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Author Friedrich, T.; Yu, C.-P.; Verbeek, J.; Pennycook, T.; Van Aert, S. pdf  url
doi  openurl
  Title Phase retrieval from 4-dimensional electron diffraction datasets Type P1 Proceeding
  Year (down) 2021 Publication Proceedings T2 – IEEE International Conference on Image Processing (ICIP), SEP 19-22, 2021, Electr. network Abbreviated Journal  
  Volume Issue Pages 3453-3457  
  Keywords P1 Proceeding; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract We present a computational imaging mode for large scale electron microscopy data, which retrieves a complex wave from noisy/sparse intensity recordings using a deep learning approach and subsequently reconstructs an image of the specimen from the Convolutional Neural Network (CNN) predicted exit waves. We demonstrate that an appropriate forward model in combination with open data frameworks can be used to generate large synthetic datasets for training. In combination with augmenting the data with Poisson noise corresponding to varying dose-values, we effectively eliminate overfitting issues. The U-NET[1] based architecture of the CNN is adapted to the task at hand and performs well while maintaining a relatively small size and fast performance. The validity of the approach is confirmed by comparing the reconstruction to well-established methods using simulated, as well as real electron microscopy data. The proposed method is shown to be effective particularly in the low dose range, evident by strong suppression of noise, good spatial resolution, and sensitivity to different atom types, enabling the simultaneous visualisation of light and heavy elements and making different atomic species distinguishable. Since the method acts on a very local scale and is comparatively fast it bears the potential to be used for near-real-time reconstruction during data acquisition.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000819455103114 Publication Date 2021-08-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 978-1-6654-4115-5 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:189462 Serial 7089  
Permanent link to this record
 

 
Author Baral, P.; Orekhov, A.; Dohmen, R.; Coulombier, M.; Raskin, J.P.; Cordier, P.; Idrissi, H.; Pardoen, T. url  doi
openurl 
  Title Rheology of amorphous olivine thin films characterized by nanoindentation Type A1 Journal article
  Year (down) 2021 Publication Acta Materialia Abbreviated Journal Acta Mater  
  Volume 219 Issue Pages 117257  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The rheological properties of amorphous olivine thin films deposited by pulsed laser deposition have been studied based on ambient temperature nanoindentation under constant strain-rate as well as re-laxation conditions. The amorphous olivine films exhibit a viscoelastic-viscoplastic behavior with a significant rate dependency. The strain-rate sensitivity m is equal to similar to 0 . 05 which is very high for silicates, indicating a complex out-of-equilibrium structure. The minimum apparent activation volume determined from nanoindentation experiments corresponds to Mg and Fe atomic metallic sites in the (Mg,Fe)(2)SiO4 crystalline lattice. The ambient temperature creep behavior of the amorphous olivine films differs very much from the one of single crystal olivine. This behavior directly connects to the recent demonstration of the activation of grain boundary sliding in polycrystalline olivine following grain boundary amorphization under high-stress. (C) 2021 The Authors. Published by Elsevier Ltd on behalf of Acta Materialia Inc.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000706867800004 Publication Date 2021-08-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 5.301 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 5.301  
  Call Number UA @ admin @ c:irua:182592 Serial 6882  
Permanent link to this record
 

 
Author Neelisetty, K.K.; Kumar C.N., S.; Kashiwar, A.; Scherer, T.; Chakravadhanula, V.S.K.; Kuebel, C. doi  openurl
  Title Novel thin film lift-off process for in situ TEM tensile characterization Type A1 Journal article
  Year (down) 2021 Publication Microscopy And Microanalysis Abbreviated Journal Microsc Microanal  
  Volume 27 Issue S1 Pages 216-217  
  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 Publication Date 2021-07-30  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1431-9276 ISBN Additional Links UA library record  
  Impact Factor 1.891 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 1.891  
  Call Number UA @ admin @ c:irua:183617 Serial 6873  
Permanent link to this record
 

 
Author Esteban, D.A.; Vanrompay, H.; Skorikov, A.; Béché, A.; Verbeeck, J.; Freitag, B.; Bals, S. pdf  url
doi  openurl
  Title Fast electron low dose tomography for beam sensitive materials Type A1 Journal article
  Year (down) 2021 Publication Microscopy And Microanalysis Abbreviated Journal Microsc Microanal  
  Volume 27 Issue S1 Pages 2116-2118  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos Publication Date 2021-07-30  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1431-9276 ISBN Additional Links UA library record  
  Impact Factor 1.891 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 1.891  
  Call Number EMAT @ emat @c:irua:183278 Serial 6813  
Permanent link to this record
 

 
Author Gonzalez-Nelson, A.; Mula, S.; Simenas, M.; Balciunas, S.; Altenhof, A.R.; Vojvodin, C.S.; Canossa, S.; Banys, J.; Schurko, R.W.; Coudert, F.-X.; van der Veen, M.A. url  doi
openurl 
  Title Emergence of coupled rotor dynamics in metal-organic frameworks via tuned steric interactions Type A1 Journal article
  Year (down) 2021 Publication Journal Of The American Chemical Society Abbreviated Journal J Am Chem Soc  
  Volume 143 Issue 31 Pages 12053-12062  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract The organic components in metal-organic frameworks (MOFs) are unique: they are embedded in a crystalline lattice, yet, as they are separated from each other by tunable free space, a large variety of dynamic behavior can emerge. These rotational dynamics of the organic linkers are especially important due to their influence over properties such as gas adsorption and kinetics of guest release. To fully exploit linker rotation, such as in the form of molecular machines, it is necessary to engineer correlated linker dynamics to achieve their cooperative functional motion. Here, we show that for MIL-53, a topology with closely spaced rotors, the phenylene functionalization allows researchers to tune the rotors' steric environment, shifting linker rotation from completely static to rapid motions at frequencies above 100 MHz. For steric interactions that start to inhibit independent rotor motion, we identify for the first time the emergence of coupled rotation modes in linker dynamics. These findings pave the way for function-specific engineering of gear-like cooperative motion in MOFs.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000684581100022 Publication Date 2021-07-29  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.858 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 13.858  
  Call Number UA @ admin @ c:irua:180504 Serial 6867  
Permanent link to this record
 

 
Author Barbiellini, B.; Kuriplach, J.; Saniz, R. url  doi
openurl 
  Title Study of rechargeable batteries using advanced spectroscopic and computational techniques Type Editorial
  Year (down) 2021 Publication Condensed Matter Abbreviated Journal  
  Volume 6 Issue 3 Pages 26  
  Keywords Editorial; Electron microscopy for materials research (EMAT)  
  Abstract Improving the efficiency and longevity of energy storage systems based on Li- and Na-ion rechargeable batteries presents a major challenge. The main problems are essentially capacity loss and limited cyclability. These effects are due to a hierarchy of factors spanning various length and time scales, interconnected in a complex manner. As a consequence, and in spite of several decades of research, a proper understanding of the ageing process has remained somewhat elusive. In recent years, however, combinations of advanced spectroscopy techniques and first-principles simulations have been applied with success to tackle this problem. In this Special Issue, we are pleased to present a selection of articles that, by precisely applying these methods, unravel key aspects of the reduction-oxidation reaction and intercalation processes. Furthermore, the approaches presented provide improvements to standard diagnostic and characterisation techniques, enabling the detection of possible Li-ion flow bottlenecks causing the degradation of capacity and cyclability.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000699368400001 Publication Date 2021-07-26  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2410-3896 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:181630 Serial 6890  
Permanent link to this record
 

 
Author Kadu, A.; van Leeuwen, T.; Batenburg, K.J. pdf  url
doi  openurl
  Title CoShaRP : a convex program for single-shot tomographic shape sensing Type A1 Journal article
  Year (down) 2021 Publication Inverse Problems Abbreviated Journal Inverse Probl  
  Volume 37 Issue 10 Pages 105005  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract We introduce single-shot x-ray tomography that aims to estimate the target image from a single cone-beam projection measurement. This linear inverse problem is extremely under-determined since the measurements are far fewer than the number of unknowns. Moreover, it is more challenging than conventional tomography, where a sufficiently large number of projection angles forms the measurements, allowing for a simple inversion process. However, single-shot tomography becomes less severe if the target image is only composed of known shapes. This paper restricts analysis to target image function that can be decomposed into known compactly supported non-negative-valued functions termed shapes. Hence, the shape prior transforms a linear ill-posed image estimation problem to a non-linear problem of estimating the roto-translations of the shapes. We circumvent the non-linearity by using a dictionary of possible roto-translations of the shapes. We propose a convex program CoShaRP, to recover the dictionary coefficients successfully. CoShaRP relies on simplex-type constraints and can be solved quickly using a primal-dual algorithm. The numerical experiments show that CoShaRP recovers shape stably from moderately noisy measurements.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000691743700001 Publication Date 2021-07-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0266-5611 ISBN Additional Links UA library record; WoS full record  
  Impact Factor 1.62 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 1.62  
  Call Number UA @ admin @ c:irua:181617 Serial 6859  
Permanent link to this record
 

 
Author Leinders, G.; Baldinozzi, G.; Ritter, C.; Saniz, R.; Arts, I.; Lamoen, D.; Verwerft, M. pdf  url
doi  openurl
  Title Charge Localization and Magnetic Correlations in the Refined Structure of U3O7 Type A1 Journal article
  Year (down) 2021 Publication Inorganic Chemistry Abbreviated Journal Inorg Chem  
  Volume 60 Issue 14 Pages 10550-10564  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Atomic arrangements in the mixed-valence oxide U3O7 are refined from high-resolution neutron scattering data. The crystallographic model describes a long-range structural order in a U60O140 primitive cell (space group P42/n) containing distorted cuboctahedral oxygen clusters. By combining experimental data and electronic structure calculations accounting for spin–orbit interactions, we provide robust evidence of an interplay between charge localization and the magnetic moments carried by the uranium atoms. The calculations predict U3O7 to be a semiconducting solid with a band gap of close to 0.32 eV, and a more pronounced charge-transfer insulator behavior as compared to the well-known Mott insulator UO2. Most uranium ions (56 out of 60) occur in 9-fold and 10-fold coordinated environments, surrounding the oxygen clusters, and have a tetravalent (24 out of 60) or pentavalent (32 out of 60) state. The remaining uranium ions (4 out of 60) are not contiguous to the oxygen cuboctahedra and have a very compact, 8-fold coordinated environment with two short (2 × 1.93(3) Å) “oxo-type” bonds. The higher Hirshfeld charge and the diamagnetic character point to a hexavalent state for these four uranium ions. Hence, the valence state distribution corresponds to 24/60 × U(IV) + 32/60 U(V) + 4/60 U(VI). The tetravalent and pentavalent uranium ions are predicted to carry noncollinear magnetic moments (with amplitudes of 1.6 and 0.8 μB, respectively), resulting in canted ferromagnetic order in characteristic layers within the overall fluorite-related structure.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000675430900049 Publication Date 2021-07-19  
  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 OpenAccess  
  Notes Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD – Spent Fuel CORrosion MODeling). This work was performed in part using HPC resources from GENCI-IDRIS (Grants 2020-101450 and 2020-101601), and in part 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. GL thanks E. Suard and C. Schreinemachers for assistance during the neutron scattering experiments at the ILL. GB acknowledges V. Petříček for suggestions on using JANA2006. Approved Most recent IF: 4.857  
  Call Number EMAT @ emat @c:irua:179907 Serial 6801  
Permanent link to this record
 

 
Author Wang, X.; Yao, X.; Schryvers, D.; Verlinden, B.; Wang, G.; Zhao, G.; Van Humbeeck, J.; Kustov, S. pdf  url
doi  openurl
  Title Anomalous stress-strain behavior of NiTi shape memory alloy close to the border of superelastic window Type A1 Journal article
  Year (down) 2021 Publication Scripta Materialia Abbreviated Journal Scripta Mater  
  Volume 204 Issue Pages 114135  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract In this work, we report an anomalous phenomenon on superelastic cycling of NiTi shape memory alloys when deforming at the temperature close to the border of superelastic window. New unexpected effects are found-(i) critical stress for inducing martensite transformation during the second loading cycle is higher than that of the first cycle; ( ii ) the plateau stress of the second cycle decreases to the original level when the strain overcomes the limit of the first cycle; ( iii ) transition from good superelasticity in the first cycle to fully irreversible strain in the second. We propose that defects generated during the first superelastic cycle close to the border of superelastic window impede following stress-induced martensitic transformations, leading to the increase of critical stress beyond yield stress of the B2 matrix, and thus functional fatigue of NiTi alloys. (c) 2021 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000690441400007 Publication Date 2021-07-14  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1359-6462 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.747 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 3.747  
  Call Number UA @ admin @ c:irua:181658 Serial 6853  
Permanent link to this record
 

 
Author Mychinko, M.; Skorikov, A.; Albrecht, W.; Sánchez‐Iglesias, A.; Zhuo, X.; Kumar, V.; Liz‐Marzán, L.M.; Bals, S. pdf  url
doi  openurl
  Title The Influence of Size, Shape, and Twin Boundaries on Heat‐Induced Alloying in Individual Au@Ag Core–Shell Nanoparticles Type A1 Journal article
  Year (down) 2021 Publication Small Abbreviated Journal Small  
  Volume Issue Pages 2102348  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Environmental conditions during real-world application of bimetallic core–shell nanoparticles (NPs) often include the use of elevated temperatures, which are known to cause elemental redistribution, in turn significantly altering the properties of these nanomaterials. Therefore, a thorough understanding of such processes is of great importance. The recently developed combination of fast electron tomography with in situ heating holders is a powerful approach to investigate heat-induced processes at the single NP level, with high spatial resolution in 3D. In combination with 3D finite-difference diffusion simulations, this method can be used to disclose the influence of various NP parameters on the diffusion dynamics in Au@Ag core–shell systems. A detailed study of the influence of heating on atomic diffusion and alloying for Au@Ag NPs with varying core morphology and crystallographic details is carried out. Whereas the core shape and aspect ratio of the NPs play a minor role, twin boundaries are found to have a strong influence on the elemental diffusion.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000673326600001 Publication Date 2021-07-14  
  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 8 Open Access OpenAccess  
  Notes The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO) and European Commission (grant 731019, EUSMI and grant 26019, ESTEEM). This work was performed under the Maria de Maeztu Units of Excellence Programme-Grant No. MDM-2017-0720, Ministry of Science and Innovation.; sygmaSB Approved Most recent IF: 8.643  
  Call Number EMAT @ emat @c:irua:179856 Serial 6804  
Permanent link to this record
 

 
Author Albrecht, W.; Arslan Irmak, E.; Altantzis, T.; Pedrazo‐Tardajos, A.; Skorikov, A.; Deng, T.‐S.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S. pdf  url
doi  openurl
  Title 3D Atomic‐Scale Dynamics of Laser‐Light‐Induced Restructuring of Nanoparticles Unraveled by Electron Tomography Type A1 Journal article
  Year (down) 2021 Publication Advanced Materials Abbreviated Journal Adv Mater  
  Volume Issue Pages 2100972  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract Understanding light–matter interactions in nanomaterials is crucial for

optoelectronic, photonic, and plasmonic applications. Specifically, metal

nanoparticles (NPs) strongly interact with light and can undergo shape

transformations, fragmentation and ablation upon (pulsed) laser excitation.

Despite being vital for technological applications, experimental insight into

the underlying atomistic processes is still lacking due to the complexity of

such measurements. Herein, atomic resolution electron tomography is performed

on the same mesoporous-silica-coated gold nanorod, before and after

femtosecond laser irradiation, to assess the missing information. Combined

with molecular dynamics (MD) simulations based on the experimentally

determined 3D atomic-scale morphology, the complex atomistic rearrangements,

causing shape deformations and defect generation, are unraveled.

These rearrangements are simultaneously driven by surface diffusion, facet

restructuring, and strain formation, and are influenced by subtleties in the

atomic distribution at the surface.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000671662000001 Publication Date 2021-07-11  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0935-9648 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 19.791 Times cited 8 Open Access OpenAccess  
  Notes W.A. and E.A.I. contributed equally to this work. The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 – REALNANO and No. 770887 – PICOMETRICS), the European Union’s Seventh Framework Programme (ERC Advanced Grant No. 291667 – HierarSACol), and the European Commission (EUSMI). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon2020 program (Grant 797153, SOPMEN). T.-S.D. acknowledges financial support from the National Science Foundation of China (NSFC, Grant No. 61905056). The authors also acknowledge financial support by the Research Foundation Flanders (FWO Grant G.0267.18N).; sygmaSB Approved Most recent IF: 19.791  
  Call Number EMAT @ emat @c:irua:179781 Serial 6805  
Permanent link to this record
 

 
Author Skorikov, A.; Heyvaert, W.; Albecht, W.; Pelt, D.M.; Bals, S. pdf  url
doi  openurl
  Title Deep learning-based denoising for improved dose efficiency in EDX tomography of nanoparticles Type A1 Journal article
  Year (down) 2021 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 13 Issue Pages 12242-12249  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The combination of energy-dispersive X-ray spectroscopy (EDX) and electron tomography is a powerful approach to retrieve the 3D elemental distribution in nanomaterials, providing an unprecedented level of information for complex, multi-component systems, such as semiconductor devices, as well as catalytic and plasmonic nanoparticles. Unfortunately, the applicability of EDX tomography is severely limited because of extremely long acquisition times and high electron irradiation doses required to obtain 3D EDX reconstructions with an adequate signal-to-noise ratio. One possibility to address this limitation is intelligent denoising of experimental data using prior expectations about the objects of interest. Herein, this approach is followed using the deep learning methodology, which currently demonstrates state-of-the-art performance for an increasing number of data processing problems. Design choices for the denoising approach and training data are discussed with a focus on nanoparticle-like objects and extremely noisy signals typical for EDX experiments. Quantitative analysis of the proposed method demonstrates its significantly enhanced performance in comparison to classical denoising approaches. This allows for improving the tradeoff between the reconstruction quality, acquisition time and radiation dose for EDX tomography. The proposed method is therefore especially beneficial for the 3D EDX investigation of electron beam-sensitive materials and studies of nanoparticle transformations.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000671395800001 Publication Date 2021-07-08  
  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 7.367 Times cited 11 Open Access OpenAccess  
  Notes Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 016.Veni.192.235 ; H2020 European Research Council, 815128 ; H2020 Marie Skłodowska-Curie Actions, 797153 ; H2020 Research Infrastructures, 731019; realnano; sygmaSB Approved Most recent IF: 7.367  
  Call Number EMAT @ emat @c:irua:179756 Serial 6799  
Permanent link to this record
 

 
Author Peng, X.; Peng, H.; Zhao, K.; Zhang, Y.; Xia, F.; Lyu, J.; Van Tendeloo, G.; Sun, C.; Wu, J. pdf  doi
openurl 
  Title Direct visualization of atomic-scale heterogeneous structure dynamics in MnO₂ nanowires Type A1 Journal article
  Year (down) 2021 Publication Acs Applied Materials & Interfaces Abbreviated Journal Acs Appl Mater Inter  
  Volume 13 Issue 28 Pages 33644-33651  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Manganese oxides are attracting great interest owing to their rich polymorphism and multiple valent states, which give rise to a wide range of applications in catalysis, capacitors, ion batteries, and so forth. Most of their functionalities are connected to transitions among the various polymorphisms and Mn valences. However, their atomic-scale dynamics is still a great challenge. Herein, we discovered a strong heterogeneity in the crystalline structure and defects, as well as in the Mn valence state. The transitions are studied by in situ transmission electron microscopy (TEM), and they involve a complex ordering of [MnO6] octahedra as the basic building tunnels. MnO2 nanowires synthesized using solution-based hydrothermal methods usually exhibit a large number of multiple polymorphism impurities with different tunnel sizes. Upon heating, MnO2 nanowires undergo a series of stoichiometric polymorphism changes, followed by oxygen release toward an oxygen-deficient spinel and rock-salt phase. The impurity polymorphism exhibits an abnormally high stability with interesting small-large-small tunnel size transition, which is attributed to a preferential stabilizer (K+) concentration, as well as a strong competition of kinetics and thermodynamics. Our results unveil the complicated intergrowth of polymorphism impurities in MnO2, which provide insights into the heterogeneous kinetics, thermodynamics, and transport properties of the tunnel-based building blocks.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000677540900101 Publication Date 2021-07-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 7.504 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 7.504  
  Call Number UA @ admin @ c:irua:180450 Serial 6861  
Permanent link to this record
 

 
Author Abakumov, A.M.; Li, C.; Boev, A.; Aksyonov, D.A.; Savina, A.A.; Abakumova, T.A.; Van Tendeloo, G.; Bals, S. pdf  doi
openurl 
  Title Grain boundaries as a diffusion-limiting factor in lithium-rich NMC cathodes for high-energy lithium-ion batteries Type A1 Journal article
  Year (down) 2021 Publication ACS applied energy materials Abbreviated Journal  
  Volume 4 Issue 7 Pages 6777-6786  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract High-energy lithium-rich layered transition metal oxides are capable of delivering record electrochemical capacity and energy density as positive electrodes for Li-ion batteries. Their electrochemical behavior is extremely complex due to sophisticated interplay between crystal structure, electronic structure, and defect structure. Here we unravel an extra level of this complexity by revealing that the most typical representative Li1.2Ni0.13Mn0.54Co0.13O2 material, prepared by a conventional coprecipitation technique with Na2CO3 as a precipitating agent, contains abundant coherent (001) grain boundaries with a Na-enriched P2-structured block due to segregation of the residual sodium traces. The trigonal prismatic oxygen coordination of Na triggers multiple nanoscale twinning, giving rise to incoherent (104) boundaries. The cationic layers at the (001) grain boundaries are filled with transition metal cations being Mn-depleted and Co-enriched; this makes them virtually not permeable for the Li+ cations, and therefore they negatively influence the Li diffusion in and out of the spherical agglomerates. These results demonstrate that besides the mechanisms intrinsic to the crystal and electronic structure of Li-rich cathodes, their rate capability might also be depreciated by peculiar microstructural aspects. Dedicated engineering of grain boundaries opens a way for improving inherently sluggish kinetics of these materials.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000678382900042 Publication Date 2021-07-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2574-0962 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 4 Open Access Not_Open_Access  
  Notes We thank Dr. M. V. Berekchiian (MSU) for assisting in ICPMS measurements. We acknowledge Russian Science Foundation (Grant 20-43-01012) and Research Foundation Flanders (FWO Vlaanderen, Project No. G0F1320N) for financial support. Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:180556 Serial 6841  
Permanent link to this record
 

 
Author Zhao, H.; Li, C.-F.; Hu, Z.-Y.; Liu, J.; Li, Y.; Hu, J.; Van Tendeloo, G.; Chen, L.-H.; Su, B.-L. pdf  doi
openurl 
  Title Size effect of bifunctional gold in hierarchical titanium oxide-gold-cadmium sulfide with slow photon effect for unprecedented visible-light hydrogen production Type A1 Journal article
  Year (down) 2021 Publication Journal Of Colloid And Interface Science Abbreviated Journal J Colloid Interf Sci  
  Volume 604 Issue Pages 131-139  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Gold nanoparticles (Au NPs) with surface plasmonic resonance (SPR) effect and excellent internal electron transfer ability have widely been combined with semiconductors for photocatalysis. However, the in-depth effects of Au NPs in multicomponent photocatalysts have not been completely understood. Herein, ternary titanium oxide-gold-cadmium sulfide (TiO2-Au-CdS, TAC) photocatalysts, based on hierarchical TiO2 inverse opal photonic crystal structure with different Au NPs sizes have been designed to reveal the SPR effect and internal electron transfer of Au NPs in the presence of slow photon effect. It appears that the SPR effect and internal electron transfer ability of Au NPs, depending on their sizes, play a synergistic effect on the photocatalytic enhancement. The ternary TAC-10 photocatalyst with – 10 nm Au NPs demonstrates an unprecedented hydrogen evolution rate of 47.6 mmolh-1g 1 under visible-light, demonstrating- 48% enhancement comparing to the sample without slow photon effect. In particular, a 9.83% apparent quantum yield under 450 nm monochromatic light is achieved for TAC-10. A model is proposed and finite-difference time-domain (FDTD) simulations reveal the size influence of Au NPs in ternary TAC photocatalysts. This work suggests that the rational design of bifunctional Au NPs coupling with slow photon effect could largely promote hydrogen production from visible-light driven water splitting. (c) 2021 Elsevier Inc. All rights reserved.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000704428600004 Publication Date 2021-07-01  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0021-9797 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.233 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 4.233  
  Call Number UA @ admin @ c:irua:182531 Serial 6886  
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Author Pramanik, G.; Kvakova, K.; Thottappali, M.A.; Rais, D.; Pfleger, J.; Greben, M.; El-Zoka, A.; Bals, S.; Dracinsky, M.; Valenta, J.; Cigler, P. url  doi
openurl 
  Title Inverse heavy-atom effect in near infrared photoluminescent gold nanoclusters Type A1 Journal article
  Year (down) 2021 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 12 Issue 23 Pages 10462-10467  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Fluorophores functionalized with heavy elements show enhanced intersystem crossing due to increased spin-orbit coupling, which in turn shortens the fluorescence decay lifetime (tau(PL)). This phenomenon is known as the heavy-atom effect (HAE). Here, we report the observation of increased tau(PL) upon functionalisation of near-infrared photoluminescent gold nanoclusters with iodine. The heavy atom-mediated increase in tau(PL) is in striking contrast with the HAE and referred to as inverse HAE. Femtosecond and nanosecond transient absorption spectroscopy revealed overcompensation of a slight decrease in lifetime of the transition associated with the Au core (ps) by a large increase in the long-lived triplet state lifetime associated with the Au shell, which contributed to the observed inverse HAE. This unique observation of inverse HAE in gold nanoclusters provides the means to enhance the triplet excited state lifetime.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000657052500001 Publication Date 2021-06-30  
  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 1 Open Access OpenAccess  
  Notes The authors acknowledge support from GACR project no. 18-12533S. G. P. acknowledges support from EUSMI project no. E180200060; J. P. from the Ministry of Education, Youth and Sports of the Czech Republic – Program INTER-EXCELLENCE (LTAUSA19066). Approved Most recent IF: 7.367  
  Call Number UA @ admin @ c:irua:179052 Serial 6843  
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Author Boschker, H.T.S.; Cook, P.L.M.; Polerecky, L.; Eachambadi, R.T.; Lozano, H.; Hidalgo-Martinez, S.; Khalenkow, D.; Spampinato, V.; Claes, N.; Kundu, P.; Wang, D.; Bals, S.; Sand, K.K.; Cavezza, F.; Hauffman, T.; Bjerg, J.T.; Skirtach, A.G.; Kochan, K.; McKee, M.; Wood, B.; Bedolla, D.; Gianoncelli, A.; Geerlings, N.M.J.; Van Gerven, N.; Remaut, H.; Geelhoed, J.S.; Millan-Solsona, R.; Fumagalli, L.; Nielsen, L.P.; Franquet, A.; Manca, J.V.; Gomila, G.; Meysman, F.J.R. url  doi
openurl 
  Title Efficient long-range conduction in cable bacteria through nickel protein wires Type A1 Journal article
  Year (down) 2021 Publication Nature Communications Abbreviated Journal Nat Commun  
  Volume 12 Issue 1 Pages 3996  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Filamentous cable bacteria display long-range electron transport, generating electrical currents over centimeter distances through a highly ordered network of fibers embedded in their cell envelope. The conductivity of these periplasmic wires is exceptionally high for a biological material, but their chemical structure and underlying electron transport mechanism remain unresolved. Here, we combine high-resolution microscopy, spectroscopy, and chemical imaging on individual cable bacterium filaments to demonstrate that the periplasmic wires consist of a conductive protein core surrounded by an insulating protein shell layer. The core proteins contain a sulfur-ligated nickel cofactor, and conductivity decreases when nickel is oxidized or selectively removed. The involvement of nickel as the active metal in biological conduction is remarkable, and suggests a hitherto unknown form of electron transport that enables efficient conduction in centimeter-long protein structures.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000669944900006 Publication Date 2021-06-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 23 Open Access OpenAccess  
  Notes The authors thank Marlies Neiemeisland for assistance with Raman microscopy, Michiel Kienhuis for assistance with NanoSIMS analysis, Peter Hildebrandt and Diego Millo for helping with the interpretation of the Raman spectra, IONTOF for the Orbitrap Hybrid- SIMS analysis, and Rene Fabregas for helping with finite-element numerical modeling for SDM. H.T.S.B. and F.J.R.M. were financially supported by the Netherlands Organization for Scientific Research (VICI grant 016.VICI.170.072). Research Foundation Flanders supported F.J.R.M., J.V.M., and R.T.E. through FWO grant G031416N, and F.J.R.M. and J.S.G. through FWO grant G038819N. N.M.J.G. is the recipient of a Ph.D. scholarship for teachers from NWO in the Netherlands (grant 023.005.049). The NanoSIMS facility at Utrecht University was financed through a large infrastructure grant by the Netherlands Organization for Scientific Research (NWO, grant no. 175.010.2009.011) and through a Research Infrastructure Fund by the Utrecht University Board. A.G.S. is supported by the Special Research Fund (BOF) of Ghent University (BOF14/IOP/003, BAS094-18, 01IO3618) and FWO (G043219). The ToF-SIMS was funded by FWO Hercules grant (ZW/13/07) to J.V.M. and A.F. H.L., R.M.S., and G.G. were funded by the European Union H2020 Framework Programme (MSCA-ITN-2016) under grant agreement n 721874.EU, the Spanish Agencia Estatal de Investigación and EU FEDER under grant agreements TEC2016-79156-P and TEC2015-72751-EXP, the Generalitat de Catalunya through 2017-SGR1079 grant and CERCA Program. G.G. was recipient of an ICREA Academia Award, and H.L. of a FPI fellowship (BES-2015-074799) from the Agencia Estatal de Investigación/Fondo Social Europeo. L.F. received funding from the European Research Council (grant agreement No. 819417) under the European Union’s Horizon 2020 research and innovation programme. Approved Most recent IF: 12.124  
  Call Number EMAT @ emat @c:irua:179813 Serial 6803  
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Author Wang, D.; van der Wee, E.B.; Zanaga, D.; Altantzis, T.; Wu, Y.; Dasgupta, T.; Dijkstra, M.; Murray, C.B.; Bals, S.; van Blaaderen, A. url  doi
openurl 
  Title Quantitative 3D real-space analysis of Laves phase supraparticles Type A1 Journal article
  Year (down) 2021 Publication Nature Communications Abbreviated Journal Nat Commun  
  Volume 12 Issue 1 Pages 3980  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract 3D real-space analysis of thick nanoparticle crystals is non-trivial. Here, the authors demonstrate the structural analysis of a bulk-like Laves phase by imaging an off-stoichiometric binary mixture of hard-sphere-like nanoparticles in spherical confinement by electron tomography, enabling defect analysis on the single-particle level. Assembling binary mixtures of nanoparticles into crystals, gives rise to collective properties depending on the crystal structure and the individual properties of both species. However, quantitative 3D real-space analysis of binary colloidal crystals with a thickness of more than 10 layers of particles has rarely been performed. Here we demonstrate that an excess of one species in the binary nanoparticle mixture suppresses the formation of icosahedral order in the self-assembly in droplets, allowing the study of bulk-like binary crystal structures with a spherical morphology also called supraparticles. As example of the approach, we show single-particle level analysis of over 50 layers of Laves phase binary crystals of hard-sphere-like nanoparticles using electron tomography. We observe a crystalline lattice composed of a random mixture of the Laves phases. The number ratio of the binary species in the crystal lattice matches that of a perfect Laves crystal. Our methodology can be applied to study the structure of a broad range of binary crystals, giving insights into the structure formation mechanisms and structure-property relations of nanomaterials.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000687320200032 Publication Date 2021-06-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 10 Open Access OpenAccess  
  Notes M. Hermes is sincerely thanked for providing interactive views of the structures in this work. The authors thank I. Lobato, S. Dussi, L. Filion, E. Boattini, S. Paliwal, B. van der Meer and X. Xie for fruitful discussions. D.W., E.B.v.d.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union’s Seventh Framework Program (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. T.D. and M.D. acknowledge financial support from the Industrial Partnership Program, “Computational Sciences for Energy Research” (Grant no. 13CSER025), of the Netherlands Organization for Scientific Research (NWO), which was co-financed by Shell Global Solutions International B.V. S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. T.A. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). C.B.M and Y.W. acknowledge support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge EM Square center at Utrecht University for the access to the microscopes.; sygmaSB Approved Most recent IF: 12.124  
  Call Number UA @ admin @ c:irua:181662 Serial 6845  
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Author Arenas-Vivo, A.; Rojas, S.; Ocaña, I.; Torres, A.; Liras, M.; Salles, F.; Arenas-Esteban, D.; Bals, S.; Ávila, D.; Horcajada, P. url  doi
openurl 
  Title Ultrafast reproducible synthesis of a Ag-nanocluster@MOF composite and its superior visible-photocatalytic activity in batch and in continuous flow Type A1 Journal article
  Year (down) 2021 Publication Journal Of Materials Chemistry A Abbreviated Journal J Mater Chem A  
  Volume 9 Issue 28 Pages 15704-15713  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The (photo)catalytic properties of metal–organic frameworks (MOFs) can be enhanced by post-synthetic inclusion of metallic species in their porosity. Due to their extraordinarily high surface area and well defined porous structure, MOFs can be used for the stabilization of metal nanoparticles with adjustable size within their porosity. Originally, we present here an optimized ultrafast photoreduction protocol for the<italic>in situ</italic>synthesis of tiny and monodisperse silver nanoclusters (AgNCs) homogeneously supported on a photoactive porous titanium carboxylate MIL-125-NH<sub>2</sub>MOF. The strong metal–framework interaction between –NH<sub>2</sub>and Ag atoms influences the AgNC growth, leading to the surfactant-free efficient catalyst AgNC@MIL-125-NH<sub>2</sub>with improved visible light absorption. The potential use of AgNC@MIL-125-NH<sub>2</sub>was further tested in challenging applications: (i) the photodegradation of the emerging organic contaminants (EOCs) methylene blue (MB-dye) and sulfamethazine (SMT-antibiotic) in water treatment, and (ii) the catalytic hydrogenation of<italic>p</italic>-nitroaniline (4-NA) to<italic>p</italic>-phenylenediamine (PPD) with industrial interest. It is noteworthy that compared with the pristine MIL-125-NH<sub>2</sub>, the composite presents an improved catalytic activity and stability, being able to photodegrade 92% of MB in 60 min and 96% of SMT in 30 min, and transform 100% of 4-NA to PPD in 30 min. Aside from these very good results, this study describes for the first time the use of a MOF in a visible light continuous flow reactor for wastewater treatment. With only 10 mg of AgNC@MIL-125-NH<sub>2</sub>, high SMT removal efficiency over 70% is maintained after >2 h under water flow conditions found in real wastewater treatment plants, signaling a future real application of MOFs in water remediation.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000671839200001 Publication Date 2021-06-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 8.867 Times cited 18 Open Access OpenAccess  
  Notes Comunidad de Madrid, CAM PEJD-2016/IND-2828 Talento Modality 2, 2017-T2/IND-5149 ; Secretaría de Estado de Investigación, Desarrollo e Innovación, Raphuel project (ENE2016-79608-C2-1-R) Retos Project MAT2017-84385-R ; Ministerio de Ciencia e Innovación, Juan de la Cierva Incorporación Fellowship (grant agreement no. IJC2019-038894-I) MOFSEIDON project (PID2019-104228RB-I00) Ramón y Cajal, Grant Agreements 2014-15039 and 2015-18677 ; Fundación BBVA, IN[17]CBBQUI_0197 ; H2020 European Research Council, ERC Consolidator Grant REALNANO 815128 Grant Agreement no. 731019 (EUSMI) ; sygmaSB; Approved Most recent IF: 8.867  
  Call Number EMAT @ emat @c:irua:179791 Serial 6802  
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Author Dey, A.; Ye, J.; De, A.; Debroye, E.; Ha, S.K.; Bladt, E.; Kshirsagar, A.S.; Wang, Z.; Yin, J.; Wang, Y.; Quan, L.N.; Yan, F.; Gao, M.; Li, X.; Shamsi, J.; Debnath, T.; Cao, M.; Scheel, M.A.; Kumar, S.; Steele, J.A.; Gerhard, M.; Chouhan, L.; Xu, K.; Wu, X.-gang; Li, Y.; Zhang, Y.; Dutta, A.; Han, C.; Vincon, I.; Rogach, A.L.; Nag, A.; Samanta, A.; Korgel, B.A.; Shih, C.-J.; Gamelin, D.R.; Son, D.H.; Zeng, H.; Zhong, H.; Sun, H.; Demir, H.V.; Scheblykin, I.G.; Mora-Sero, I.; Stolarczyk, J.K.; Zhang, J.Z.; Feldmann, J.; Hofkens, J.; Luther, J.M.; Perez-Prieto, J.; Li, L.; Manna, L.; Bodnarchuk, M., I; Kovalenko, M., V; Roeffaers, M.B.J.; Pradhan, N.; Mohammed, O.F.; Bakr, O.M.; Yang, P.; Muller-Buschbaum, P.; Kamat, P., V; Bao, Q.; Zhang, Q.; Krahne, R.; Galian, R.E.; Stranks, S.D.; Bals, S.; Biju, V.; Tisdale, W.A.; Yan, Y.; Hoye, R.L.Z.; Polavarapu, L. pdf  url
doi  openurl
  Title State of the art and prospects for Halide Perovskite Nanocrystals Type A1 Journal article
  Year (down) 2021 Publication Acs Nano Abbreviated Journal Acs Nano  
  Volume 15 Issue 7 Pages 10775-10981  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000679406500006 Publication Date 2021-06-17  
  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 538 Open Access OpenAccess  
  Notes E.D. and J.H. acknowledge financial support from the Research FoundationFlanders (FWO Grant Nos. S002019N, G.0B39.15, G.0B49.15, G.0962.13, G098319N, and ZW15_09-GOH6316), the Research Foundation Flanders postdoctoral fellowships to J.A.S. and E.D. (FWO Grant Nos. 12Y7218N and 12O3719N, respectively), Approved Most recent IF: 13.942  
  Call Number UA @ admin @ c:irua:180553 Serial 6846  
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Author Coeck, R.; Meeprasert, J.; Li, G.; Altantzis, T.; Bals, S.; Pidko, E.A.; De Vos, D.E. pdf  url
doi  openurl
  Title Gold and silver-catalyzed reductive amination of aromatic carboxylic acids to benzylic amines Type A1 Journal article
  Year (down) 2021 Publication Acs Catalysis Abbreviated Journal Acs Catal  
  Volume 11 Issue 13 Pages 7672-7684  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract The reductive amination of benzoic acid and its derivatives would be an effective addition to current synthesis methods for benzylamine. However, with current technology it is very difficult to keep the aromaticity intact when starting from benzoic acid, and salt wastes are often generated in the process. Here, we report a heterogeneous catalytic system for such a reductive amination, requiring solely H-2 and NH3 as the reactants. The Ag/TiO2 or Au/TiO2 catalysts can be used multiple times, and very little noble metal is required, only 0.025 mol % Au. The catalysts are bifunctional: the support catalyzes the dehydration of both the ammonium carboxylate to the amide and of the amide to the nitrile, while the sites at the metal-support interface promote the hydrogenation of the in situ generated nitrile. Yields of up to 92% benzylamine were obtained.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000670659900005 Publication Date 2021-06-10  
  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 16 Open Access OpenAccess  
  Notes R.C. thanks the FWO for his SB PhD fellowship. D.E.D.V. acknowledges FWO for research project funding, as well as KU Leuven for funding in the Metusalem program Casas. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO). T.A. acknowledges funding from the University of Antwerp Research fund (BOF). E.A.P. acknowledges the support from the European Research Council (ERC Consolidator grant #725686 DeliCAT). J.M. acknowledges financial support through the Royal Thai Government Scholarship. DFT calculations on SURFsara supercomputer facilities were performed with support from the Netherlands Organization for Scientific Research (NWO).; sygmaSB Approved Most recent IF: 10.614  
  Call Number UA @ admin @ c:irua:179851 Serial 6840  
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Author Golovachev, I.B.; Mychinko, M.Y.; Volkova, N.E.; Gavrilova, L.Y.; Raveau, B.; Maignan, A.; Cherepanov, V.A. pdf  url
doi  openurl
  Title Effect of cobalt content on the properties of quintuple perovskites Sm₂Ba₃Fe₅-xCoxO₁₅-δ Type A1 Journal article
  Year (down) 2021 Publication Journal Of Solid State Chemistry Abbreviated Journal J Solid State Chem  
  Volume 301 Issue Pages 122324  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Quintuple perovskites Sm2Ba3Fe5-xCoxO15-delta = 0.5, 1.0 and 1.5) have been prepared by glycerin-nitrate tech- nique in air. The phase purity was confirmed by XRD. Partial substitution of Co for Fe decreases the oxygen content and thus the mean oxidation state of 3d-metals. It also slightly decreases the thermal expansion coefficient of oxides. Positive value of the Seebeck coefficient confirmed p-type conductivity, though the thermopower decreases as the Co content increases. The temperature dependence of electrical conductivity reveals a maximum at 550-750 degrees C.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000684543700028 Publication Date 2021-06-03  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0022-4596 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.299 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 2.299  
  Call Number UA @ admin @ c:irua:181656 Serial 6864  
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Author Charalampopoulou, E.; Lambrinou, K.; Van der Donck, T.; Paladino, B.; Di Fonzo, F.; Azina, C.; Eklund, P.; Mraz, S.; Schneider, J.M.; Schryvers, D.; Delville, R. pdf  url
doi  openurl
  Title Early stages of dissolution corrosion in 316L and DIN 1.4970 austenitic stainless steels with and without anticorrosion coatings in static liquid lead-bismuth eutectic (LBE) at 500 degrees C Type A1 Journal article
  Year (down) 2021 Publication Materials Characterization Abbreviated Journal Mater Charact  
  Volume 178 Issue Pages 111234  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract This work addresses the early stages (<= 1000 h) of the dissolution corrosion behavior of 316L and DIN 1.4970 austenitic stainless steels in contact with oxygen-poor (C-O < 10(-8) mass%), static liquid lead-bismuth eutectic (LBE) at 500 degrees C for 600-1000 h. The objective of this study was to determine the relative early-stage resistance of the uncoated steels to dissolution corrosion and to assess the protectiveness of select candidate coatings (Cr2AlC, Al2O3, V2AlxCy). The simultaneous exposure of steels with intended differences in microstructure and thermomechanical state showed the effects of steel grain size, density of annealing/deformation twins, and secondary precipitates on the steel dissolution corrosion behavior. The findings of this study provide recommendations on steel manufacturing with the aim of using the steels to construct Gen-IV lead-cooled fast reactors.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000752582700001 Publication Date 2021-06-01  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1044-5803 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.714 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 2.714  
  Call Number UA @ admin @ c:irua:186509 Serial 7061  
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Author Duarte, M.; Daems, N.; Hereijgers, J.; Arenas Esteban, D.; Bals, S.; Breugelmans, T. pdf  url
doi  openurl
  Title Enhanced CO2 electroreduction with metal-nitrogen-doped carbons in a continuous flow reactor Type A1 Journal article
  Year (down) 2021 Publication Journal Of Co2 Utilization Abbreviated Journal J Co2 Util  
  Volume 50 Issue Pages 101583-12  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract As part of a mitigation and adaptation approach to increasing carbon dioxide atmospheric concentrations, we report superior performance of various metal-nitrogen-doped carbon catalysts, synthesized using an easily up-scalable method, for the electrochemical reduction to carbon monoxide and/or formate at industrially relevant current densities up to 200 mAcm−2. Altering the embedded transition metal (i.e. Sn, Co, Fe, Mn and Ni) allowed to tune the selectivity towards the desired product. Mn-N-C and Fe-N-C performance was compromised by its high CO* binding energy, while Co-N-C catalyzed preferentially the HER. Ni-N-C and Sn-N-C revealed to be promising electrocatalysts, the latter being evaluated for the first time in a flow reactor. A productivity of 589 L CO m-2 h-1 at -1.39 VRHE with Ni-N-C and 751 g HCOO- m-2 h-1 at -1.47 VRHE with Sn-N-C was achieved with no signs of degradation detected after 24 h of operation at industrially relevant current densities (100 mAcm−2). Stable operation at 200 mAcm−2 led to turnover frequencies for the production of carbon products of up to 5176 h-1. These enhanced productivities, in combination with high stability, constitute an essential step towards the scalability and ultimately towards the economical valorization of CO2 electrolyzers using metal-containing nitrogen-doped catalysts.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000670316000002 Publication Date 2021-05-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2212-9820 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.292 Times cited 14 Open Access OpenAccess  
  Notes The authors acknowledge sponsoring from the Research Foundation – Flanders (FWO) in the frame of a post-doctoral grant (12Y3919N – ND). This project was co-funded by the Interreg 2 Seas-Program 2014-2020, co-financed 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 MOT project D2M (“Dioxide to Monoxide (D2M): Innovative catalysis for CO2 to CO conversion”). We thank Lien Pacquets for analyzing the samples with SEM-EDX, Saskia Defoss´e for helping with the N2 physisorption measurements and Kitty Baert (VUB) for analyzing the samples with XPS and Raman. Approved Most recent IF: 4.292  
  Call Number UA @ admin @ c:irua:178151 Serial 6779  
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Author Feng, H.L.; Kang, C.-J.; Manuel, P.; Orlandi, F.; Su, Y.; Chen, J.; Tsujimoto, Y.; Hadermann, J.; Kotliar, G.; Yamaura, K.; McCabe, E.E.; Greenblatt, M. pdf  url
doi  openurl
  Title Antiferromagnetic order breaks inversion symmetry in a metallic double perovskite, Pb₂NiOsO₆ Type A1 Journal article
  Year (down) 2021 Publication Chemistry Of Materials Abbreviated Journal Chem Mater  
  Volume 33 Issue 11 Pages 4188-4195  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract A polycrystalline sample of Pb2NiOsO6 was synthesized under high-pressure (6 GPa) and high-temperature (1575 K) conditions. Pb2NiOsO6 crystallizes in a monoclinic double perovskite structure with a centrosymmetric space group P2(1)/n at room temperature. Pb2NiOsO6 is metallic down to 2 K and shows a single antiferromagnetic (AFM) transition at T-N = 58 K. Pb2NiOsO6 is a new example of a metallic and AFM oxide with three-dimensional connectivity. Neutron powder diffraction and first-principles calculation studies indicate that both Ni and Os moments are ordered below T-N and the AFM magnetic order breaks inversion symmetry. This loss of inversion symmetry driven by AFM order is unusual in metallic systems, and the 3d-Sd double-perovskite oxides represent a new class of noncentrosymmetric AFM metallic oxides.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000661521800032 Publication Date 2021-05-26  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 9.466  
  Call Number UA @ admin @ c:irua:179679 Serial 6854  
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Author Pramanik, G.; Kvakova, K.; Thottappali, M.A.; Rais, D.; Pfleger, J.; Greben, M.; El-Zoka, A.; Bals, S.; Dracinsky, M.; Valenta, J.; Cigler, P. url  doi
openurl 
  Title Inverse heavy-atom effect in near infrared photoluminescent gold nanoclusters Type A1 Journal Article
  Year (down) 2021 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 13 Issue 23 Pages 10462-10467  
  Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;  
  Abstract Fluorophores functionalized with heavy elements show enhanced intersystem crossing due to increased spin–orbit coupling, which in turn shortens the fluorescence decay lifetime (<italic>τ</italic><sup>PL</sup>). This phenomenon is known as the heavy-atom effect (HAE). Here, we report the observation of increased<italic>τ</italic><sup>PL</sup>upon functionalisation of near-infrared photoluminescent gold nanoclusters with iodine. The heavy atom-mediated increase in<italic>τ</italic><sup>PL</sup>is in striking contrast with the HAE and referred to as inverse HAE. Femtosecond and nanosecond transient absorption spectroscopy revealed overcompensation of a slight decrease in lifetime of the transition associated with the Au core (ps) by a large increase in the long-lived triplet state lifetime associated with the Au shell, which contributed to the observed inverse HAE. This unique observation of inverse HAE in gold nanoclusters provides the means to enhance the triplet excited state lifetime.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos Publication Date 2021-05-24  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2040-3364 ISBN Additional Links  
  Impact Factor 7.367 Times cited 7 Open Access Not_Open_Access  
  Notes The authors acknowledge support from GACR project Nr.18- 12533S. G. P. acknowledges support from EUSMI project No. E180200060; J.P. from the Ministry of Education, Youth and Sports of the Czech Republic – Program INTER-EXCELLENCE (LTAUSA19066). Approved Most recent IF: 7.367  
  Call Number EMAT @ emat @ Serial 6950  
Permanent link to this record
 

 
Author Lebedev, N.; Stehno, M.; Rana, A.; Reith, P.; Gauquelin, N.; Verbeeck, J.; Hilgenkamp, H.; Brinkman, A.; Aarts, J. url  doi
openurl 
  Title Gate-tuned anomalous Hall effect driven by Rashba splitting in intermixed LaAlO3/GdTiO3/SrTiO3 Type A1 Journal article
  Year (down) 2021 Publication Scientific Reports Abbreviated Journal Sci Rep-Uk  
  Volume 11 Issue 1 Pages 10726  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The Anomalous Hall Effect (AHE) is an important quantity in determining the properties and understanding the behaviour of the two-dimensional electron system forming at the interface of SrTiO<sub>3</sub>-based oxide heterostructures. The occurrence of AHE is often interpreted as a signature of ferromagnetism, but it is becoming more and more clear that also paramagnets may contribute to AHE. We studied the influence of magnetic ions by measuring intermixed LaAlO<sub>3</sub>/GdTiO<sub>3</sub>/SrTiO<sub>3</sub>at temperatures below 10 K. We find that, as function of gate voltage, the system undergoes a Lifshitz transition while at the same time an onset of AHE is observed. However, we do not observe clear signs of ferromagnetism. We argue the AHE to be due to the change in Rashba spin-orbit coupling at the Lifshitz transition and conclude that also paramagnetic moments which are easily polarizable at low temperatures and high magnetic fields lead to the presence of AHE, which needs to be taken into account when extracting carrier densities and mobilities.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000658820100014 Publication Date 2021-05-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.259 Times cited 5 Open Access OpenAccess  
  Notes J.V. and N.G. acknowledge funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the European Union’s horizon 2020 research and innovation programme ESTEEM3 under grant agreement 823717. The Qu-Ant-EM microscope used in this study was partly funded by the Hercules fund from the Flemish Government.; esteem3TA; esteem3reported Approved Most recent IF: 4.259  
  Call Number EMAT @ emat @c:irua:179608 Serial 6822  
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Author Safdel, A.; Zarei-Hanzaki, A.; Abedi, H.R.; Pourbabak, S.; Schryvers, D.; Basu, R. pdf  url
doi  openurl
  Title Asymmetrical superelastic behavior of thermomechanically processed semi-equiatomic NiTi alloy in tensile and compressive modes of deformation Type A1 Journal article
  Year (down) 2021 Publication Journal Of Alloys And Compounds Abbreviated Journal J Alloy Compd  
  Volume 878 Issue Pages 160443  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract In the present work two different cold working and annealing schemes were utilized, and the asymmetric superelastic response of thermomechanically processed materials were then assessed through cyclic tensile and compressive modes of deformation. The values of transformation stress, transformation strain, and pseudoelastic strain were measured for each treated and solutionized specimens and the asymmetric response was compared. In the solution annealed state, the difference of these parameters at different deformation modes was negligible due to the weak texture of the material, while for thermomechanically treated ones, development of specific deformation and recrystallization texture components was identified to be one of the underlying reasons of intensified asymmetry. The evolved substructure during the thermomechanical processing also played a substantial role in determining the asymmetric response. The presence of fine grains and dense dislocation substructure could hinder the movement of the transformation front, thus limiting the range of transformation. In tensile mode, the transformation stress was lower, but higher transformation strain was achieved, which was discussed relying on the slip activity in specified oriented grains. The lower transformation strain in compression mode led to lower pseudoelastic strain due to the narrow transformation range which finally degraded superelastic response of the material. (C) 2021 Elsevier B.V. All rights reserved.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000660477400005 Publication Date 2021-05-18  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0925-8388 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.133 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 3.133  
  Call Number UA @ admin @ c:irua:179564 Serial 6855  
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Author Ghidelli, M.; Orekhov, A.; Bassi, A.L.; Terraneo, G.; Djemia, P.; Abadias, G.; Nord, M.; Béché, A.; Gauquelin, N.; Verbeeck, J.; Raskin, J.-p.; Schryvers, D.; Pardoen, T.; Idrissi, H. url  doi
openurl 
  Title Novel class of nanostructured metallic glass films with superior and tunable mechanical properties Type A1 Journal article
  Year (down) 2021 Publication Acta Materialia Abbreviated Journal Acta Mater  
  Volume Issue Pages 116955  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract A novel class of nanostructured Zr50Cu50 (%at.) metallic glass films with superior and tunable mechanical

properties is produced by pulsed laser deposition. The process can be controlled to synthetize a wide

range of film microstructures including dense fully amorphous, amorphous embedded with nanocrystals

and amorphous nano-granular. A unique dense self-assembled nano-laminated atomic arrangement

characterized by alternating Cu-rich and Zr/O-rich nanolayers with different local chemical enrichment

and amorphous or amorphous-crystalline composite nanostructure has been discovered, while

significant in-plane clustering is reported for films synthetized at high deposition pressures. This unique

nanoarchitecture is at the basis of superior mechanical properties including large hardness and elastic

modulus up to 10 and 140 GPa, respectively and outstanding total elongation to failure (>9%), leading to

excellent strength/ductility balance, which can be tuned by playing with the film architecture. These

results pave the way to the synthesis of novel class of engineered nanostructured metallic glass films

with high structural performances attractive for a number of applications in microelectronics and

coating industry.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000670077800004 Publication Date 2021-05-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 5.301 Times cited 27 Open Access OpenAccess  
  Notes H.I. is mandated by the Belgian National Fund for Scientific Research (FSR-FNRS). This work was supported by the Fonds de la Recherche Scientifique – FNRS under Grant T.0178.19 and Grant CDR– J011320F. We acknowledge funding for the direct electron detector used in the 4D stem studies from the Hercules fund 'Direct electron detector for soft matter TEM' from the Flemish Government J.V acknowledges funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. A.O. has received partial funding from the GOA project “Solarpaint” of the University of Antwerp. A.B. and J.V. acknowledge funding through FWO project G093417N ('Compressed sensing enabling low dose imaging in transmission electron microscopy') from the Flanders Research Fund. M.G. and A.L.B acknowledge Chantelle Ekanem for support in PLD depositions. Approved Most recent IF: 5.301  
  Call Number EMAT @ emat @c:irua:178142 Serial 6761  
Permanent link to this record
 

 
Author Zhou, X.-G.; Yang, C.-Q.; Sang, X.; Li, W.; Wang, L.; Yin, Z.-W.; Han, J.-R.; Li, Y.; Ke, X.; Hu, Z.-Y.; Cheng, Y.-B.; Van Tendeloo, G. pdf  doi
openurl 
  Title Probing the electron beam-induced structural evolution of halide perovskite thin films by scanning transmission electron microscopy Type A1 Journal article
  Year (down) 2021 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C  
  Volume 125 Issue 19 Pages 10786-10794  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract A deep understanding of the fine structure at the atomic scale of halide perovskite materials has been limited by their sensitivity to the electron beam that is widely used for structural characterization. The sensitivity of a gamma-CsPbIBr2 perovskite thin film under electron beam irradiation is revealed by scanning transmission electron microscopy (STEM) through a universal large-range electron dose measurement, which is based on discrete single-electron events in the STEM mode. Our research indicates that the gamma-CsPbIBr2 thin film undergoes structural changes with increasing electron overall dose (e(-).A(-2)) rather than dose rate (e(-).A(-2).s(-1)), which suggests that overall dose is the key operative parameter. The electron beam-induced structural evolution of gamma-CsPbIBr2 is monitored by fine control of the electron beam dose, together with the analysis of high-resolution (S)TEM, diffraction, and energy-dispersive X-ray spectroscopy. Our results show that the gamma-CsPbIBr2 phase first forms an intermediate phase [e.g., CsPb(1-x)(IBr)((3-y))] with a superstructure of ordered vacancies in the pristine unit cell, while a fraction of Pb2+ is reduced to Pb-0. As the electron dose increases, Pb nanoparticles precipitate, while the remaining framework forms the Cs2IBr phase, accompanied by some amorphization. This work provides guidelines to minimize electron beam irradiation artifacts for atomic-resolution imaging on CsPbIBr2 thin films.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000655640900061 Publication Date 2021-05-11  
  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 4.536 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 4.536  
  Call Number UA @ admin @ c:irua:179187 Serial 6880  
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