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Author Zhao, H.; Li, C.-F.; Yong, X.; Kumar, P.; Palma, B.; Hu, Z.-Y.; Van Tendeloo, G.; Siahrostami, S.; Larter, S.; Zheng, D.; Wang, S.; Chen, Z.; Kibria, M.G.; Hu, J.
Title Coproduction of hydrogen and lactic acid from glucose photocatalysis on band-engineered Zn1-xCdxS homojunction Type A1 Journal article
Year 2021 Publication iScience Abbreviated Journal
Volume 24 Issue 2 Pages 102109
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Photocatalytic transformation of biomass into value-added chemicals coupled with co-production of hydrogen provides an explicit route to trap sunlight into the chemical bonds. Here, we demonstrate a rational design of Zn1-xCdxS solidsolution homojunction photocatalyst with a pseudo-periodic cubic zinc blende (ZB) and hexagonal wurtzite (WZ) structure for efficient glucose conversion to simultaneously produce hydrogen and lactic acid. The optimized Zn0.6Cd0.4S catalyst consists of a twinning superlattice, has a tuned bandgap, and displays excellent efficiency with respect to hydrogen generation (690 +/- 27.6 mu mol.h(-1).g(cat).(-1)), glucose conversion (similar to 90%), and lactic acid selectivity (similar to 87%) without any co-catalyst under visible light irradiation. The periodic WZ/ZB phase in twinning superlattice facilitates better charge separation, while superoxide radical (center dot O-2(-)) and photogenerated holes drive the glucose transformation and water oxidation reactions, respectively. This work demonstrates that rational photocatalyst design could realize an efficient and concomitant production of hydrogen and value-added chemicals from glucose photocatalysis.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000621266700080 Publication Date 2021-01-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2589-0042 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:176744 Serial 6720
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Author Li, C.-F.; Zhao, K.; Liao, X.; Hu, Z.-Y.; Zhang, L.; Zhao, Y.; Mu, S.; Li, Y.; Li, Y.; Van Tendeloo, G.; Sun, C.
Title Interface cation migration kinetics induced oxygen release heterogeneity in layered lithium cathodes Type A1 Journal article
Year 2021 Publication Energy Storage Materials Abbreviated Journal
Volume 36 Issue Pages 115-122
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The irreversible release of the lattice oxygen in layered cathodes is one of the major degradation mechanisms of lithium ion batteries, which accounts for a number of battery failures including the voltage/capacity fade, loss of cation ions and detachment of the primary particles, etc. Oxygen release is generally attributed to the stepwise thermodynamic controlled phase transitions from the layered to spinel and rock salt phases. Here, we report a strong kinetic effect from the mobility of cation ions, whose migration barrier can be significantly modulated by the phase epitaxy at the degrading interface. It ends up with a clear oxygen release heterogeneity and completely different reaction pathways between the thin and thick areas, as well as the interparticle valence boundaries, both of which widely exist in the mainstream cathode design with the secondary agglomerates. This work unveils the origin of the heterogenous oxygen release in the layered cathodes. It also sheds light on the rational design of cathode materials with enhanced oxygen stability by suppressing the cation migration.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000620584300009 Publication Date 2020-12-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access OpenAccess
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:176654 Serial 6730
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Author Abakumov, A.M.; Li, C.; Boev, A.; Aksyonov, D.A.; Savina, A.A.; Abakumova, T.A.; Van Tendeloo, G.; Bals, S.
Title Grain boundaries as a diffusion-limiting factor in lithium-rich NMC cathodes for high-energy lithium-ion batteries Type A1 Journal article
Year 2021 Publication ACS applied energy materials Abbreviated Journal
Volume 4 Issue 7 Pages 6777-6786
Keywords (up) 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 OpenAccess
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
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Author Peng, X.; Peng, H.; Zhao, K.; Zhang, Y.; Xia, F.; Lyu, J.; Van Tendeloo, G.; Sun, C.; Wu, J.
Title Direct visualization of atomic-scale heterogeneous structure dynamics in MnO₂ nanowires Type A1 Journal article
Year 2021 Publication Acs Applied Materials & Interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 13 Issue 28 Pages 33644-33651
Keywords (up) 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
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Author Liang, Q.; Yang, D.; Xia, F.; Bai, H.; Peng, H.; Yu, R.; Yan, Y.; He, D.; Cao, S.; Van Tendeloo, G.; Li, G.; Zhang, Q.; Tang, X.; Wu, J.
Title Phase-transformation-induced giant deformation in thermoelectric Ag₂Se semiconductor Type A1 Journal article
Year 2021 Publication Advanced Functional Materials Abbreviated Journal Adv Funct Mater
Volume Issue Pages 2106938
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract In most semiconducting metal chalcogenides, a large deformation is usually accompanied by a phase transformation, while the deformation mechanism remains largely unexplored. Herein, a phase-transformation-induced deformation in Ag2Se is investigated by in situ transmission electron microscopy, and a new ordered high-temperature phase (named as alpha '-Ag2Se) is identified. The Se-Se bonds are folded when the Ag+-ion vacancies are ordered and become stretched when these vacancies are disordered. Such a stretch/fold of the Se-Se bonds enables a fast and large deformation occurring during the phase transition. Meanwhile, the different Se-Se bonding states in alpha-, alpha '-, beta-Ag2Se phases lead to the formation of a large number of nanoslabs and the high concentration of dislocations at the interface, which flexibly accommodate the strain caused by the phase transformation. This study reveals the atomic mechanism of the deformation in Ag2Se inorganic semiconductors during the phase transition, which also provides inspiration for understanding the phase transition process in other functional materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000695142800001 Publication Date 2021-09-13
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 Open Access Not_Open_Access
Notes Approved Most recent IF: 12.124
Call Number UA @ admin @ c:irua:181527 Serial 6879
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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.
Title Probing the electron beam-induced structural evolution of halide perovskite thin films by scanning transmission electron microscopy Type A1 Journal article
Year 2021 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume 125 Issue 19 Pages 10786-10794
Keywords (up) 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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Author Yang, M.; Orekhov, A.; Hu, Z.-Y.; Feng, M.; Jin, S.; Sha, G.; Li, K.; Samaee, V.; Song, M.; Du, Y.; Van Tendeloo, G.; Schryvers, D.
Title Shearing and rotation of β'' and β' precipitates in an Al-Mg-Si alloy under tensile deformation : in-situ and ex-situ studies Type A1 Journal article
Year 2021 Publication Acta Materialia Abbreviated Journal Acta Mater
Volume 220 Issue Pages 117310
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The interaction between dislocations and nano-precipitates during deformation directly influences hardening response of precipitation-strengthening metals such as Al-Mg-Si alloys. However, how coherent and semi-coherent nano-precipitates accommodate external deformation applied to an Al alloy remains to be elucidated. In-situ tensile experiments in a transmission electron microscope (TEM) were conducted to study the dynamic process of dislocations cutting through coherent needle-like beta '' precipitates with diameters of 3 similar to 8 nm. Comprehensive investigations using in-situ, ex-situ TEM and atom probe tomography uncovered that beta '' precipitates were firstly sheared into small fragments, and then the rotation of the fragments, via sliding along precipitate/matrix interfaces, destroyed their initially coherent interface with the Al matrix. In contrast, semi-coherent beta' precipitates with sizes similar to beta '' were more difficult to be fragmented and accumulation of dislocations at the interface increased interface misfit between beta' and the Al matrix. Consequently, beta' precipitates could basically maintain their needle-like shape after the tensile deformation. This research gains new insights into the interaction between nano-precipitates and dislocations. (C) 2021 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000705535300005 Publication Date 2021-09-12
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 Open Access OpenAccess
Notes Approved Most recent IF: 5.301
Call Number UA @ admin @ c:irua:182528 Serial 6884
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Author Wang, L.; Li, Y.; Yang, X.-Y.; Zhang, B.-B.; Ninane, N.; Busscher, H.J.; Hu, Z.-Y.; Delneuville, C.; Jiang, N.; Xie, H.; Van Tendeloo, G.; Hasan, T.; Su, B.-L.
Title Single-cell yolk-shell nanoencapsulation for long-term viability with size-dependent permeability and molecular recognition Type A1 Journal article
Year 2021 Publication National Science Review Abbreviated Journal Natl Sci Rev
Volume 8 Issue 4 Pages
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Like nanomaterials, bacteria have been unknowingly used for centuries. They hold significant economic potential for fuel and medicinal compound production. Their full exploitation, however, is impeded by low biological activity and stability in industrial reactors. Though cellular encapsulation addresses these limitations, cell survival is usually compromised due to shell-to-cell contacts and low permeability. Here, we report ordered packing of silica nanocolloids with organized, uniform and tunable nanoporosities for single cyanobacterium nanoencapsulation using protamine as an electrostatic template. A space between the capsule shell and the cell is created by controlled internalization of protamine, resulting in a highly ordered porous shell-void-cell structure formation. These unique yolk-shell nano structures provide long-term cell viability with superior photosynthetic activities and resistance in harsh environments. In addition, engineering the colloidal packing allows tunable shell-pore diameter for size-dependent permeability and introduction of new functionalities for specific molecular recognition. Our strategy could significantly enhance the activity and stability of cyanobacteria for various nanobiotechnological applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000651827200002 Publication Date 2020-05-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2095-5138 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.843 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 8.843
Call Number UA @ admin @ c:irua:179085 Serial 6885
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Author Sun, C.; Liao, X.; Peng, H.; Zhang, C.; Van Tendeloo, G.; Zhao, Y.; Wu, J.
Title Interfacial gliding-driven lattice oxygen release in layered cathodes Type A1 Journal article
Year 2022 Publication Cell reports physical science Abbreviated Journal
Volume 3 Issue 1 Pages
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The oxygen release of layered cathodes causes many battery failures, but the underlying mechanism in an actual working cathode is still elusive as it involves secondary agglomerates that introduce complicated boundary structures. Here, we report a general structure instability on the mismatch boundaries driven by interfacial gliding-it introduces a shear stress causing a distortion of the metal-oxygen octahedra framework that reduces its kinetic stability. The migration of cations and diffusion of oxygen vacancies continue to degrade the whole particle from the boundary to the interior, followed by the formation of nano-sized cracks on the fast-degrading interfaces. This work reveals a robust chemical and mechanical interplay on the oxygen release inherent to the intergranular boundaries of layered cathodes. It also suggests that radially patterned columnar grains with low-angle planar boundaries would be an efficient approach to mitigate the boundary oxygen release.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000745659500012 Publication Date 2021-12-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access OpenAccess
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:186420 Serial 6961
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Author Ding, Y.; Maitra, S.; Arenas Esteban, D.; Bals, S.; Vrielinck, H.; Barakat, T.; Roy, S.; Van Tendeloo, G.; Liu, J.; Li, Y.; Vlad, A.; Su, B.-L.
Title Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in carbon nitride Type A1 Journal article
Year 2022 Publication Cell reports physical science Abbreviated Journal
Volume 3 Issue 5 Pages 100874-17
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (O-center dot(2)-) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 mM g(-1) h(-1) under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000805830100006 Publication Date 2022-04-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 12 Open Access OpenAccess
Notes Y.D. thanks the China Scholarship Council (201808310127) for financial support. This work is financially supported by the National Natural Science Foundation of China (U1663225) , Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) of the Chinese Ministry of Education, Program of Introducing Talents of Discipline to Universities-Plan 111 (grant no. B20002) from the Ministry of Science and Technology and the Ministry of Education of China, and the National Key R&D Program of China (2016YFA0202602) . This research was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project “DepollutAir”. Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:189706 Serial 7090
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Author Guo, A.; Bai, H.; Liang, Q.; Feng, L.; Su, X.; Van Tendeloo, G.; Wu, J.
Title Resistive switching in Ag₂Te semiconductor modulated by Ag+-ion diffusion and phase transition Type A1 Journal article
Year 2022 Publication Advanced Electronic Materials Abbreviated Journal Adv Electron Mater
Volume Issue Pages 2200850-2200858
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Memristors are considered to be the fourth circuit element and have great potential in areas like logic operations, information storage, and neuromorphic computing. The functional material in a memristor, which has a nonlinear resistance, is the key component to be developed. Herein, resistive switching is demonstrated and the structural evolutions in Ag2Te are examined under an external electric field. It is shown that the electroresistance effect is originating from an electronically triggered phase transition together with directional Ag+-ion diffusion. Using in situ transmission electron microscopy, the phase transition from the monoclinic alpha-Ag2Te into the face-centered cubic beta-Ag2Te, accompanied by a change in resistance, is directly observed. Diffusion of Ag+-ions modulates the localized density of Ag+-ion vacancies, leading to a change in electrical conductivity and influences the threshold voltage to trigger the phase transition. During the electric field-driven phase transition, the spontaneous and localized multiple polarizations from the low-symmetry alpha-Ag2Te (referring to an antiferroelectric structure) are vanishing in the cubic beta-Ag2Te (referring to a paraelectric structure). The abrupt resistance change of thin Ag2Te caused by the phase transition and modulated by the applied electric field demonstrates its great potential as functional material in volatile memory and memristors with a low-energy consumption.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000855728500001 Publication Date 2022-09-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2199-160x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.2 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 6.2
Call Number UA @ admin @ c:irua:190582 Serial 7203
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Author Zhang, Z.; Chen, X.; Shi, X.; Hu, Y.; Huang, J.; Liu, S.; Ren, Z.; Huang, H.; Han, G.; Van Tendeloo, G.; Tian, H.
Title Morphotropic phase boundary in pure perovskite lead titanate at room temperature Type A1 Journal article
Year 2022 Publication Materials Today Nano Abbreviated Journal
Volume 20 Issue Pages 100275-5
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract For many decades, great efforts have been devoted to pursue a large piezoelectric response by an intelligent design of morphotropic phase boundaries (MPB) in solid solutions, where tetragonal (T) and rhombohedral (R) structures coexist. For example, classical PbZrxTi1-xO3 and Pb(Mg1/3Nb2/3)O-3-PbTiO3 single crystals demonstrate a giant piezoelectric response near MPB. However, as the end member of these solids, perovskite-structured PbTiO3 always adopts the T phase at room temperature. Here, we report a pathway to create room temperature MPB in a single-phase PbTiO3. The uniaxial stress along the c-axis drives a T-R phase transition bridged by a monoclinic (M) phase, which facilitates a polarization rotation in the monodomain PbTiO3. Meanwhile, we demonstrate that the coexistence of T and R phases at room temperature can be achieved via an extremely mismatched heterointerface system. The uniaxial pressure is proved as an efficient way to break the inherent symmetry and able to substantially tailor the phase transition temperature Tc. These findings provide new insights into MPB, offering the opportunity to explore the giant piezoelectric response in single-phase materials. (c) 2022 Elsevier Ltd. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000906548600002 Publication Date 2022-10-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2588-8420 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 10.3 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 10.3
Call Number UA @ admin @ c:irua:193477 Serial 7324
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Author Yang, C.-Q.; Zhi, R.; Rothmann, M.U.; Xu, Y.-Y.; Li, L.-Q.; Hu, Z.-Y.; Pang, S.; Cheng, Y.-B.; Van Tendeloo, G.; Li, W.
Title Unveiling the intrinsic structure and intragrain defects of organic-inorganic hybrid perovskites by ultralow dose transmission electron microscopy Type A1 Journal article
Year 2023 Publication Advanced materials Abbreviated Journal
Volume Issue Pages 1-9
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Transmission electron microscopy (TEM) is a powerful tool for unveiling the structural, compositional, and electronic properties of organic-inorganic hybrid perovskites (OIHPs) at the atomic to micrometer length scales. However, the structural and compositional instability of OIHPs under electron beam radiation results in misunderstandings of the microscopic structure-property-performance relationship in OIHP devices. Here, ultralow dose TEM is utilized to identify the mechanism of the electron-beam-induced changes in OHIPs and clarify the cumulative electron dose thresholds (critical dose) of different commercially interesting state-of-the-art OIHPs, including methylammonium lead iodide (MAPbI(3)), formamidinium lead iodide (FAPbI(3)), FA(0.83)Cs(0.17)PbI(3), FA(0.15)Cs(0.85)PbI(3), and MAPb(0.5)Sn(0.5)I(3). The critical dose is related to the composition of the OIHPs, with FA(0.15)Cs(0.85)PbI(3) having the highest critical dose of approximate to 84 e angstrom(-2) and FA(0.83)Cs(0.17)PbI(3) having the lowest critical dose of approximate to 4.2 e angstrom(-2). The electron beam irradiation results in the formation of a superstructure with ordered I and FA vacancies along (c), as identified from the three major crystal axes in cubic FAPbI(3), (c), (c), and (c). The intragrain planar defects in FAPbI(3) are stable, while an obvious modification is observed in FA(0.83)Cs(0.17)PbI(3) under continuous electron beam exposure. This information can serve as a guide for ensuring a reliable understanding of the microstructure of OIHP optoelectronic devices by TEM.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000950461600001 Publication Date 2023-02-13
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 29.4 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 29.4; 2023 IF: 19.791
Call Number UA @ admin @ c:irua:195116 Serial 7349
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Author Wang, Y.; Yuan, Y.; Liao, X.; Van Tendeloo, G.; Zhao, Y.; Sun, C.
Title Chip-based in situ TEM investigation of structural thermal instability in aged layered cathode Type A1 Journal article
Year 2023 Publication Nanoscale Advances Abbreviated Journal
Volume 5 Issue 16 Pages 4182-4190
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Thermally induced oxygen release is an intrinsic structural instability in layered cathodes, which causes thermal runaway issues and becomes increasingly critical with the continuous improvement in energy density. Furthermore, thermal runaway events always occur in electrochemically aged cathodes, where the coupling of the thermal and electrochemical effect remains elusive. Herein, we report the anomalous segregation of cobalt metal in an aged LiCoO2 cathode, which is attributed to the local exposure of the high-energy (100) surface of LiCoO2 and weak interface Co-O dangling bonds significantly promoting the diffusion of Co. The presence of the LCO-Co interface severely aggregated the oxygen release in the form of dramatic Co growth. A unique particle-to-particle oxygen release pathway was also found, starting from the isolated high reduction areas induced by the cycling heterogeneity. This study provides atomistic insight into the robust coupling between the intrinsic structural instability and electrochemical cycling.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001030149900001 Publication Date 2023-07-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2516-0230 ISBN Additional Links UA library record; WoS full record
Impact Factor 4.7 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 4.7; 2023 IF: NA
Call Number UA @ admin @ c:irua:198281 Serial 8841
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Author Ying, J.; Xiao, Y.; Chen, J.; Hu, Z.-Y.; Tian, G.; Van Tendeloo, G.; Zhang, Y.; Symes, M.D.D.; Janiak, C.; Yang, X.-Y.
Title Fractal design of hierarchical PtPd with enhanced exposed surface atoms for highly catalytic activity and stability Type A1 Journal article
Year 2023 Publication Nano letters Abbreviated Journal
Volume 23 Issue 16 Pages 7371-7378
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Hierarchicalassembly of arc-like fractal nanostructures not onlyhas its unique self-similarity feature for stability enhancement butalso possesses the structural advantages of highly exposed surface-activesites for activity enhancement, remaining a great challenge for high-performancemetallic nanocatalyst design. Herein, we report a facile strategyto synthesize a novel arc-like hierarchical fractal structure of PtPdbimetallic nanoparticles (h-PtPd) by using pyridinium-type ionic liquidsas the structure-directing agent. Growth mechanisms of the arc-likenanostructured PtPd nanoparticles have been fully studied, and precisecontrol of the particle sizes and pore sizes has been achieved. Dueto the structural features, such as size control by self-similaritygrowth of subunits, structural stability by nanofusion of subunits,and increased numbers of exposed active atoms by the curved homoepitaxialgrowth, h-PtPd displays outstanding electrocatalytic activity towardoxygen reduction reaction and excellent stability during hydrothermaltreatment and catalytic process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001042181100001 Publication Date 2023-08-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1530-6984 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 10.8 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 10.8; 2023 IF: 12.712
Call Number UA @ admin @ c:irua:198408 Serial 8870
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Author Yu, R.; Zeng, W.; Zhou, L.; Van Tendeloo, G.; Mai, L.; Yao, Z.; Wu, J.
Title Layer-by-layer delithiation during lattice collapse as the origin of planar gliding and microcracking in Ni-rich cathodes Type A1 Journal article
Year 2023 Publication Cell reports physical science Abbreviated Journal
Volume 4 Issue 7 Pages 101480-14
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract High-energy-density nickel (Ni)-rich cathode materials are used in commercial lithium (Li)-ion batteries for electric vehicles, but they suffer from severe structural degradation upon cycling. Planar gliding and microcracking are seeds for fatal mechanical fracture, but their origin remains unclear. Herein, we show that “layer-by -layer delithiation”is activated at high voltages during the charge process when the “lattice collapse”(a characteristic high-voltage lattice evolution in Ni-rich cathodes) occurs. Layer-by-layer deli-thiation is evidenced by direct observation of the consecutive lattice collapse using in situ scanning transmission electron micro-scopy (STEM). The collapsing of the lattice initiates in the expanded planes and consecutively extends to the whole crystal. Localized strain will be induced at lattice-collapsing interface where planar gliding and intragranular microcracks are generated to release this strain. Our study reveals that layer-by-layer delithia-tion during lattice collapse is the fundamental origin of the mechanical instability in single-crystalline Ni-rich cathodes.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001048074500001 Publication Date 2023-06-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access OpenAccess
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:198299 Serial 8893
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Author Cui, W.; Lin, W.; Lu, W.; Liu, C.; Gao, Z.; Ma, H.; Zhao, W.; Van Tendeloo, G.; Zhao, W.; Zhang, Q.; Sang, X.
Title Direct observation of cation diffusion driven surface reconstruction at van der Waals gaps Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal
Volume 14 Issue 1 Pages 554-10
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Weak interlayer van der Waals (vdW) bonding has significant impact on the surface/interface structure, electronic properties, and transport properties of vdW layered materials. Unraveling the complex atomistic dynamics and structural evolution at vdW surfaces is therefore critical for the design and synthesis of the next-generation vdW layered materials. Here, we show that Ge/Bi cation diffusion along the vdW gap in layered GeBi2Te4 (GBT) can be directly observed using in situ heating scanning transmission electron microscopy (STEM). The cation concentration variation during diffusion was correlated with the local Te-6 octahedron distortion based on a quantitative analysis of the atomic column intensity and position in time-elapsed STEM images. The in-plane cation diffusion leads to out-of-plane surface etching through complex structural evolutions involving the formation and propagation of a non-centrosymmetric GeTe2 triple layer surface reconstruction on fresh vdW surfaces, and GBT subsurface reconstruction from a septuple layer to a quintuple layer. Our results provide atomistic insight into the cation diffusion and surface reconstruction in vdW layered materials. Weak interlayer van der Waals (vdW) bonding has significant impact on the structure and properties of vdW layered materials. Here authors use in-situ aberration-corrected ADF-STEM for an atomistic insight into the cation diffusion in the vdW gaps and the etching of vdW surfaces at high temperatures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001076227200001 Publication Date 2023-02-02
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 16.6 Times cited Open Access
Notes Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number UA @ admin @ c:irua:201342 Serial 9021
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Author Yang, C.-Q.; Yin, Z.-W.; Li, W.; Cui, W.-J.; Zhou, X.-G.; Wang, L.-D.; Zhi, R.; Xu, Y.-Y.; Tao, Z.-W.; Sang, X.; Cheng, Y.-B.; Van Tendeloo, G.; Hu, Z.-Y.; Su, B.-L.
Title Atomically deciphering the phase segregation in mixed halide perovskite Type A1 Journal article
Year 2024 Publication Advanced functional materials Abbreviated Journal
Volume Issue Pages 1-10
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Mixed-halide perovskites show promising applications in tandem solar cells owing to their adjustable bandgap. One major obstacle to their commercialization is halide phase segregation, which results in large open-circuit voltage deficiency and J-V hysteresis. However, the ambiguous interplay between structural origin and phase segregation often results in aimless and unspecific optimization strategies for the device's performance and stability. An atomic scale is directly figured out the abundant Ruddlesden-Popper anti-phase boundaries (RP-APBs) within a CsPbIBr2 polycrystalline film and revealed that phase segregation predominantly occurs at RP-APB-enriched interfaces due to the defect-mediated lattice strain. By compensating their structural lead halide, such RP-APBs are eliminated, and the decreasing of strain can be observed, resulting in the suppression of halide phase segregation. The present work provides the deciphering to precisely regulate the perovskite atomic structure for achieving photo-stable mixed halide wide-bandgap perovskites of high-efficiency tandem solar cell commercial applications. The phase segregation in mixed halide perovskite film predominantly occurs at Ruddlesden-Popper anti-phase boundaries (RP-APBs)-enriched interfaces due to the defect-mediated lattice strain. The RP-APBs defects can be eliminated by compensating for their structural lead halide deficiency, resulting in the suppression of halide phase segregation. image
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001200673300001 Publication Date 2024-04-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1616-301x ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:205509 Serial 9134
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Author Wang, G.; Xie, C.; Wang, H.; Li, Q.; Xia, F.; Zeng, W.; Peng, H.; Van Tendeloo, G.; Tan, G.; Tian, J.; Wu, J.
Title Mitigated oxygen loss in lithium-rich manganese-based cathode enabled by strong Zr-O affinity Type A1 Journal article
Year 2024 Publication Advanced functional materials Abbreviated Journal
Volume Issue Pages 2313672
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Oxygen loss is a serious problem of lithium-rich layered oxide (LLO) cathodes, as the high capacity of LLO relies on reversible oxygen redox. Oxygen release can occur at the surface leading to the formation of spinel or rock salt structures. Also, the lattice oxygen will usually become unstable after long cycling, which remains a major roadblock in the application of LLO. Here, it is shown that Zr doping is an effective strategy to retain lattice oxygen in LLO due to the high affinity between Zr and O. A simple sol-gel method is used to dope Zr4+ into the LLOs to adjust the local electronic structure and inhibit the diffusion of oxygen anions to the surface during cycling. Compared with untreated LLOs, LLO-Zr cathodes exhibit a higher cycling stability, with 94% capacity retention after 100 cycles at 0.4 C, up to 223 mAh g-1 at 1 C, and 88% capacity retention after 300 cycles. Theoretical calculations show that due to the strong Zr-O covalent bonding, the formation energy of oxygen vacancies has effectively increased and the loss of lattice oxygen under high voltage can be suppressed. This study provides a simple method for developing high-capacity and cyclability Li-rich cathode materials for lithium-ion batteries. Oxygen release can occur at the cathode surface leading to the formation of spinel or rock salt structures. Here, it is shown that Zr doping is an effective strategy to retain lattice oxygen in lithium-rich layered oxides (LLO) due to the high affinity between Zr and O. LLO-Zr exhibit higher cycling stability, with 88% capacity retention after 300 cycles at 1 C. image
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001159843800001 Publication Date 2024-02-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1616-301x ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:203812 Serial 9161
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Author Bals, S.; Van Aert, S.; Romero, C.P.; Lauwaet, K.; Van Bael, M.J.; Schoeters, B.; Partoens, B.; Yuecelen, E.; Lievens, P.; Van Tendeloo, G.
Title Atomic scale dynamics of ultrasmall germanium clusters Type A1 Journal article
Year 2012 Publication Nature communications Abbreviated Journal Nat Commun
Volume 3 Issue 897 Pages 897
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Starting from the gas phase, small clusters can be produced and deposited with huge flexibility with regard to composition, materials choice and cluster size. Despite many advances in experimental characterization, a detailed morphology of such clusters is still lacking. Here we present an atomic scale observation as well as the dynamical behaviour of ultrasmall germanium clusters. Using quantitative scanning transmission electron microscopy in combination with ab initio calculations, we are able to characterize the transition between different equilibrium geometries of a germanium cluster consisting of less than 25 atoms. Seven-membered rings, trigonal prisms and some smaller subunits are identified as possible building blocks that stabilize the structure.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000306099900024 Publication Date 2012-06-12
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 90 Open Access
Notes Fwo; Iap; Iwt Approved Most recent IF: 12.124; 2012 IF: 10.015
Call Number UA @ lucian @ c:irua:100340 Serial 183
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Author Galván-Moya, J.E.; Altantzis, T.; Nelissen, K.; Peeters, F.M.; Grzelczak, M.; Liz-Marán, L.M.; Bals, S.; Van Tendeloo, G.
Title Self-organization of highly symmetric nanoassemblies : a matter of competition Type A1 Journal article
Year 2014 Publication ACS nano Abbreviated Journal Acs Nano
Volume 8 Issue 4 Pages 3869-3875
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract The properties and applications of metallic nanoparticles are inseparably connected not only to their detailed morphology and composition but also to their structural configuration and mutual interactions. As a result, the assemblies often have superior properties as compared to individual nanoparticles. Although it has been reported that nanoparticles can form highly symmetric clusters, if the configuration can be predicted as a function of the synthesis parameters, more targeted and accurate synthesis will be possible. We present here a theoretical model that accurately predicts the structure and configuration of self-assembled gold nanoclusters. The validity of the model is verified using quantitative experimental data extracted from electron tomography 3D reconstructions of different assemblies. The present theoretical model is generic and can in principle be used for different types of nanoparticles, providing a very wide window of potential applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000334990600084 Publication Date 2014-03-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 34 Open Access OpenAccess
Notes FWO; Methusalem; 246791 COUNTATOMS; 335078 COLOURATOM; 262348 ESMI; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2014 IF: 12.881
Call Number UA @ lucian @ c:irua:116955 Serial 2977
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Author Willhammar, T.; Sentosun, K.; Mourdikoudis, S.; Goris, B.; Kurttepeli, M.; Bercx, M.; Lamoen, D.; Partoens, B.; Pastoriza-Santos, I.; Pérez-Juste, J.; Liz-Marzán, L.M.; Bals, S.; Van Tendeloo, G.
Title Structure and vacancy distribution in copper telluride nanoparticles influence plasmonic activity in the near-infrared Type A1 Journal article
Year 2017 Publication Nature communications Abbreviated Journal Nat Commun
Volume 8 Issue 8 Pages 14925
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Copper chalcogenides find applications in different domains including photonics, photothermal therapy and photovoltaics. CuTe nanocrystals have been proposed as an alternative to noble metal particles for plasmonics. Although it is known that deviations from stoichiometry are a prerequisite for plasmonic activity in the near-infrared, an accurate description of the material and its (optical) properties is hindered by an insufficient understanding of the atomic structure and the influence of defects, especially for materials in their nanocrystalline form. We demonstrate that the structure of Cu1.5±xTe nanocrystals canbe determined using electron diffraction tomography. Real-space high-resolution electron tomography directly reveals the three-dimensional distribution of vacancies in the structure. Through first-principles density functional theory, we furthermore demonstrate that the influence of these vacancies on the optical properties of the nanocrystals is determined. Since our methodology is applicable to a variety of crystalline nanostructured materials, it is expected to provide unique insights concerning structure–property correlations.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000397799700001 Publication Date 2017-03-30
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 37 Open Access OpenAccess
Notes The work was financially supported by the European Research Council through an ERC Starting Grant (#335078-COLOURATOMS). T.W. acknowledges the Swedish Research Council for an international postdoc grant. We acknowledge financial support of FWO-Vlaanderen through project G.0216.14N, G.0369.15N and a postdoctoral research grant to B.G. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government–Department EWI. The work was further supported by the Spanish MINECO (MAT2013-45168-R). S.M. thanks the Action ooSupporting Postdoctoral Researchers44 of the Operational Program ‘Education and Lifelong Learning’ (Action’s Beneficiary: General Secretariat for Research and Technology of Greece), which was co-financed by the European Social Fund (ESF) and the Greek State. (ROMEO:green; preprint:; postprint:can ; pdfversion:can); ECAS_Sara Approved Most recent IF: 12.124
Call Number EMAT @ emat @ c:irua:142203UA @ admin @ c:irua:142203 Serial 4538
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Author Lebedev, O.I.; Turner, S.; Liu, S.; Cool, P.; Van Tendeloo, G.
Title New nano-architectures of mesoporous silica spheres analyzed by advanced electron microscopy Type A1 Journal article
Year 2012 Publication Nanoscale Abbreviated Journal Nanoscale
Volume 4 Issue 5 Pages 1722-1727
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract Using template-containing silica microspheres as a precursor, novel ordered mesoporous silica nanoparticles with a narrow pore size distribution and high crystallinity have been synthesized by various hydrothermal merging processes. Several architectures like chains, dumbbells, triangles, squares and flowers have been discovered. The linking mechanisms of these interacting silica spheres leading to the formation of ordered nano-structures are studied by HRTEM, HAADF-STEM and electron tomography and a plausible model is presented for several merging processes.
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000300433700051 Publication Date 2011-12-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364;2040-3372; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.367 Times cited 5 Open Access
Notes Fwo Approved Most recent IF: 7.367; 2012 IF: 6.233
Call Number UA @ lucian @ c:irua:95038 Serial 2328
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Author Ribbens, S.; Beyers, E.; Schellens, K.; Mertens, M.; Ke, X.; Bals, S.; Van Tendeloo, G.; Meynen, V.; Cool, P.
Title Systematic evaluation of thermal and mechanical stability of different commercial and synthetic photocatalysts in relation to their photocatalytic activity Type A1 Journal article
Year 2012 Publication Microporous and mesoporous materials: zeolites, clays, carbons and related materials Abbreviated Journal Micropor Mesopor Mat
Volume 156 Issue Pages 62-72
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract The effect of thermal treatment and mechanical stress on the structural and photocatalytic properties of eight different (synthetic and commercial) photocatalysts has been thoroughly investigated. Different mesoporous Ti-based materials were prepared via surfactant based synthesis routes (e.g. Pluronic 123, CTMABr = Cetyltrimethylammonium bromide) or via template-free synthesis routes (e.g. trititanate nanotubes). Also, the stabilizing effect of the NaOH/NH4OH post-treatment on the templated mesoporous materials and their photocatalytic activity was investigated. Furthermore, the thermal and mechanical properties of commercially available titanium dioxides such as P25 Evonik® and Millenium PC500® were studied. The various photocatalysts were analyzed with N2-sorption, X-ray diffraction (XRD), high resolution transmission electron microscopy (HR-TEM), differential scanning calorimetry (DSC) and thermal gravimetric analysis (TGA) to obtain information concerning the specific surface area, pore volume, crystal structure, morphology, phase transitions, etc. In general, results show that the NaOH post-treatment leads to an increased control of the crystallization process during calcination resulting in a higher thermal stability, but at the same time diminishes the photocatalytic activity. Mesoporous materials in which pre-synthesized nanoparticles are used as titania source have the best mechanical stability whereas the mechanical stability of the nanotubes is the most limited. At increased temperatures and pressures, the tested commercial titanium dioxides lose their superior photocatalytic activity caused by a decreased accessibility of the active sites. The observed changes in adsorption capacities and photocatalytic activities cannot be assigned to one single phenomenon. In this respect, it shows the need to define a general/standard method to compare different photocatalysts. Furthermore, it is shown that the photocatalytic properties do not necessarily deteriorate under thermal stress, but can be improved due to crystallization, even though the initial material is (partially) destroyed. It is shown that the usefulness of a specific type of photocatalyst strongly depends on the application and the temperature/pressure to which it needs to resist.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000303625200010 Publication Date 2012-02-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1387-1811; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.615 Times cited 8 Open Access
Notes Fwo Approved Most recent IF: 3.615; 2012 IF: 3.365
Call Number UA @ lucian @ c:irua:96910 Serial 3466
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Author Verbruggen, S.W.; Keulemans, M.; Filippousi, M.; Flahaut, D.; Van Tendeloo, G.; Lacombe, S.; Martens, J.A.; Lenaerts, S.
Title Plasmonic goldsilver alloy on TiO2 photocatalysts with tunable visible light activity Type A1 Journal article
Year 2014 Publication Applied catalysis : B : environmental Abbreviated Journal Appl Catal B-Environ
Volume 156 Issue Pages 116-121
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract Adaptation of the photoresponse of anatase TiO2 to match the solar spectrum is an important scientific challenge. Modification of TiO2 with noble metal nanoparticles displaying surface plasmon resonance effects is one of the promising approaches. Surface plasmon resonance typically depends on chemical composition, size, shape and spatial organization of the metal nanoparticles in contact with TiO2. AuxAg(1 − x) alloy nanoparticles display strong composition-dependent surface plasmon resonance in the visible light region of the spectrum. In this work, a general strategy is presented to prepare plasmonic TiO2-based photocatalysts with a visible light response that can be accurately tuned over a broad range of the spectrum. The application as self-cleaning material toward the degradation of stearic acid is demonstrated for a plasmonic TiO2 photocatalyst displaying visible light photoactivity at the intensity maximum of solar light around 490 nm.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000336013200014 Publication Date 2014-03-22
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 9.446 Times cited 84 Open Access
Notes Flanders(FWO); Methusalem Approved Most recent IF: 9.446; 2014 IF: 7.435
Call Number UA @ lucian @ c:irua:115552 Serial 2646
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Author Kurttepeli, M.; Deng, S.; Verbruggen, S.W.; Guzzinati, G.; Cott, D.J.; Lenaerts, S.; Verbeeck, J.; Van Tendeloo, G.; Detavernier, C.; Bals, S.
Title Synthesis and characterization of photoreactive TiO2carbon nanosheet composites Type A1 Journal article
Year 2014 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
Volume 118 Issue 36 Pages 21031-21037
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract We report the atomic layer deposition of titanium dioxide on carbon nanosheet templates and investigate the effects of postdeposition annealing in a helium environment using different characterization techniques. The crystallization of the titanium dioxide coating upon annealing is observed using in situ X-ray diffraction. The (micro)structural characterization of the films is carried out by scanning electron microscopy and advanced transmission electron microscopy techniques. Our study shows that the annealing of the atomic layer deposition processed and carbon nanosheets templated titanium dioxide layers in helium environment resulting in the formation of a porous, nanocrystalline and photocatalytically active titanium dioxide-carbon nanosheet composite film. Such composites are suitable for photocatalysis and dye-sensitized solar cells applications.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000341619500034 Publication Date 2014-08-23
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 9 Open Access OpenAccess
Notes This research was funded by the Flemish research foundation FWO-Vlaanderen, by the European Research Council (Starting Grant No. 239865) and by the Special Research Fund BOF of Ghent University (GOA-01G01513). G.G, M.K., J.V., S.B., and G.V.T. acknowledge funding from the European Research Council under the seventh Framework Program (FP7), ERC Starting Grant No. 278510 VORTEX and No. 335078 COLOURATOMS. ECASJO;; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 4.536; 2014 IF: 4.772
Call Number UA @ lucian @ c:irua:119085 Serial 3416
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Author Van Eynde, E.; Hu, Z.-Y.; Tytgat, T.; Verbruggen, S.W.; Watte, J.; Van Tendeloo, G.; Van Driessche, I.; Blust, R.; Lenaerts, S.
Title Diatom silica-titania photocatalysts for air purification by bio-accumulation of different titanium sources Type A1 Journal article
Year 2016 Publication Environmental science : nano Abbreviated Journal Environ Sci-Nano
Volume 3 Issue 5 Pages 1052-1061
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract We present a green, biological production route for silica-titania photocatalysts using diatom microalgae. Diatoms are single-celled, eukaryotic microalgae (2-2000 mu m) that self-assemble soluble silicon (Si(OH)(4)) into intricate silica cell walls, called frustules. These diatom frustules are formed under ambient conditions and consist of hydrated silica with specific 3D morphologies and micro-meso or macroporosity. A remarkable characteristic of diatoms is their ability to bioaccumulate soluble titanium from cell culture medium and incorporate them into their nanostructured silica cell wall. Controlled cultivation of the diatom Pinnularia sp. on soluble titanium in a batch process resulted in the biological immobilisation of titanium dioxide in the porous 3D architecture of the frustules. Six different titanium sources are tested. The silica-titania frustules were isolated by treating the harvested Pinnularia cells with nitric acid (65%) or by high temperature treatment. Thermal annealing converted the amorphous titania into crystalline titania. The produced silica-titania material is evaluated towards photocatalytic activity for acetaldehyde (C2H4O) abatement. Frustules cultivated with TiBaldH showed the highest photocatalytic performance. Comparison of the photocatalytic activity with P25 reveals that P25 has a 4 fold higher photocatalytic activity, but when photocatalytic activity is normalized for titania content, the frustules show double activity. Further material characterization (morphology, crystallinity, surface area and elemental distribution) of the TiBaldH silica-titania frustules provides additional insight into their structure-activity relationship. These natural biosilicatitania materials have excellent properties for photocatalytic purposes, including high surface area (108 m(2) g(-1)) and good porosity, and show reliable immobilization of TiO2 in the ordered structure of the diatom frustule.
Address
Corporate Author Thesis
Publisher Royal Society of Chemistry Place of Publication Cambridge Editor
Language Wos 000385257900011 Publication Date 2016-07-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2051-8153; 2051-8161 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.047 Times cited 7 Open Access
Notes ; ; Approved Most recent IF: 6.047
Call Number UA @ lucian @ c:irua:144751 Serial 4644
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Author Lu, Y.; Cheng, X.; Tian, G.; Zhao, H.; He, L.; Hu, J.; Wu, S.-M.; Dong, Y.; Chang, G.-G.; Lenaerts, S.; Siffert, S.; Van Tendeloo, G.; Li, Z.-F.; Xu, L.-L.; Yang, X.-Y.; Su, B.-L.
Title Hierarchical CdS/m-TiO 2 /G ternary photocatalyst for highly active visible light-induced hydrogen production from water splitting with high stability Type A1 Journal article
Year 2018 Publication Nano energy Abbreviated Journal Nano Energy
Volume 47 Issue Pages 8-17
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract Hierarchical semiconductors are the most important photocatalysts, especially for visible light-induced hydrogen production from water splitting. We demonstrate herein a hierarchical electrostatic assembly approach to hierarchical CdS/m-TiO2/G ternary photocatalyst, which exhibits high photoactivity and excellent photostability (more than twice the activity of pure CdS while 82% of initial photoactivity remained after 15 recycles during 80 h irradiation). The ternary nanojunction effect of the photocatalyst has been investigated from orbitals hybrid, bonding energy to atom-stress distortion and nano-interface fusion. And a coherent separation mechanism of charge carriers in the ternary system has been proposed at an atomic/nanoscale. This work offers a promising way to inhibit the photocorrosion of CdS and, more importantly, provide new insights for the design of ternary nanostructured photocatalysts with an ideal heterojunction.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000430057000002 Publication Date 2018-02-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2211-2855 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.343 Times cited 58 Open Access Not_Open_Access
Notes This work supported by National Key R&D Program of China (2017YFC1103800), Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52), National Natural Science Foundation of China (U1663225, U1662134, 51472190, 51611530672, 21711530705, 51503166, 51602236, 21706199), International Science & Technology Cooperation Program of China (2015DFE52870), Natural Science Foundation of Hubei Province (2016CFA033, 2017CFB487), Open 22 Project Program of State Key Laboratory of Petroleum Pollution Control (PPC2016007) CNPC Research Institute of Safety and Environmental Technology., China Postdoctoral Science Foundation (2016M592400), Fundamental Research Funds for the Central Universities (WUT: 2017IVB012). Approved Most recent IF: 12.343
Call Number EMAT @ lucian @c:irua:150720 Serial 4925
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Author Van Tendeloo, G.; Bals, S.; Van Aert, S.; Verbeeck, J.; van Dyck, D.
Title Advanced electron microscopy for advanced materials Type A1 Journal article
Year 2012 Publication Advanced materials Abbreviated Journal Adv Mater
Volume 24 Issue 42 Pages 5655-5675
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab
Abstract The idea of this Review is to introduce newly developed possibilities of advanced electron microscopy to the materials science community. Over the last decade, electron microscopy has evolved into a full analytical tool, able to provide atomic scale information on the position, nature, and even the valency atoms. This information is classically obtained in two dimensions (2D), but can now also be obtained in 3D. We show examples of applications in the field of nanoparticles and interfaces.
Address
Corporate Author Thesis
Publisher Place of Publication Weinheim Editor
Language Wos 000310602200001 Publication Date 2012-08-21
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 107 Open Access
Notes This work was supported by funding from the European Research Council under the 7th Framework Program (FP7), ERC grant No 246791 – COUNTATOMS. J.V. Acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant 278510 VORTEX. The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium). The Qu-Ant-EM microscope was partly funded by the Hercules Fund from the Flemish Government. We thank Rafal Dunin-Borkowski for providing Figure 5d. The authors would like to thank the colleagues who have contributed to this work over the years, including K.J. Batenburg, R. Erni, B. Goris, F. Leroux, H. Lichte, A. Lubk, B. Partoens, M. D. Rossell, P. Schattschneider, B. Schoeters, D. Schryvers, H. Tan, H. Tian, S. Turner, M. van Huis. ECASJO_; Approved Most recent IF: 19.791; 2012 IF: 14.829
Call Number UA @ lucian @ c:irua:100470UA @ admin @ c:irua:100470 Serial 70
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Author Goris, B.; de Beenhouwer, J.; de Backer, A.; Zanaga, D.; Batenburg, K.J.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Van Aert, S.; Bals, S.; Sijbers, J.; Van Tendeloo, G.
Title Measuring lattice strain in three dimensions through electron microscopy Type A1 Journal article
Year 2015 Publication Nano letters Abbreviated Journal Nano Lett
Volume 15 Issue 15 Pages 6996-7001
Keywords (up) A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab
Abstract The three-dimensional (3D) atomic structure of nanomaterials, including strain, is crucial to understand their properties. Here, we investigate lattice strain in Au nanodecahedra using electron tomography. Although different electron tomography techniques enabled 3D characterizations of nanostructures at the atomic level, a reliable determination of lattice strain is not straightforward. We therefore propose a novel model-based approach from which atomic coordinates are measured. Our findings demonstrate the importance of investigating lattice strain in 3D.
Address
Corporate Author Thesis
Publisher Place of Publication Washington Editor
Language Wos 000363003100108 Publication Date 2015-09-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1530-6984;1530-6992; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.712 Times cited 87 Open Access OpenAccess
Notes Fwo; 335078 Colouratom; 267867 Plasmaquo; 312483 Esteem2; 262348 Esmi; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 12.712; 2015 IF: 13.592
Call Number c:irua:127639 c:irua:127639 Serial 1965
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