to SB, Grant 770887 PICOMETRICS to SVA, Grant 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 project funding G.0267.18N.; sygma; esteem3JRA; esteem3reported Approved Most recent IF: 7.367
Call Number EMAT @ emat @c:irua:174858 Serial 6665
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Author Wu, L.; Kolmeijer, K.E.; Zhang, Y.; An, H.; Arnouts, S.; Bals, S.; Altantzis, T.; Hofmann, J.P.; Costa Figueiredo, M.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W.
Title Stabilization effects in binary colloidal Cu and Ag nanoparticle electrodes under electrochemical CO₂ reduction conditions Type A1 Journal article
Year 2021 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 13 Issue 9 Pages 4835-4844
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Nanoparticle modified electrodes constitute an attractive way to tailor-make efficient carbon dioxide (CO2) reduction catalysts. However, the restructuring and sintering processes of nanoparticles under electrochemical reaction conditions not only impedes the widespread application of nanoparticle catalysts, but also misleads the interpretation of the selectivity of the nanocatalysts. Here, we colloidally synthesized metallic copper (Cu) and silver (Ag) nanoparticles with a narrow size distribution (<10%) and utilized them in electrochemical CO2 reduction reactions. Monometallic Cu and Ag nanoparticle electrodes showed severe nanoparticle sintering already at low overpotential of -0.8 V vs. RHE, as evidenced by ex situ SEM investigations, and potential-dependent variations in product selectivity that resemble bulk Cu (14% for ethylene at -1.3 V vs. RHE) and Ag (69% for carbon monoxide at -1.0 V vs. RHE). However, by co-deposition of Cu and Ag nanoparticles, a nanoparticle stabilization effect was observed between Cu and Ag, and the sintering process was greatly suppressed at CO2 reducing potentials (-0.8 V vs. RHE). Furthermore, by varying the Cu/Ag nanoparticle ratio, the CO2 reduction reaction (CO2RR) selectivity towards methane (maximum of 20.6% for dense Cu-2.5-Ag-1 electrodes) and C-2 products (maximum of 15.7% for dense Cu-1-Ag-1 electrodes) can be tuned, which is attributed to a synergistic effect between neighbouring Ag and Cu nanoparticles. We attribute the stabilization of the nanoparticles to the positive enthalpies of Cu-Ag solid solutions, which prevents the dissolution-redeposition induced particle growth under CO2RR conditions. The observed nanoparticle stabilization effect enables the design and fabrication of active CO2 reduction nanocatalysts with high durability.
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Language Wos 000628024200011 Publication Date 2021-02-22
Series Editor Series Title Abbreviated Series Title
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ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 24 Open Access OpenAccess
Notes This work is funded by the Strategic UU-TU/e Alliance project ‘Joint Centre for Chemergy Research’ (budget holder B. M. W.). S. B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). S. A. and T. A. acknowledge funding from the University of Antwerp Research fund (BOF). We thank Eric Hellebrand (Faculty of Geosciences, Utrecht University) for the assistance in SEM measurements. Dr Ramon Oord (ARC Chemical Building Blocks Consortium, Faculty of Science, Utrecht University) is acknowledged for assisting with the grazing incidence XRD measurements; sygma Approved Most recent IF: 7.367
Call Number UA @ admin @ c:irua:176723 Serial 6737
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Author Jovanović, Z.; Gauquelin, N.; Koster, G.; Rubio-Zuazo, J.; Ghosez, P.; Verbeeck, J.; Suvorov, D.; Spreitzer, M.
Title Simultaneous heteroepitaxial growth of SrO (001) and SrO (111) during strontium-assisted deoxidation of the Si (001) surface Type A1 Journal article
Year 2020 Publication Rsc Advances Abbreviated Journal Rsc Adv
Volume 10 Issue 52 Pages 31261-31270
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Epitaxial integration of transition-metal oxides with silicon brings a variety of functional properties to the well-established platform of electronic components. In this process, deoxidation and passivation of the silicon surface are one of the most important steps, which in our study were controlled by an ultra-thin layer of SrO and monitored by using transmission electron microscopy (TEM), electron energy-loss spectroscopy (EELS), synchrotron X-ray diffraction (XRD) and reflection high energy electron diffraction (RHEED) methods. Results revealed that an insufficient amount of SrO leads to uneven deoxidation of the silicon surface<italic>i.e.</italic>formation of pits and islands, whereas the composition of the as-formed heterostructure gradually changes from strontium silicide at the interface with silicon, to strontium silicate and SrO in the topmost layer. Epitaxial ordering of SrO, occurring simultaneously with silicon deoxidation, was observed. RHEED analysis has identified that SrO is epitaxially aligned with the (001) Si substrate both with SrO (001) and SrO (111) out-of-plane directions. This observation was discussed from the point of view of SrO desorption, SrO-induced deoxidation of the Si (001) surface and other interfacial reactions as well as structural ordering of deposited SrO. Results of the study present an important milestone in understanding subsequent epitaxial integration of functional oxides with silicon using SrO.
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Language Wos 000566579400025 Publication Date 2020-08-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2046-2069 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.9 Times cited 1 Open Access OpenAccess
Notes Vlaamse regering, Hercules Fund ; Ministarstvo Prosvete, Nauke i Tehnološkog Razvoja, III 45006 ; Javna Agencija za Raziskovalno Dejavnost RS, J2-9237 P2-0091 ; Fonds Wetenschappelijk Onderzoek, G.0044.13N ; Ministerio de Ciencia, Innovación y Universidades; Universiteit Antwerpen, GOA project Solarpaint ; F.R.S.-FNRS, PDR project PROMOSPAN ; Consejo Superior de Investigaciones Cientificas; University of Liège, ARC project AIMED ; Ministry of Education, Science and Sport, M.ERA-NET project SIOX ; Approved Most recent IF: 3.9; 2020 IF: 3.108
Call Number EMAT @ emat @c:irua:172059 Serial 6416
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Author Liu, F.; Meng, J.; Xia, F.; Liu, Z.; Peng, H.; Sun, C.; Xu, L.; Van Tendeloo, G.; Mai, L.; Wu, J.
Title Origin of the extra capacity in nitrogen-doped porous carbon nanofibers for high-performance potassium ion batteries Type A1 Journal article
Year 2020 Publication Journal Of Materials Chemistry A Abbreviated Journal J Mater Chem A
Volume 8 Issue 35 Pages 18079-18086
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract While graphite has limited capacity as an anode material for potassium-ion batteries, nitrogen-doped carbon materials are more promising as extra capacity can usually be produced. However, the mechanism behind the origin of the extra capacity remains largely unclear. Here, the potassium storage mechanisms have been systematically studied in freestanding and porous N-doped carbon nanofibers with an additional similar to 100 mA h g(-1)discharge capacity at 0.1 A g(-1). The extra capacity is generated in the whole voltage window range from 0.01 to 2 V, which corresponds to both surface/interface K-ion absorptions due to the pyridinic N and pyrrolic N induced atomic vacancies and layer-by-layer intercalation due to the effects of graphitic N. As revealed by transmission electron microscopy, the N-doped samples have a clear and enhanced K-intercalation reaction. Theoretical calculations confirmed that the micropores with pyridinic N and pyrrolic N provide extra sites to form bonds with K, resulting in the extra capacity at high voltage. The chemical absorption of K-ions occurring inside the defective graphitic layer will prompt fast diffusion of K-ions and full realization of the intercalation capacity at low voltage. The approach of preparing N-doped carbon-based materials and the mechanism revealed by this work provide directions for the development of advanced materials for efficient energy storage.
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Publisher Place of Publication Editor
Language Wos 000569873400015 Publication Date 2020-08-03
Series Editor Series Title Abbreviated Series Title
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ISSN 2050-7488; 2050-7496 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 11.9 Times cited 2 Open Access OpenAccess
Notes ; F. Liu and J. S. Meng contributed equally to this work. This work was supported by the National Natural Science Foundation of China (51832004 and 51521001), the National Key Research and Development Program of China (2016YFA0202603), and the Natural Science Foundation of Hubei Province (2019CFA001). The S/TEM work was performed at the Nanostructure Research Center (NRC), which is supported by the Fundamental Research Funds for the Central Universities (WUT: 2019III012GX, 2020III002GX), the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, and the State Key Laboratory of Silicate Materials for Architectures (all of the laboratories are at Wuhan University of Technology). ; Approved Most recent IF: 11.9; 2020 IF: 8.867
Call Number UA @ admin @ c:irua:172741 Serial 6573
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