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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.
Address
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 (down) 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 Gonzalez-Rubio, G.; Kumar, V.; Llombart, P.; Diaz-Nunez, P.; Bladt, E.; Altantzis, T.; Bals, S.; Pena-Rodriguez, O.; Noya, E.G.; MacDowell, L.G.; Guerrero-Martinez, A.; Liz-Marzan, L.M.
Title Disconnecting Symmetry Breaking from Seeded Growth for the Reproducible Synthesis of High Quality Gold Nanorods Type A1 Journal article
Year 2019 Publication ACS nano Abbreviated Journal Acs Nano
Volume 13 Issue 13 Pages 4424-4435
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract One of the major difficulties hindering the widespread application of colloidal anisotropic plasmonic nanoparticles is the limited robustness and reproducibility of multistep synthetic methods. We demonstrate herein that the reproducibility and reliability of colloidal gold nanorod (AuNR) synthesis can be greatly improved by disconnecting the symmetry-breaking event from the seeded growth process. We have used a modified silver-assisted seeded growth method in the presence of the surfactant hexadecyltrimethylammonium bromide and n-decanol as a co-surfactant to prepare small AuNRs in high yield, which were then used as seeds for the growth of high quality AuNR colloids. Whereas the use of n-decanol provides a more-rigid micellar system, the growth on anisotropic seeds avoids sources of irreproducibility during the symmetry breaking step, yielding uniform AuNR colloids with narrow plasmon bands, ranging from 600 to 1270 nm, and allowing the fine-tuning of the final dimensions. This method provides a robust route for the preparation of high quality AuNR colloids with tunable morphology, size, and optical response in a reproducible and scalable manner.
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Publisher Place of Publication Editor
Language Wos 000466052900067 Publication Date 2019-04-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 100 Open Access (down) OpenAccess
Notes ; This work has been funded by the Spanish MINECO (grant nos. FIS2017-89361-C3-2-P and MAT2017-86659-R), the Madrid Regional Government (grant no. P2018/NMT-4389) and the Complutense University of Madrid (grant no. PR75/18-21616). Funding is acknowledged from the European Commission (grant no. EUSMI 731019). G.G.-R. acknowledges receipt of FPI Fellowship from the Spanish MINECO. E.B. and T.A. acknowledge postdoctoral grants from the Research Foundation Flanders (FWO). The authors are indebted to Profs. Justin Gooding, Watson Loh, Nicholas Kotov, Deqing Zhang, Mihaela Delcea, Maurizio Prato, and Krishna Ganesh, for providing milli-Q water samples. ; Approved Most recent IF: 13.942
Call Number UA @ admin @ c:irua:160417 Serial 5246
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Author O'Donnell, D.; Hassan, S.; Du, Y.; Gauquelin, N.; Krishnan, D.; Verbeeck, J.; Fan, R.; Steadman, P.; Bencok, P.; Dobrynin, A.N.
Title Etching induced formation of interfacial FeMn in IrMn/CoFe bilayers Type A1 Journal article
Year 2019 Publication Journal of physics: D: applied physics Abbreviated Journal J Phys D Appl Phys
Volume 52 Issue 16 Pages 165002
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The effect of ion etching on exchange bias in IrMn3/Co70Fe30 bilayers is investigated. In spite of the reduction of saturation magnetization caused by the embedding of Tr from the capping layer into the Co70Fe30 layer during the etching process, the exchange bias in samples with the same thickness of the Co70Fe30 layer is reducing in proportion to the etching power. X-ray magnetic circular dichroism measurements revealed the emergence of an uncompensated Mn magnetization after etching, which is antiferromagnetically coupled to the ferromagnetic layer. This suggests etching induced formation of small interfacial FeMn regions which leads to the decrease of effective exchange coupling between ferromagnetic and antiferromagnetic layers.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000458524800001 Publication Date 2019-01-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0022-3727 ISBN Additional Links UA library record; WoS full record
Impact Factor 2.588 Times cited Open Access (down) OpenAccess
Notes ; This work was supported by Seagate Technology (Ireland). Beamline I10, Diamond Light Source, is acknowledged for provided beamtime. ; Approved Most recent IF: 2.588
Call Number UA @ admin @ c:irua:157458 Serial 5247
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Author Behera, B.C.; Jana, S.; Bhat, S.G.; Gauquelin, N.; Tripathy, G.; Kumar, P.S.A.; Samal, D.
Title Evidence for exchange bias coupling at the perovskite/brownmillerite interface in spontaneously stabilized SrCoO3-\delta/SrCoO2.5 bilayers Type A1 Journal article
Year 2019 Publication Physical review B Abbreviated Journal Phys Rev B
Volume 99 Issue 2 Pages 024425
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Interface effect in complex oxide thin-film heterostructures lies at the vanguard of current research to design technologically relevant functionality and explore emergent physical phenomena. While most of the previous works focus on the perovskite/perovskite heterostructures, the study of perovskite/brownmillerite interfaces remains in its infancy. Here, we investigate spontaneously stabilized perovskite-ferromagnet (SrCoO3-delta)/brownmillerite-antiferromagnet (SrCoO2.5) bilayer with T-N > T-C and discover an unconventional interfacial magnetic exchange bias effect. From magnetometry investigations, it is rationalized that the observed effect stems from the interfacial ferromagnet/antiferromagnet coupling. The possibility for coupled ferromagnet/spin-glass interface engendering such effect is ruled out. Strikingly, a finite coercive field persists in the paramagnetic state of SrCoO3-delta,whereas the exchange bias field vanishes at T-C . We conjecture the observed effect to be due to the effective external quenched staggered field provided by the antiferromagnetic layer for the ferromagnetic spins at the interface. Our results not only unveil a paradigm to tailor the interfacial magnetic properties in oxide heterostructures without altering the cations at the interface, but also provide a purview to delve into the fundamental aspects of exchange bias in such unusual systems, paving a big step forward in thin-film magnetism.
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Publisher Place of Publication Editor
Language Wos 000456481900003 Publication Date 2019-01-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2469-9969; 2469-9950 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.836 Times cited 2 Open Access (down) OpenAccess
Notes ; We are grateful to Sachin Sarangi for his superb technical support during magnetic measurements. We thank Gopal Pradhan for fruitful discussion. We thank Zhicheng Zhong for reading the manuscript and for suggestions. We thank T. Som for extending laboratory facility. D.S. and B.C.B. acknowledge the financial support from Max-Planck Society through Max Planck Partner Group. S.G.B. acknowledges the INSPIRE Faculty Fellowship Programme (DSTO1899) for the financial support. ; Approved Most recent IF: 3.836
Call Number UA @ admin @ c:irua:157562 Serial 5248
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Author Akkerman, Q.A.; Bladt, E.; Petralanda, U.; Dang, Z.; Sartori, E.; Baranov, D.; Abdelhady, A.L.; Infante, I.; Bals, S.; Manna, L.
Title Fully inorganic Ruddlesden-Popper double CI-I and triple CI-Br-I lead halide perovskite nanocrystals Type A1 Journal article
Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 31 Issue 31 Pages 2182-2190
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl3, CsPbBr3, and CsPbI3) or an alloyed mixture of bromide with either Cl- or I- [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we present the synthesis as well as a detailed optical and structural study of two halide alloying cases that have not previously been reported for LHP NCs: Cs2PbI2Cl2 NCs and triple halide CsPb(Cl:Br:I)(3) NCs. In the case of Cs2PbI2Cl2, we observe for the first time NCs with a fully inorganic Ruddlesden-Popper phase (RPP) crystal structure. Unlike the well-explored organic-inorganic RPP, here, the RPP formation is triggered by the size difference between the halide ions. These NCs exhibit a strong excitonic absorption, albeit with a weak photoluminescence quantum yield (PLQY). In the case of the triple halide CsPb(Cl:Br:I)(3) composition, the NCs comprise a CsPbBr2Cl perovskite crystal lattice with only a small amount of incorporated iodide, which segregates at RPP planes' interfaces within the CsPb(Cl:Br:I)(3) NCs. Supported by density functional theory calculations and postsynthetic surface treatments to enhance the PLQY, we show that the combination of iodide segregation and defective RPP interfaces are most likely linked to the strong PL quenching observed in these nanostructures. In summary, this work demonstrates the limits of halide alloying in LHP NCs because a mixture that contains halide ions of very different sizes leads to the formation of defective RPP interfaces and a severe quenching of LHP NC's optical properties.
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Publisher Place of Publication Editor
Language Wos 000462950400038 Publication Date 2019-03-04
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 9.466 Times cited 58 Open Access (down) OpenAccess
Notes ; Q.A.A. and L.M. acknowledge funding from the European Union Seventh Framework Programme under grant agreement no. 614897 (ERC Consolidator Grant “TRANS-NANO”). The work of D.B. was supported by the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 794560. E.B. and S.B. acknowledge funding from the Research Foundation Flanders (G.038116N, G.03691, and funding of a postdoctoral grant to E.B.). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (grant no. 723.013.002). The computational work was carried out on the Dutch national e-infrastructure with the support of the SURF Cooperative. ; Approved Most recent IF: 9.466
Call Number UA @ admin @ c:irua:159414 Serial 5250
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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.
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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 (down) 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 Cassidy, S.J.; Pitcher, M.J.; Lim, J.J.K.; Hadermann, J.; Allen, J.P.; Watson, G.W.; Britto, S.; Chong, E.J.; Free, D.G.; Grey, C.P.; Clarke, S.J.
Title Layered CeSO and LiCeSO oxide chalcogenides obtained via topotactic oxidative and reductive transformations Type A1 Journal article
Year 2019 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 58 Issue 6 Pages 3838-3850
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The chemical accessibility of the Celv oxidation state enables redox chemistry to be performed on the naturally coinagemetal -deficient phases CeM1-xSO (M = Cu, Ag). A metastable black compound with the PbFC1 structure type (space group P4/nmm: a = 3.8396(1) angstrom, c = 6.607(4) angstrom, V = 97.40(6) angstrom(3)) and a composition approaching CeSO is obtained by deintercalation of Ag from CeAg0.8SO. High-resolution transmission electron microscopy reveals the presence of large defect-free regions in CeSO, but stacking faults are also evident which can be incorporated into a quantitative model to account for the severe peak anisotropy evident in all the highresolution X-ray and neutron diffractograms of bulk CeSO samples; these suggest that a few percent of residual Ag remains. A strawcolored compound with the filled PbFCI (i.e., ZrSiCuAs- or HfCuSi2type) structure (space group P4/nmm: a = 3.98171(1) angstrom, c = 8.70913(5) angstrom, V = 138.075(1) angstrom 3) and a composition close to LiCeSO, but with small amounts of residual Ag, is obtained by direct reductive lithiation of CeAga8S0 or by insertion of Li into CeSO using chemical or electrochemical means. Computation of the band structure of pure, stoichiometric CeSO predicts it to be a Ce' compound with the 4f-states lying approximately 1 eV above the sulfide-dominated valence band maximum. Accordingly, the effective magnetic moment per Ce ion measured in the CeSO samples is much reduced from the value found for the Ce3+-containing LiCeSO, and the residual paramagnetism corresponds to the Ce3+ ions remaining due to the presence of residual Ag, which presumably reflects the difficulty of stabilizing Ce' in the presence of sulfide (S2-). Comparison of the behavior of CeCu0.8SO with that of CeCu0.8SO reveals much slower reaction kinetics associated with the Cu,_xS layers, and this enables intermediate CeCui LixSO phases to be isolated.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000461978700036 Publication Date 2019-02-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited Open Access (down) OpenAccess
Notes ; We thank the UK EPSRC (EP/M020517/1 and EP/P018874/1), the Leverhulme Trust (RPG-2014-221), and Science Foundation Ireland (Grant 12/IA/1414) for funding and the EPSRC for additional studentship support. We acknowledge the ISIS pulsed neutron and muon source and the Diamond Light Source Ltd. (EE13284 and EE18786) and the ESRF for the award of beam time. We thank Dr. R I. Smith for assistance on the neutron beamlines, Dr. A. Baker and Dr. C. Murray for support on III, and Dr. C. Curls for support on ID31. ; Approved Most recent IF: 4.857
Call Number UA @ admin @ c:irua:159426 Serial 5253
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Author Das, S.; Rata, A.D.; Maznichenko, I., V; Agrestini, I.S.; Pippel, E.; Gauquelin, N.; Verbeeck, J.; Chen, K.; Valvidares, S.M.; Vasili, H.B.; Herrero-Martin, J.; Pellegrin, E.; Nenkov, K.; Herklotz, A.; Ernst, A.; Mertig, I.; Hu, Z.; Doerr, K.
Title Low-field switching of noncollinear spin texture at La0.7Sr0.3MnO3-SrRuO3interfaces Type A1 Journal article
Year 2019 Publication Physical review B Abbreviated Journal Phys Rev B
Volume 99 Issue 2 Pages 024416
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Interfaces of ferroic oxides can show complex magnetic textures which have strong impact on spintronics devices. This has been demonstrated recently for interfaces with insulating antiferromagnets such as BiFeO3. Here, noncollinear spin textures which can be switched in very low magnetic field are reported for conducting ferromagnetic bilayers of La0.7Sr0.3MnO3-SrRuO3 (LSMO-SRO). The magnetic order and switching are fundamentally different for bilayers coherently grown in reversed stacking sequence. The SRO top layer forms a persistent exchange spring which is antiferromagnetically coupled to LSMO and drives switching in low fields of a few milliteslas. Density functional theory reveals the crucial impact of the interface termination on the strength of Mn-Ru exchange coupling across the interface. The observation of an exchange spring agrees with ultrastrong coupling for the MnO2/SrO termination. Our results demonstrate low-field switching of noncollinear spin textures at an interface between conducting oxides, opening a pathway for manipulating and utilizing electron transport phenomena in controlled spin textures at oxide interfaces.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000455821400005 Publication Date 2019-01-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2469-9969; 2469-9950 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.836 Times cited 19 Open Access (down) OpenAccess
Notes ; The research in Halle was supported by Deutsche Forschungsgemeinschaft (DFG), SFB 762 Functional Oxide Interfaces (Projects No. A9 and No. B1). K.C. benefited from support of the DFG (Project 600575). Discussions with M. Trassin, M. Ziese, H. M. Christen, E.-J. Guo, F. Grcondciel, M. Bibes, and H. N. Lee are gratefully acknowledged. N. G. and J. V. acknowledge funding under 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. ; Approved Most recent IF: 3.836
Call Number UA @ admin @ c:irua:156717 Serial 5255
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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 (down) 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 Tan, X.; Stephens, P.W.; Hendrickx, M.; Hadermann, J.; Segre, C.U.; Croft, M.; Kang, C.-J.; Deng, Z.; Lapidus, S.H.; Kim, S.W.; Jin, C.; Kotliar, G.; Greenblatt, M.
Title Tetragonal Cs1.17In0.81Cl3 : a charge-ordered indium halide perovskite derivative Type A1 Journal article
Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 31 Issue 6 Pages 1981-1989
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Polycrystalline samples of Cs1.17In0.81Cl3 were prepared by annealing a mixture of CsCl, InCl, and InCl3, stoichiometric for the targeted CsInCl3. Synchrotron powder X-ray diffraction refinement and chemical analysis by energy dispersive X-ray indicated that Cs1.17In0.81Cl3, a tetragonal distorted perovskite derivative (I4/m), is the thermodynamically stable product. The refined unit cell parameters and space group were confirmed by electron diffraction. In the tetragonal structure, In+ and In3+ are located in four different crystallographic sites, consistent with their corresponding bond lengths. In1, In2, and In3 are octahedrally coordinated, whereas In4 is at the center of a pentagonal bipyramid of Cl because of the noncooperative octahedral tilting of In4Cl6. The charged-ordered In+ and In3+ were also confirmed by X-ray absorption and Raman spectroscopy. Cs1.17In0.81Cl3 is the first example of an inorganic halide double perovskite derivative with charged-ordered In+ and In3+. Band structure and optical conductivity calculations were carried out with both generalized gradient approximation (GGA) and modified Becke-Johnson (mBJ) approach; the GGA calculations estimated the band gap and optical band gap to be 2.27 eV and 2.4 eV, respectively. The large and indirect band gap suggests that Cs1.17In0.81Cl3 is not a good candidate for photovoltaic application.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000462950400017 Publication Date 2019-02-19
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 9.466 Times cited 6 Open Access (down) OpenAccess
Notes ; M.G. and X.T. were supported by the Center for Computational Design of Functional Strongly Correlated Materials and Theoretical Spectroscopy under DOE Grant No. DE-FOA-0001276. M.G. also acknowledges support of NSF-DMR-1507252 grant. G.K. and C.-J.K. were supported by the Air Force Office of Scientific Research. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The use of the Advanced Photon Source at the Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The works at IOPCAS were supported by NSF & MOST of China through research projects. ; Approved Most recent IF: 9.466
Call Number UA @ admin @ c:irua:159413 Serial 5262
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Author Queralto, A.; Graf, D.; Frohnhoven, R.; Fischer, T.; Vanrompay, H.; Bals, S.; Bartasyte, A.; Mathur, S.
Title LaFeO3 nanofibers for high detection of sulfur-containing gases Type A1 Journal article
Year 2019 Publication ACS Sustainable Chemistry and Engineering Abbreviated Journal Acs Sustain Chem Eng
Volume 7 Issue 7 Pages 6023-6032
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Lanthanum ferrite nanofibers were electrospun from a chemical sol and calcined at 600 degrees C to obtain singlephase LaFeO3 (LFO) perovskite. High-resolution transmission electron microscopy in conjunction with 3D tomographic analysis confirmed an interwoven network of hollow and porous (surface) LFO nanofibers. Owing to their high surface area and p-type behavior, the nanofiber meshes showed high chemoselectivity toward reducing toxic gases (SO2, H2S) that could be reproducibly detected at very low concentrations (<1 ppm), well below the threshold values for occupational safety and health. An increased sensitivity was observed in the temperature range of 150-300 degrees C with maximum sensor response at 250 degrees C. The surface reaction at the heterogeneous solid (LFO)/gas (SO2) interface that confirmed the formation of La-2(SO4)(3) was investigated by X-ray photoelectron spectroscopy. Moreover, the LFO fibers showed a high selectivity in the detection of oxidizing and reducing gases. Whereas superior detection of NH3 and H2S was measured, little response was observed for CO and NO2. Finally, the integration of nanowire meshes in commercial sensor platforms was successfully demonstrated.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000461978200047 Publication Date 2019-02-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2168-0485 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.951 Times cited 41 Open Access (down) OpenAccess
Notes ; The authors kindly acknowledge the ERA.Net RUS Plus project FONSENS funded by the German Federal Ministry of Education and Research (BMBF) under the grant no. 01DJ16017. A.Q. highly appreciates the support of the Alexander von Humboldt Foundation (grant no. AVH 1184642) and the BMBF for his postdoctoral fellowship. A.Q., D.G., R.F., T.F., and S.M. also kindly acknowledge the financial support of the University of Cologne. H.V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS). We also express our gratitude to Prof. Dr. J. Hadermann from the Electron Microscopy for Materials Science group at the University of Antwerp for her assistance. A.B. is grateful for the EUR EIPHI program (grant no. ANR-17-EURE-0002). ; Approved Most recent IF: 5.951
Call Number UA @ admin @ c:irua:158535 Serial 5263
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Author Tong, Y.; Fu, M.; Bladt, E.; Huang, H.; Richter, A.F.; Wang, K.; Mueller-Buschbaum, P.; Bals, S.; Tamarat, P.; Lounis, B.; Feldmann, J.; Polavarapu, L.
Title Chemical cutting of perovskite nanowires into single-photon emissive low-aspect-ratio CsPbX3(X = Cl, Br, I) nanorods Type A1 Journal article
Year 2018 Publication Angewandte Chemie: international edition in English Abbreviated Journal Angew Chem Int Edit
Volume 57 Issue 57 Pages 16094-16098
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Post-synthetic shape-transformation processes provide access to colloidal nanocrystal morphologies that are unattainable by direct synthetic routes. Herein, we report our finding about the ligand-induced fragmentation of CsPbBr3 perovskite nanowires (NWs) into low aspect-ratio CsPbX3 (X = Cl, Br and I) nanorods (NRs) during halide ion exchange reaction with PbX2-ligand solution. The shape transformation of NWs-to-NRs resulted in an increase of photoluminescence efficiency owing to a decrease of nonradiative decay rates. Importantly, we found that the perovskite NRs exhibit single photon emission as revealed by photon antibunching measurements, while it is not detected in parent NWs. This work not only reports on the quantum light emission of low aspect ratio perovskite NRs, but also expands our current understanding of shape-dependent optical properties of perovskite nanocrystals.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000452235600024 Publication Date 2018-10-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1433-7851; 0570-0833 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 11.994 Times cited 70 Open Access (down) OpenAccess
Notes ; This work was supported by the Bavarian State Ministry of Science, Research, and Arts through the grant “Solar Technologies go Hybrid (SolTech)”, by the China Scholarship Council (Y.T. and K.W.), by the Horizon 2020 research and innovation program under the Marie Skodowska-Curie Grant Agreement COMPASS No. 691185 and by LMU Munich's Institutional Strategy LMU excellent (L.P., J.F.). M.F., P.T. and B.L. acknowledge the financial support from the French National Agency for Research, the French Excellence Initiative (Idex Bordeaux, LAPHIA Program) and the Institut Universitaire de France. E.B. and S.B. acknowledge the financial support from the European Research Council Starting Grant # 335078-COLOURATOMS. L.P. thank the EU Infrastructure Project EUSMI (European Union's Horizon 2020, grant No 731019). ; Approved Most recent IF: 11.994
Call Number UA @ admin @ c:irua:156246 Serial 5283
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Author Albrecht, W.; Bladt, E.; Vanrompay, H.; Smith, J.D.; Skrabalak, S.E.; Bals, S.
Title Thermal Stability of Gold/Palladium Octopods Studied in Situ in 3D: Understanding Design Rules for Thermally Stable Metal Nanoparticles Type A1 Journal article
Year 2019 Publication ACS nano Abbreviated Journal Acs Nano
Volume 13 Issue 13 Pages 6522-6530
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Multifunctional metal nanoparticles (NPs) such as anisotropic multimetallic NPs are crucial for boosting nanomaterial based applications. Advanced synthetic protocols exist to make a large variety of such nanostructures. However, a major limiting factor for the usability of them in real life applications is their stability. Here, we show that Au/Pd octopods, 8-branched nanocrystals with Oh symmetry, with only a low amount of Pd exhibited a high thermal stability and maintained strong plasmon resonances up to 600 ◦C. Furthermore, we study the influence of the composition, morphology and environment on the thermal stability and define key parameters for the design of thermally stable multifunctional NPs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000473248300038 Publication Date 2019-06-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 46 Open Access (down) OpenAccess
Notes W. A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020. 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). J. D. S. and S.E.S acknowledge funding from the US National Science Foundation (award number: CHE-1602476). The authors acknowledge funding from the European Commission Grant (EUSMI E180600101 to S. B. and S. E. S.) and European Research Council (ERC Starting Grant #335078-COLOURATOMS). Realnano 815128; sygma Approved Most recent IF: 13.942
Call Number EMAT @ emat @c:irua:161356 Serial 5285
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Author Blommaerts, N.; Vanrompay, H.; Nuti, S.; Lenaerts, S.; Bals, S.; Verbruggen, S.W.
Title Unraveling Structural Information of Turkevich Synthesized Plasmonic Gold-Silver Bimetallic Nanoparticles Type A1 Journal article
Year 2019 Publication Small Abbreviated Journal Small
Volume 15 Issue 15 Pages 1902791
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract For the synthesis of gold-silver bimetallic nanoparticles, the Turkevich method has been the state-of-the-art method for several decades. It has been presumed that this procedure results in a homogeneous alloy, although this has been debatable for many years. In this work, it is shown that neither a full alloy, nor a perfect core-shell particle is formed but rather a core-shell-like particle with altering metal composition along the radial direction. In-depth wet-chemical experiments are performed in combination with advanced transmission electron microscopy, including EDX tomography, and Finite Element Method modeling to support the observations. From the electron tomography results, the core-shell structure could be clearly visualized and the spatial distribution of gold and silver atoms could be quantified. Theoretical simulations are performed to demonstrate that even though UV-Vis spectra show only one plasmon band, this still originates from core-shell type structures. The simulations also indicate that the core-shell morphology does not so much affect the location of the plasmon band, but mainly results in significant band broadening. Wet-chemistry experiments provide the evidence that the synthesis pathway starts with gold enriched alloy cores, and later on in the synthesis mainly silver is incorporated to end up with a silver enriched alloy shell.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000482637100001 Publication Date 2019-08-25
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 26 Open Access (down) OpenAccess
Notes Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 1S32617N G.0369.15N G.0381.16N ; Approved Most recent IF: 8.643
Call Number EMAT @ emat @c:irua:161636 Serial 5290
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Author Cremers, V.; Rampelberg, G.; Baert, K.; Abrahami, S.; Claes, N.; de Oliveira, T.M.; Terryn, H.; Bals, S.; Dendooven, J.; Detavernier, C.
Title Corrosion protection of Cu by atomic layer deposition Type A1 Journal article
Year 2019 Publication Journal of vacuum science and technology: A: vacuum surfaces and films Abbreviated Journal J Vac Sci Technol A
Volume 37 Issue 37 Pages 060902
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Atomic layer deposition (ALD) is a vapor phase technique that is able to deposit uniform, conformal thin films with an excellent thickness control at the atomic scale. 18 nm thick Al2O3 and TiO2 coatings were deposited conformaly and pinhole-free onto micrometer-sized Cu powder, using trimethylaluminum and tetrakis(dimethylamido)titanium(IV), respectively, as a precursor and de-ionized water as a reactant. The capability of the ALD coating to protect the Cu powder against corrosion was investigated. Therefore, the stability of the coatings was studied in solutions with different pH in the range of 0–14, and in situ raman spectroscopy was used to detect the emergence of corrosion products of Cu as an indication that the protective coating starts to fail. Both ALD coatings provide good protection at standard pH values in the range of 5–7. In general, the TiO2 coating shows a better barrier protection against corrosion than the Al2O3 coating. However, for the most extreme pH conditions, pH 0 and pH 14, the TiO2 coating starts also to degrade.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000517925800003 Publication Date 2019-09-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0734-2101 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 1.374 Times cited 7 Open Access (down) OpenAccess
Notes The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (No. GOA 01G01513). J.D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. Approved Most recent IF: 1.374
Call Number EMAT @ emat @c:irua:162640 Serial 5361
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Author Samaee, V.; Sandfeld, S.; Idrissi, H.; Groten, J.; Pardoen, T.; Schwaiger, R.; Schryvers, D.
Title Dislocation structures and the role of grain boundaries in cyclically deformed Ni micropillars Type A1 Journal article
Year 2020 Publication Materials Science And Engineering A-Structural Materials Properties Microstructure And Processing Abbreviated Journal Mat Sci Eng A-Struct
Volume 769 Issue Pages 138295
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Transmission electron microscopy and finite element-based dislocation simulations were combined to study the development of dislocation microstructures after cyclic deformation of single crystal and bicrystal Ni micropillars oriented for multi-slip. A direct correlation between large accumulation of plastic strain and the presence of dislocation cell walls in the single crystal micropillars was observed, while the presence of the grain boundary hampered the formation of wall-like structures in agreement with a smaller accumulated plastic strain. Automated crystallographic orientation and nanostrain mapping using transmission electron microscopy revealed the presence of lattice heterogeneities associated to the cell walls including long range elastic strain fields. By combining the nanostrain mapping with an inverse modelling approach, information about dislocation density, line orientation and Burgers vector direction was derived, which is not accessible otherwise in such dense dislocation structures. Simulations showed that the image forces associated with the grain boundary in this specific bicrystal configuration have only a minor influence on dislocation behavior. Thus, the reduced occurrence of “mature” cell walls in the bicrystal can be attributed to the available volume, which is too small to accommodate cell structures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000500373800018 Publication Date 2019-08-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0921-5093 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited 1 Open Access (down) OpenAccess
Notes Financial support from the Flemish (FWO) and German Research Foundation (DFG) through the European M-ERA.NET project “FaSS” (Fatigue Simulation near Surfaces) under the grant numbers GA.014.13 N,SCHW855/5-1, and SA2292/2-1 is gratefully acknowledged. V.S. acknowledges the FWO research project G012012 N “Understanding nanocrystalline mechanical behaviour from structural investigations”. H.I. is mandated by the Belgian National Fund for Scientific Research (FSR-FNRS). S.S. acknowledges financial support from the European Research Council through the ERC Grant Agreement No. 759419 (MuDiLingo – A Multiscale Dislocation Language for Data- Driven Materials Science). Approved Most recent IF: 6.4; 2020 IF: 3.094
Call Number EMAT @ emat @c:irua:163475 Serial 5371
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Author Nerl, H.C.; Pokle, A.; Jones, L.; Müller‐Caspary, K.; Bos, K.H.W.; Downing, C.; McCarthy, E.K.; Gauquelin, N.; Ramasse, Q.M.; Lobato, I.; Daly, D.; Idrobo, J.C.; Van Aert, S.; Van Tendeloo, G.; Sanvito, S.; Coleman, J.N.; Cucinotta, C.S.; Nicolosi, V.
Title Self‐Assembly of Atomically Thin Chiral Copper Heterostructures Templated by Black Phosphorus Type A1 Journal article
Year 2019 Publication Advanced functional materials Abbreviated Journal Adv Funct Mater
Volume 29 Issue 37 Pages 1903120
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000478478400001 Publication Date 2019-07-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1616-301X ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 1 Open Access (down) OpenAccess
Notes European Research Council, 2DNanoCaps TC2D CoG 3D2DPrint CoG Picometrics grant agreement No. 770887; Engineering and Physical Sciences Research Council, EP/P033555/1 EP/R029431 ; Science Foundation Ireland, HPC1600932 ; Approved Most recent IF: 12.124
Call Number EMAT @ emat @c:irua:161901 Serial 5362
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Author Skorikov, A.; Albrecht, W.; Bladt, E.; Xie, X.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S.
Title Quantitative 3D Characterization of Elemental Diffusion Dynamics in Individual Ag@Au Nanoparticles with Different Shapes Type A1 Journal article
Year 2019 Publication ACS nano Abbreviated Journal Acs Nano
Volume 13 Issue 13 Pages 13421-13429
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Anisotropic bimetallic nanoparticles are promising candidates for plasmonic and catalytic applications. Their catalytic performance and plasmonic properties are closely linked to the distribution of the two metals, which can change during applications in which the particles are exposed to heat. Due to this fact, correlating the thermal stability of complex heterogeneous nanoparticles to their microstructural properties is of high interest for the practical applications of such materials. Here, we employ quantitative electron tomography in high-angle annular dark-field scanning transmission electron microscopy (HAADFSTEM) mode to measure the 3D elemental diffusion dynamics in individual anisotropic Au−Ag nanoparticles upon heating in situ. This approach allows us to study the elemental redistribution in complex, asymmetric nanoparticles on a single particle level, which has been inaccessible to other techniques so far. In this work, we apply the proposed method to compare the alloying dynamics of Au−Ag nanoparticles with different shapes and compositions and find that the shape of the nanoparticle does not exhibit a significant effect on the alloying speed whereas the composition does. Finally, comparing the experimental results to diffusion simulations allows us to estimate the diffusion coefficients of the metals for individual nanoparticles.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000500650000115 Publication Date 2019-10-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 29 Open Access (down) OpenAccess
Notes This project has received funding from the European Commission (grant 731019, EUSMI) and European Research Council (ERC Consolidator Grants 815128, REALNANO; 770887, PICOMETRICS; 648991, 3MC; and ERC Advanced Grant 291667, HierarSACol). This project has also received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement 823717, ESTEEM3. W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 797153, SOPMEN). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). X.X. acknowledges financial support from the EU H2020-MSCAITN-2015 project 676045, MULTIMAT. The authors also acknowledge financial support by the Research Foundation Flanders (FWO grants G038116N, G026718N, and G036915N).; sygma; esteem3JRA; esteem3reported Approved Most recent IF: 13.942
Call Number EMAT @ emat @c:irua:164061 Serial 5379
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Author Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J.
Title Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition Type A1 Journal article
Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 31 Issue 31 Pages 9673-9683
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD

cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000502418000010 Publication Date 2019-11-11
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 9.466 Times cited 6 Open Access (down) OpenAccess
Notes This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. Approved Most recent IF: 9.466
Call Number EMAT @ emat @c:irua:164056 Serial 5380
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Author Kirkwood, N.; De Backer, A.; Altantzis, T.; Winckelmans, N.; Longo, A.; Antolinez, F.V.; Rabouw, F.T.; De Trizio, L.; Geuchies, J.J.; Mulder, J.T.; Renaud, N.; Bals, S.; Manna, L.; Houtepen, A.J.
Title Locating and controlling the Zn content in In(Zn)P quantum dots Type A1 Journal article
Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 32 Issue 32 Pages 557-565
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Zinc is routinely employed in the synthesis of InP quantum dots (QDs) to improve the photoluminescence efficiency and carrier mobility of the resulting In(Zn)P alloy nanostructures. The exact location of Zn in the final structures and the mechanism by which it enhances the optoelectronic properties of the QDs is debated. We use synchrotron X-ray absorbance spectroscopy to show that the majority of Zn in In(Zn)P QDs is located at their surface as Zn-carboxylates. However, a small amount of Zn is present inside the bulk of the QDs with the consequent contraction of their lattice, as confirmed by combining high resolution high-angle annular dark-field imaging scanning transmission electron microscopy (HAADF-STEM) with statistical parameter estimation theory. We further demonstrate that the Zn content and its incorporation into the QDs can be tuned by the ligation of commonly employed Zn carboxylate precursors: the use of highly reactive Zn-acetate leads to the formation of undesired Zn3P2 and the final nanostructures being characterized by broad optical features, whereas Zn-carboxylates with longer carbon chains lead to InP crystals with much lower zinc content and narrow optical features. These results can explain the differences between structural and optical properties of In(Zn)P samples reported across the literature, and provide a rational method to tune the amount of Zn in InP nanocrystals and to drive the incorporation of Zn either as surface Zn-carboxylate, as a substitutional dopant inside the InP crystal lattice, or even predominantly as Zn3P2.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000507721600056 Publication Date 2019-12-13
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 9.466 Times cited 39 Open Access (down) OpenAccess
Notes A.J.H. acknowledges support from the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand). This research is supported by the Dutch Technology Foundation TTW, which is part of The Netherlands Organization for Scientific Research (NWO), and which is partly funded by Ministry of Economic Affairs. SB acknowledges funding from the European Research Council (grant 815128 REALNANO). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and a postdoctoral grant to A.D.B. AJH, LM and JM acknowledge support from the H2020 Collaborative Project TEQ (Grant No. 766900).; sygma Approved Most recent IF: 9.466
Call Number EMAT @ emat @c:irua:165234 Serial 5438
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Author Yang, M.; Chen, H.; Orekhov, A.; Lu, Q.; Lan, X.; Li, K.; Zhang, S.; Song, M.; Kong, Y.; Schryvers, D.; Du, Y.
Title Quantified contribution of β″ and β′ precipitates to the strengthening of an aged Al–Mg–Si alloy Type A1 Journal article
Year 2020 Publication Materials Science And Engineering A-Structural Materials Properties Microstructure And Processing Abbreviated Journal Mat Sci Eng A-Struct
Volume 774 Issue Pages 138776
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract It is generally believed that β00 precipitates, rather than β0 precipitates, are the major strengthening precipitates in

aged Al–Mg–Si alloys. The reason for this difference is not well understood. To clarify this, two samples of the

same Al–Mg–Si alloy but with different aging states were prepared. The under-aged sample only contains nanoprecipitates

of the β00 type, while the peak-aged one contains nearly equal volumes of β00 and β0 precipitates. We

have, for the first time, separated the strengthening effect of the contribution from βʺ and βʹ precipitates,

respectively, by an indirect approach based on high-precision measurements of volume fractions, number densities,

sizes, proportions of the precipitates, their lattice strains, the composition and grain size of the matrix. The

β0 precipitates, which take 45.6% of the total precipitate volume in the peak-aged sample, contribute to the entire

precipitation strengthening by only 31.6%. The main reason why they are less useful compared to β00 precipitates

has been found to be associated with their smaller lattice strains relative to the matrix, which is 0.99% versus

2.10% (for β00 ).
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000514747200001 Publication Date 2019-12-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0921-5093 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited Open Access (down) OpenAccess
Notes National Natural Science Foundation of China, 51531009 51711530713 51501230 ; Central South University, 2018gczd033 ; Flemish Science Foundation, VS.026.18N ; Program for Guangdong Introducing Innovative and Entrepreneurial Teams, 2016ZT06G025 ; Guangdong Natural Science Foundation, 2017B030306014 ; Approved Most recent IF: 6.4; 2020 IF: 3.094
Call Number EMAT @ emat @c:irua:165290 Serial 5440
Permanent link to this record
 
 
Author Peeters, H.; Keulemans, M.; Nuyts, G.; Vanmeert, F.; Li, C.; Minjauw, M.; Detavernier, C.; Bals, S.; Lenaerts, S.; Verbruggen, S.W.
Title Plasmonic gold-embedded TiO2 thin films as photocatalytic self-cleaning coatings Type A1 Journal article
Year 2020 Publication Applied Catalysis B-Environmental Abbreviated Journal Appl Catal B-Environ
Volume 267 Issue 267 Pages 118654
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Sustainable Energy, Air and Water Technology (DuEL)
Abstract Transparent photocatalytic TiO2 thin films hold great potential in the development of self-cleaning glass sur-

faces, but suffer from a poor visible light response that hinders the application under actual sunlight. To alleviate this problem, the photocatalytic film can be modified with plasmonic nanoparticles that interact very effectively with visible light. Since the plasmonic effect is strongly concentrated in the near surroundings of the nano- particle surface, an approach is presented to embed the plasmonic nanostructures in the TiO2 matrix itself, rather than deposit them loosely on the surface. This way the interaction interface is maximised and the plasmonic effect can be fully exploited. In this study, pre-fabricated gold nanoparticles are made compatible with the organic medium of a TiO2 sol-gel coating suspension, resulting in a one-pot coating suspension. After spin coating, homogeneous, smooth, highly transparent and photoactive gold-embedded anatase thin films are ob- tained.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000518865300002 Publication Date 2020-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 22.1 Times cited 57 Open Access (down) OpenAccess
Notes H.P. is grateful to the Research Foundation Flanders (FWO) for an aspirant PhD scholarship. Approved Most recent IF: 22.1; 2020 IF: 9.446
Call Number EMAT @ emat @c:irua:165616 Serial 5446
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Author Choukroun, D.; Daems, N.; Kenis, T.; Van Everbroeck, T.; Hereijgers, J.; Altantzis, T.; Bals, S.; Cool, P.; Breugelmans, T.
Title Bifunctional nickel-nitrogen-doped-carbon-supported copper electrocatalyst for CO2 reduction Type A1 Journal article
Year 2020 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume 124 Issue 124 Pages 1369-1381
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Bifunctionality is a key feature of many industrial catalysts, supported metal clusters and particles in particular, and the development of such catalysts for the CO2 reduction reaction (CO2RR) to hydrocarbons and alcohols is gaining traction in light of recent advancements in the field. Carbon-supported Cu nanoparticles are suitable candidates for integration in the state-of-the-art reaction interfaces, and here, we propose, synthesize, and evaluate a bifunctional Ni–N-doped-C-supported Cu electrocatalyst, in which the support possesses active sites for selective CO2 conversion to CO and Cu nanoparticles catalyze either the direct CO2 or CO reduction to hydrocarbons. In this work, we introduce the scientific rationale behind the concept, its applicability, and the challenges with regard to the catalyst. From the practical aspect, the deposition of Cu nanoparticles onto carbon black and Ni–N–C supports via an ammonia-driven deposition precipitation method is reported and explored in more detail using X-ray diffraction, thermogravimetric analysis, and hydrogen temperature-programmed reduction. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDXS) give further evidence of the presence of Cu-containing nanoparticles on the Ni–N–C supports while revealing an additional relationship between the nanoparticle’s composition and the electrode’s electrocatalytic performance. Compared to the benchmark carbon black-supported Cu catalysts, Ni–N–C-supported Cu delivers up to a 2-fold increase in the partial C2H4 current density at −1.05 VRHE (C1/C2 = 0.67) and a concomitant 10-fold increase of the CO partial current density. The enhanced ethylene production metrics, obtained by virtue of the higher intrinsic activity of the Ni–N–C support, point out toward a synergistic action between the two catalytic functionalities.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000508467700015 Publication Date 2020-01-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447; 1932-7455 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited 24 Open Access (down) OpenAccess
Notes ; N.D. acknowledges sponsoring from the research foundation of Flanders (FWO) in the frame of a postdoctoral grant (12Y3919N N.D.). J.H. greatly acknowledges the Research Foundation Flanders (FWO) for support through a postdoctoral fellowship (28761). T.V.E. and P.C. acknowledge financial support from the EU-Partial-PGMs project (H2020NMP-686086). The authors also acknowledge financial support from the university research fund (BOF-GOA PS ID No. 33928). ; Approved Most recent IF: 3.7; 2020 IF: 4.536
Call Number UA @ admin @ c:irua:165326 Serial 6286
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Author Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E.
Title Defect-directed growth of symmetrically branched metal nanocrystals Type A1 Journal article
Year 2020 Publication Angewandte Chemie-International Edition Abbreviated Journal Angew Chem Int Edit
Volume 59 Issue 59 Pages 943-950
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near-field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single-crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000498760200001 Publication Date 2019-11-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1433-7851; 0570-0833 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 23 Open Access (down) OpenAccess
Notes ; The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi), Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Structure Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding to S.E.S. from the U.S. National Science Foundation (award numbers: 1602476 and 1904499) and Research Corporation for Scientific Advancement (2017 Frontiers in Research Excellence and Discovery Award) as well as to S.B. from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). ; sygma Approved Most recent IF: 16.6; 2020 IF: 11.994
Call Number UA @ admin @ c:irua:165124 Serial 6293
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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.
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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 (down) 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 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.
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Publisher Place of Publication Editor
Language Wos 000518690900030 Publication Date 2019-12-20
Series Editor Series Title Abbreviated Series Title
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ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 14 Open Access (down) 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 Wang, J.; Nguyen, M.D.; Gauquelin, N.; Verbeeck, J.; Do, M.T.; Koster, G.; Rijnders, G.; Houwman, E.
Title On the importance of the work function and electron carrier density of oxide electrodes for the functional properties of ferroelectric capacitors Type A1 Journal article
Year 2020 Publication Physica Status Solidi-Rapid Research Letters Abbreviated Journal Phys Status Solidi-R
Volume 14 Issue 14 Pages 1900520
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract It is important to understand the effect of the interfaces between the oxide electrode layers and the ferroelectric layer on the polarization response for optimizing the device performance of all-oxide ferroelectric devices. Herein, the effects of the oxide La0.07Ba0.93SnO3 (LBSO) as an electrode material in an PbZr0.52Ti0.48O3 (PZT) ferroelectric capacitor are compared with those of the more commonly used SrRuO3 (SRO) electrode. SRO (top)/PZT/SRO (bottom), SRO/PZT/LBSO, and SRO/PZT/2 nm SRO/LBSO devices are fabricated. Only marginal differences in crystalline properties, determined by X-ray diffraction and scanning transmission electron microscopy, are found. High-quality polarization loops are obtained, but with a much larger coercive field for the SRO/PZT/LBSO device. In contrast to the SRO/PZT/SRO device, the polarization decreases strongly with increasing field cycling. This fatigue problem can be remedied by inserting a 2 nm SRO layer between PZT and LBSO. It is argued that strongly increased charge injection into the PZT occurs at the bottom interface, because of the low PZT/LBSO interfacial barrier and the much lower carrier density in LBSO, as compared with that in SRO, causing a low dielectric constant, depleted layer in LBSO. The charge injection creates a trapped space charge in the PZT, causing the difference in fatigue behavior.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000506195600001 Publication Date 2019-12-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1862-6254 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.8 Times cited 6 Open Access (down) OpenAccess
Notes ; This work was supported by Nederlandse Organisatie voor Wetenschappelijk Onderzoek through grant no.13HTSM01. ; Approved Most recent IF: 2.8; 2020 IF: 3.032
Call Number UA @ admin @ c:irua:165681 Serial 6316
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Author Hinterding, S.O.M.; Berends, A.C.; Kurttepeli, M.; Moret, M.-E.; Meeldijk, J.D.; Bals, S.; van der Stam, W.; de Donega, C.M.
Title Tailoring Cu+ for Ga3+ cation exchange in Cu2-xS and CuInS2 nanocrystals by controlling the Ga precursor chemistry Type A1 Journal article
Year 2019 Publication ACS nano Abbreviated Journal Acs Nano
Volume 13 Issue 13 Pages 12880-12893
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Nanoscale cation exchange (CE) has resulted in colloidal nanomaterials that are unattainable by direct synthesis methods. Aliovalent CE is complex and synthetically challenging because the exchange of an unequal number of host and guest cations is required to maintain charge balance. An approach to control aliovalent CE reactions is the use of a single reactant to both supply the guest cation and extract the host cation. Here, we study the application of GaCl3-L complexes [L = trioctylphosphine (TOP), triphenylphosphite (TPP), diphenylphosphine (DPP)] as reactants in the exchange of Cu+ for Ga3+ in Cu2-xS nanocrystals. We find that noncomplexed GaCl3 etches the nanocrystals by S2- extraction, whereas GaCl3-TOP is unreactive. Successful exchange of Cu+ for Ga3+ is only possible when GaCl3 is complexed with either TPP or DPP. This is attributed to the pivotal role of the Cu2-xS-GaCl3-L activated complex that forms at the surface of the nanocrystal at the onset of the CE reaction, which must be such that simultaneous Ga3+ insertion and Cu+ extraction can occur. This requisite is only met if GaCl3 is bound to a phosphine ligand, with a moderate bond strength, to allow facile dissociation of the complex at the nanocrystal surface. The general validity of this mechanism is demonstrated by using GaCl3-DPP to convert CuInS2 into (Cu,Ga,In)S-2 nanocrystals, which increases the photoluminescence quantum yield 10 -fold, while blue -shifting the photoluminescence into the NIR biological window. This highlights the general applicability of the mechanistic insights provided by our work.
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Publisher Place of Publication Editor
Language Wos 000500650000061 Publication Date 2019-10-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 27 Open Access (down) OpenAccess
Notes ; S.O.M.H., W.v.d.S., A.C.B., and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant Nos. ECHO.712.012.0001 and ECHO.712.014.001. S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant No. 815128-REALNANO). S.O.M.H. is supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. DFT calculations were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. This work was sponsored by NWO Physical Sciences for the use of supercomputer facilities. The authors thank Jessi van der Hoeven for EDS and TEM measurements. ; sygma Approved Most recent IF: 13.942
Call Number UA @ admin @ c:irua:165149 Serial 6324
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Author Tran Phong Le, P.; Hofhuis, K.; Rana, A.; Huijben, M.; Hilgenkamp, H.; Rijnders, G.A.J.H.M.; ten Elshof, J.E.; Koster, G.; Gauquelin, N.; Lumbeeck, G.; Schuessler-Langeheine, C.; Popescu, H.; Fortuna, F.; Smit, S.; Verbeek, X.H.; Araizi-Kanoutas, G.; Mishra, S.; Vaskivskyi, I.; Duerr, H.A.; Golden, M.S.
Title Tailoring vanadium dioxide film orientation using nanosheets : a combined microscopy, diffraction, transport, and soft X-ray in transmission study Type A1 Journal article
Year 2020 Publication Advanced Functional Materials Abbreviated Journal Adv Funct Mater
Volume 30 Issue 1 Pages 1900028
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)(M1)/(110)(R) and (-402)(M1)/(002)(R) by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed.
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Publisher Place of Publication Editor
Language Wos 000505545800010 Publication Date 2019-10-31
Series Editor Series Title Abbreviated Series Title
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ISSN 1616-301x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 19 Times cited 1 Open Access (down) OpenAccess
Notes P.T.P.L. and K.H. contributed equally to this work. The authors thank Mark A. Smithers for performing high-resolution scanning electron microscopy and electron backscattering diffraction. The authors also thank Dr. Nicolas Jaouen for his contribution to the soft X-ray imaging experiments. This work is part of the DESCO research program of the Foundation for Fundamental Research on Matter (FOM), which is part of the Netherlands Organisation for Scientific Research (NWO). P.T.P.L. acknowledges the NWO/CW ECHO grant ECHO.15.CM2.043. N.G. acknowledges funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the FLAG-ERA JTC 2017 project GRAPH-EYE. G.L. acknowledges financial support from the Flemish Research Fund (FWO) under project G.0365.15N. I.V. acknowledges support by the U.S. Department of Energy, Office of Science under Award Number 0000231415. Approved Most recent IF: 19; 2020 IF: 12.124
Call Number UA @ admin @ c:irua:165705 Serial 6325
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Author Tang, Z.; Liu, P.; Cao, H.; Bals, S.; Heeres, H.J.; Pescarmona, P.P.
Title Pr/ZrO2 prepared by atomic trapping : an efficient catalyst for the conversion of glycerol to lactic acid with concomitant transfer hydrogenation of cyclohexene Type A1 Journal article
Year 2019 Publication ACS catalysis Abbreviated Journal Acs Catal
Volume 9 Issue 9 Pages 9953-9963
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A series of heterogeneous catalysts consisting of highly dispersed Pt nanoparticles supported on nanosized ZrO2 (20 to 60 nm) was synthesized and investigated for the one-pot transfer hydrogenation between glycerol and cyclohexene to produce lactic acid and cyclohexane, without any additional H-2. Different preparation methods were screened, by varying the calcination and reduction procedures with the purpose of optimizing the dispersion of Pt species (i.e., as single-atom sites or extra-fine Pt nanoparticles) on the ZrO2 support. The Pt/ZrO2 catalysts were characterized by means of transmission electron microscopy techniques (HAADF-STEM, TEM), elemental analysis (ICP-OES, EDX mapping), N-2-physisorption, H-2 temperature-programmed-reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). Based on this combination of techniques it was possible to correlate the temperature of the calcination and reduction treatments with the nature of the Pt species. The best catalyst consisted of subnanometer Pt clusters (<1 nm) and atomically dispersed Pt (as Pt2+ and Pt4+) on the ZrO2 support, which were converted into extra-fine Pt nanoparticles (average size = 1.4 nm) upon reduction. These nanoparticles acted as catalytic species for the transfer hydrogenation of glycerol with cyclohexene, which gave an unsurpassed 95% yield of lactic acid salt at 96% glycerol conversion (aqueous glycerol solution, NaOH as promoter, 160 degrees C, 4.5 h, at 20 bar N-2). This is the highest yield and selectivity of lactic acid (salt) reported in the literature so far. Reusability experiments showed a partial and gradual loss of activity of the Pt/ZrO2 catalyst, which was attributed to the experimentally observed aggregation of Pt nanoparticles.
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Publisher Place of Publication Editor
Language Wos 000494549700025 Publication Date 2019-09-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2155-5435 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 10.614 Times cited 46 Open Access (down) OpenAccess
Notes Zhenchen Tang acknowledges the financial support from the China Scholarship Council for his Ph.D. grant. All the authors are grateful for the technical support from Erwin Wilbers, Anne Appeldoorn, and Marcel de Vries, the TEM support from Dr. Marc Stuart, and the ICP-OES support from Johannes van der Velde. Pei Liu and Sara Bals acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of grant agreement No. 731019 EUSMI. Approved Most recent IF: 10.614
Call Number UA @ admin @ c:irua:164643 Serial 6326
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