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“Interface cation migration kinetics induced oxygen release heterogeneity in layered lithium cathodes”. 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, Energy Storage Materials 36, 115 (2021). http://doi.org/10.1016/J.ENSM.2020.12.018
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.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
DOI: 10.1016/J.ENSM.2020.12.018
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“Insight into the growth of multiple branched MnOOH nanorods”. Li Y, Tan H, Lebedev O, Verbeeck J, Biermans E, Van Tendeloo G, Su B-L, Crystal growth &, design 10, 2969 (2010). http://doi.org/10.1021/cg100009k
Abstract: Multiple branched manganese oxide hydroxide (MnOOH) nanorods prepared by a hydrothermal process were extensively studied by transmission electron microscopy (TEM). A model of the branch formation is proposed together with a study of the interface structure. The sword-like tip plays a crucial role for the nanorods to form different shapes. Importantly, the branching occurs at an angle of around either 57 degrees or 123 degrees. Specifically, a (111) twin plane can only be formed at the interface with a 123 degrees angle. The interfaces formed with a 57 degrees angle usually contain edge dislocations. Electron energy loss spectroscopy (EELS) demonstrates that the whole crystal has a uniform chemical composition. Interestingly, an epitaxial growth of Mn3O4 at the radial surface was also observed under electron beam irradiation; this is because of the rough purification of the products. The proposed mechanism is expected to shed light on the branched/dendrite nanostructure growth and to provide opportunities for further novel nanomaterial structure growth and design.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.055
Times cited: 41
DOI: 10.1021/cg100009k
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“Influence of neutron irradiation on X-ray diffraction, Raman spectrum and photoluminescence from pyrolytic and hot-pressed hexagonal boron nitride”. Zhou S, Xu W, Xiao Y, Xiao H, Zhang J, Wang Z, He G, Liu J, Li Y, Peeters FM, Journal of luminescence 263, 120118 (2023). http://doi.org/10.1016/J.JLUMIN.2023.120118
Abstract: Hexagonal boron nitride (hBN) is considered as an ideal semiconductor material for solid-state neutron detector, owing to its large neutron scattering section because of the low atomic number of B and excellent physical properties. Here we study the influence of neutron irradiation on crystal structure and on intermediate energy state (IMES) levels induced by the presence of impurities and defects in hBN. Large-size and thick pyrolytic and hot-pressed hBN (PBN and HBN) samples, which can be directly applied for neutron detector devices, are prepared and bombarded by neutrons with different irradiation fluences. The SEM and TEM are used to observe the sample difference of PBN and HBN. X-ray diffraction and Raman spectroscopy are applied to examine the influence of neutron irradiation on lattice structures along different crystal directions of PBN and HBN samples. Photoluminescence (PL) is employed to study the effect of neutron irradiation on IMESs in these samples. We find that the neutron irradiation does not alter the in-plane lattice structures of both PBN and HBN samples, but it can release the inter-layer tensions induced by sample growth of the PBN samples. Interestingly and surprisingly, the neutron irradiation does not affect the IMES levels responsible for PL generation, where PL is attributed mainly from phonon-assisted radiative electron-hole coupling for both PBN and HBN samples. Furthermore, the results indicate that the neutron irradiation can weaken the effective carrier-phonon coupling and exciton transitions in PBN and HBN samples. Overall, both PBN and HBN samples show some degree of the resistance to neutron irradiation in terms of these basic physical properties. The interesting and important findings from this work can help us to gain an in-depth understanding of the influence of neutron irradiation on basic physical properties of hBN materials. These effects can be taken into account when designing and applying the hBN materials for neutron detectors.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.6
Times cited: 1
DOI: 10.1016/J.JLUMIN.2023.120118
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“Identification of nano-width variants in a fully monoclinic martensitic Ni50Ti50 alloy by scanning electron microscope-based transmission Kikuchi diffraction and improved groupoid structure approach”. Zhao ZX, Ma X, Cao S, Li YY, Zeng CY, Wang DX, Yao X, Deng ZJ, Zhang XP, Materials Letters 281, 128624 (2020). http://doi.org/10.1016/J.MATLET.2020.128624
Abstract: Nano-width martensite plates in a fully martensitic Ni50Ti50 alloy are indexed successfully by using the off-axis transmission Kikuchi diffraction in scanning electron microscope (i.e., SEM-based TKD). The data obtained by SEM-TKD are effectively interpreted using an improved approach based on the framework of the theoretical groupoid structure method, where the equivalent variants transformed from the monoclinic variants are introduced to calculate all theoretical axis/angle pairs of rotation, and to formulate a complete list of source martensite to target martensite pairs. Consequently, B19' monoclinic martensite variants in NiTi alloys are identified unambiguously, by using numerical comparison between the experimental and theoretical rotation components, without the reference of retained parent phase. (C) 2020 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3
DOI: 10.1016/J.MATLET.2020.128624
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“High-voltage cycling induced thermal vulnerability in LiCoO₂, cathode : cation loss and oxygen release driven by oxygen vacancy migration”. Sun C, Liao X, Xia F, Zhao Y, Zhang L, Mu S, Shi S, Li Y, Peng H, Van Tendeloo G, Zhao K, Wu J, Acs Nano 14, 6181 (2020). http://doi.org/10.1021/ACSNANO.0C02237
Abstract: The release of the lattice oxygen due to the thermal degradation of layered lithium transition metal oxides is one of the major safety concerns in Li-ion batteries. The oxygen release is generally attributed to the phase transitions from the layered structure to spinel and rocksalt structures that contain less lattice oxygen. Here, a different degradation pathway in LiCoO2 is found, through oxygen vacancy facilitated cation migration and reduction. This process leaves undercoordinated oxygen that gives rise to oxygen release while the structure integrity of the defect-free region is mostly preserved. This oxygen release mechanism can be called surface degradation due to the kinetic control of the cation migration but has a slow surface to bulk propagation with continuous loss of the surface cation ions. It is also strongly correlated with the high-voltage cycling defects that end up with a significant local oxygen release at low temperatures. This work unveils the thermal vulnerability of high-voltage Li-ion batteries and the critical role of the surface fraction as a general mitigating approach.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 17.1
Times cited: 8
DOI: 10.1021/ACSNANO.0C02237
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“Gas permeation through graphdiyne-based nanoporous membranes”. Zhou Z, Tan Y, Yang Q, Bera A, Xiong Z, Yagmurcukardes M, Kim M, Zou Y, Wang G, Mishchenko A, Timokhin I, Wang C, Wang H, Yang C, Lu Y, Boya R, Liao H, Haigh S, Liu H, Peeters FM, Li Y, Geim AK, Hu S, Nature communications 13, 4031 (2022). http://doi.org/10.1038/S41467-022-31779-2
Abstract: Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeance. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of similar to 0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 16.6
Times cited: 21
DOI: 10.1038/S41467-022-31779-2
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“Fano resonances in bilayer phosphorene nanoring”. Zhang R, Wu Z, Li XJ, Li LL, Chen Q, Li Y-M, Peeters FM, Nanotechnology 29, 215202 (2018). http://doi.org/10.1088/1361-6528/AAB534
Abstract: Tunable transport properties and Fano resonances are predicted in a circular bilayer phosphorene nanoring. The conductance exhibits Fano resonances with varying incident energy and applied perpendicular magnetic field. These Fano resonance peaks can be accurately fitted with the well known Fano curves. When a magnetic field is applied to the nanoring, the conductance oscillates periodically with magnetic field which is reminiscent of the Aharonov-Bohm effect. Fano resonances are tightly related to the discrete states in the central nanoring, some of which are tunable by the magnetic field.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 3.44
Times cited: 4
DOI: 10.1088/1361-6528/AAB534
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“Evidence that supertriangles exist in nature from the vertical projections of Koelreuteria paniculata fruit”. Li Y, Quinn BK, Gielis J, Li Y, Shi P, Symmetry 14, 23 (2022). http://doi.org/10.3390/SYM14010023
Abstract: Many natural radial symmetrical shapes (e.g., sea stars) follow the Gielis equation (GE) or its twin equation (TGE). A supertriangle (three triangles arranged around a central polygon) represents such a shape, but no study has tested whether natural shapes can be represented as/are supertriangles or whether the GE or TGE can describe their shape. We collected 100 pieces of Koelreuteria paniculata fruit, which have a supertriangular shape, extracted the boundary coordinates for their vertical projections, and then fitted them with the GE and TGE. The adjusted root mean square errors (RMSEadj) of the two equations were always less than 0.08, and >70% were less than 0.05. For 57/100 fruit projections, the GE had a lower RMSEadj than the TGE, although overall differences in the goodness of fit were non-significant. However, the TGE produces more symmetrical shapes than the GE as the two parameters controlling the extent of symmetry in it are approximately equal. This work demonstrates that natural supertriangles exist, validates the use of the GE and TGE to model their shapes, and suggests that different complex radially symmetrical shapes can be generated by the same equation, implying that different types of biological symmetry may result from the same biophysical mechanisms.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.7
DOI: 10.3390/SYM14010023
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“Enzyme immobilization on/in polymeric membranes : status, challenges and perspectives in biocatalytic membrane reactors (BMRs)”. Jochems P, Satyawali Y, Diels L, Dejonghe W, Green chemistry : cutting-edge research for a greener sustainable future 13, 1609 (2011). http://doi.org/10.1039/C1GC15178A
Abstract: Immobilization of enzymes is beneficial in terms of improving the process economics by enabling enzyme re-use and enhancing overall productivity and robustness. Increasingly, membranes are thought to be good supports for enzyme immobilization. These resulting biocatalytic membranes are integrated in reactors known as biocatalytic membrane reactors (BMRs) which enable the integration of biocatalysis and separation. Often the available commercial membranes require modifications to make them suitable for enzyme immobilization. Different immobilization techniques can be used on such suitable membranes, but no general rules exist for making a choice between them. Despite the advantages of BMR application, there are some issues which need to be addressed in order to achieve up-scaling of such systems. In this review, the different aspects of enzyme immobilization on membranes are discussed to show the complexity of this interdisciplinary technology. In addition, the existing issues which require further investigation are highlighted.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1039/C1GC15178A
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“Engineering single crystalline Mn3O4 nano-octahedra with exposed highly active {011} facets for high performance lithium ion batteries”. Huang S-Z, Jin J, Cai Y, Li Y, Tan H-Y, Wang H-E, Van Tendeloo G, Su B-L, Nanoscale 6, 6819 (2014). http://doi.org/10.1039/c4nr01389a
Abstract: Well shaped single crystalline Mn3O4 nano-octahedra with exposed highly active {011} facets at different particle sizes have been synthesized and used as anode materials for lithium ion batteries. The electrochemical results show that the smallest sized Mn3O4 nano-octahedra show the best cycling performance with a high initial charge capacity of 907 mA h g−1 and a 50th charge capacity of 500 mA h g−1 at a current density of 50 mA g−1 and the best rate capability with a charge capacity of 350 mA h g−1 when cycled at 500 mA g−1. In particular, the nano-octahedra samples demonstrate a much better electrochemical performance in comparison with irregular shaped Mn3O4 nanoparticles. The best electrochemical properties of the smallest Mn3O4 nano-octahedra are ascribed to the lower charge transfer resistance due to the exposed highly active {011} facets, which can facilitate the conversion reaction of Mn3O4 and Li owing to the alternating Mn and O atom layers, resulting in easy formation and decomposition of the amorphous Li2O and the multi-electron reaction. On the other hand, the best electrochemical properties of the smallest Mn3O4 nano-octahedra can also be attributed to the smallest size resulting in the highest specific surface area, which provides maximum contact with the electrolyte and facilitates the rapid Li-ion diffusion at the electrode/electrolyte interface and fast lithium-ion transportation within the particles. The synergy of the exposed {011} facets and the smallest size (and/or the highest surface area) led to the best performance for the Mn3O4 nano-octahedra. Furthermore, HRTEM observations verify the oxidation of MnO to Mn3O4 during the charging process and confirm that the Mn3O4 octahedral structure can still be partly maintained after 50 dischargecharge cycles. The high Li-ion storage capacity and excellent cycling performance suggest that Mn3O4 nano-octahedra with exposed highly active {011} facets could be excellent anode materials for high-performance lithium-ion batteries.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 80
DOI: 10.1039/c4nr01389a
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“Ellipticalness index : a simple measure of the complexity of oval leaf shape”. Li Y, Quinn BK, Niinemets Ü, Schrader J, Gielis J, Liu M, Shi P, Pakistan journal of botany : An official publication of pakistan botanical society 54, 1 (2022). http://doi.org/10.30848/PJB2022-6(44)
Abstract: Plants have diverse leaf shapes that have evolved to adapt to the environments they have experienced over their evolutionary history. Leaf shape and leaf size can greatly influence the growth rate, competitive ability, and productivity of plants. However, researchers have long struggled to decide how to properly quantify the complexity of leaf shape. Prior studies recommended the leaf roundness index (RI = 4πA/P2) or dissection index (DI = ), where P is leaf perimeter and A is leaf area. However, these two indices merely measure the extent of the deviation of leaf shape from a circle, which is usually invalid as leaves are seldom circular. In this study, we proposed a simple measure, named the ellipticalness index (EI), for quantifying the complexity of leaf shape based on the hypothesis that the shape of any oval leaf can be regarded as a variation from a standard ellipse. 2220 leaves from nine species of Magnoliaceae were sampled to check the validity of the EI. We also tested the validity of the Montgomery equation (ME), which assumes a proportional relationship between leaf area and the product of leaf length and width, because the EI actually comes from the proportionality coefficient of the ME. We also compared the ME with five other models of leaf area. The ME was found to be the best model for calculating leaf area based on consideration of the trade-off between model fit vs. complexity, which strongly supported the robustness of the EI for describing oval leaf shape. The new index can account for both leaf shape and size, and we conclude that it is a promising method for quantifying and comparing oval leaf shapes across species in future studies.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 1.2
DOI: 10.30848/PJB2022-6(44)
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“Effect of Ag addition on the precipitation evolution and interfacial segregation for Al-Mg-Si alloy”. Weng Y, Ding L, Zhang Z, Jia Z, Wen B, Liu Y, Muraishi S, Li Y, Liu Q, Acta materialia 180, 301 (2019). http://doi.org/10.1016/J.ACTAMAT.2019.09.015
Abstract: The effect of Ag addition on the precipitation evolution and interfacial segregation for Al-Mg-Si alloys was systematically investigated by atomic resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), atom probe tomography (APT) and density functional theory (DFT) calculation. At the early aging stage, Ag atoms could enter clusters and refine the distribution of these clusters. Then, Ag atoms preferentially segregate at the GP zone/alpha-Al and beta ''/alpha-Al interfaces at the peak aging stage by the replacement of Al atoms in FCC matrix. With prolonging aging time, Ag atoms generally incorporate into the interior of beta '' precipitate, facilitating the formation of QP lattice (a hexagonal network of Si atomic columns) and the local symmetry substructures, Ag sub-unit (1) and Ag sub-unit (2). At the over-aged stage, the Ag sub-unit (1) and Ag sub-unit (2) could transform to the beta'(Ag) (i.e. beta'(Ag1) and beta'(Ag2).) and Q'(Ag) unit cells, respectively. All the precipitates at the over-aging stage have a composite and disordered structure due to the coexistence of different unit cells (beta'(Ag1), beta'(Ag2), Q'(Ag) and beta') and the non-periodic arrangement of Ag atoms within the precipitate. In the equilibrium stage, the incorporated Ag atoms in the precipitates release into the alpha-Al matrix as solute atoms or form Ag particles. In general, Ag atoms undergo a process of “segregate at the precipitate/matrix interface -> incorporate into the interior of precipitate -> release into the alpha-Al matrix” during the precipitation for Al-Mg-Si-Ag alloys. Besides, Ag segregation is found at the interfaces of almost all metastable phases (including GP zone, beta '', beta'/beta'(Ag) phase) in Al-Mg-Si-Ag alloys. The Ag segregation at the beta'/alpha-Al interface could increase the length/diameter ratio of beta' phase and thus promote the additional strengthening potential of these alloys. These findings provide a new route for precipitation hardening by promoting the nucleation and morphology evolution of precipitates. (C) 2019 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
DOI: 10.1016/J.ACTAMAT.2019.09.015
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“Edge stabilization in reduced-dimensional perovskites”. Quan LN, Ma D, Zhao Y, Voznyy O, Yuan H, Bladt E, Pan J, de Arquer FPG, Sabatini R, Piontkowski Z, Emwas A-H, Todorovic P, Quintero-Bermudez R, Walters G, Fan JZ, Liu M, Tan H, Saidaminov M I, Gao L, Li Y, Anjum DH, Wei N, Tang J, McCamant DW, Roeffaers MBJ, Bals S, Hofkens J, Bakr OM, Lu Z-H, Sargent EH, Nature Communications 11, 170 (2020). http://doi.org/10.1038/S41467-019-13944-2
Abstract: Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 +/- 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m(-2); their maximum luminance is 4.5 x 10(4) cd m(-2) (corresponding to an EQE of 5%); and, at 4000 cd m(-2), they achieve an operational half-lifetime of 3.5 h.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 147
DOI: 10.1038/S41467-019-13944-2
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“Directly revealing the structure-property correlation in Na+-doped cathode materials”. Li C-F, Chen L-D, Wu L, Liu Y, Hu Z-Y, Cui W-J, Dong W-D, Liu X, Yu W-B, Li Y, Van Tendeloo G, Su B-L, Applied surface science 612, 155810 (2023). http://doi.org/10.1016/J.APSUSC.2022.155810
Abstract: The introduction of Na+ is considered as an effective way to improve the performance of Ni-rich cathode materials. However, the direct structure-property correlation for Na+ doped NCM-based cathode materials remain unclear, due to the difficulty of local and accurate structural characterization for light elements such as Li and Na. Moreover, there is the complexity of the modeling for the whole Li ion battery (LIB) system. To tackle the above-mentioned issues, we prepared Na+-doped LiNi0.6Co0.2Mn0.2O2 (Na-NCM622) material. The crystal structure change and the lattice distortion with picometers precision of the Na+-doped material is revealed by Cs-corrected scanning transmission electron microscopy (STEM). Density functional theory (DFT) and the recently proposed electrochemical model, i.e., modified Planck-Nernst-Poisson coupled Frumkin-Butler-Volmer (MPNP-FBV), has been applied to reveal correlations between the activation energy and the charge transfer resistance at multiscale. It is shown that Na+ doping can reduce the activation energy barrier from. G = 1.10 eV to 1.05 eV, resulting in a reduction of the interfacial resistance from 297 O to 134 Omega. Consequently, the Na-NCM622 cathode delivers a superior capacity retention of 90.8 % (159 mAh.g(-1)) after 100 cycles compared to the pristine NCM622 (67.5 %, 108 mAh.g(-1)). Our results demonstrate that the kinetics of Li+ diffusion and the electrochemical reaction can be enhanced by Na+ doping the cathode material.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.7
DOI: 10.1016/J.APSUSC.2022.155810
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“Cut-off voltage influencing the voltage decay of single crystal lithium-rich manganese-based cathode materials in lithium-ion batteries”. Yuan M-M, Wang L-D, Zhang J, Ran M-J, Wang K, Hu Z-Y, Van Tendeloo G, Li Y, Su B-L, Journal of colloid and interface science 674, 238 (2024). http://doi.org/10.1016/J.JCIS.2024.06.131
Abstract: The voltage decay of Li -rich layered oxide cathode materials results in the deterioration of cycling performance and continuous energy loss, which seriously hinders their application in the high-energy – density lithium -ion battery (LIB) market. However, the origin of the voltage decay mechanism remains controversial due to the complex influences of transition metal (TM) migration, oxygen release, indistinguishable surface/bulk reactions and the easy intra/inter-crystalline cracking during cycling. We investigated the direct cause of voltage decay in micrometer -scale single -crystal Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 (SC-LNCM) cathode materials by regulating the cut-off voltage. The redox of TM and O 2- ions can be precisely controlled by setting different voltage windows, while the cracking can be restrained, and surface/bulk structural evaluation can be monitored because of the large single crystal size. The results show that the voltage decay of SC-LNCM is related to the combined effect of cation rearrangement and oxygen release. Maintaining the discharge cutoff voltage at 3 V or the charging cutoff voltage at 4.5 V effectively mitigates the voltage decay, which provides a solution for suppressing the voltage decay of Lirich and Mn-based layered oxide cathode materials. Our work provides significant insights into the origin of the voltage decay mechanism and an easily achievable strategy to restrain the voltage decay for Li -rich and Mn-based cathode materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.9
DOI: 10.1016/J.JCIS.2024.06.131
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“Controlling the diameters in large-scale synthesis of single-walled carbon nanotubes by catalytic decomposition of CH4”. Li Y, Zhang X, Shen L, Luo J, Tao X, Liu F, Xu G, Wang Y, Geise HJ, Van Tendeloo G, Chemical physics letters 398, 276 (2004). http://doi.org/10.1016/j.cplett.2004.09.068
Abstract: High-quality single-walled carbon nanotubes (SWNTs) are synthesized in gram amount on Fe-Mo/MgO catalysts by catalytic decomposition of CH4 in H-2 or N-2. Raman data reveal that the as-prepared SATNTs have a diameter of about 0.74-1.29 nm. It is found that the diameter of the as-prepared SWNTs can be controlled mainly by adjusting the molar ratio of Fe-Mo versus the MgO support. Several other factors that potentially influence the growth of SWNTs have been studied in detail. The experimental results show that the nature of the catalyst determines the diameter of the as-prepared SWNTs. (C) 2004 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.815
Times cited: 45
DOI: 10.1016/j.cplett.2004.09.068
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“Controllable synthesis of novel one-dimensional carbon nanomaterials on an alkali-element-modified Cu catalyst”. Tao XY, Zhang XB, Cheng J-P, Liu F, Li Y, Van Tendeloo G, Nanotechnology 17, 224 (2006). http://doi.org/10.1088/0957-4484/17/1/037
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.44
Times cited: 4
DOI: 10.1088/0957-4484/17/1/037
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“Cocatalyzing Pt/PtO phase-junction nanodots on hierarchically porous TiO2 for highly enhanced photocatalytic hydrogen production”. Ren X-N, Hu Z-Y, Jin J, Wu L, Wang C, Liu J, Liu F, Wu M, Li Y, Van Tendeloo G, Su B-L, ACS applied materials and interfaces 9, 29687 (2017). http://doi.org/10.1021/ACSAMI.7B07226
Abstract: Phase-junctions. between a cocatalyst and its semiconductor host are quite effective to enhance the photo catalytic activity and are widely studied, while reports on the phase-juncted cocatalyst are still rare. In this work, we report the deposition of the Pt/PtO phase-juncted nanodots as cocatalyst via NaOH modification of an interconnected meso-macroporous TiO2 network with high surface area and inner-particle mesopores to enhance the performance of photocatalytic H-2 production. Our results show that NaOH modification can largely influence Pt/PtO phase-juncted nanodot formation and dispersity. Compared to the TiO2 nano particles, the hierarchically meso-macroporous TiO2 network containing 0.18 wt % Pt/PtO phase-juneted cocatalyst demonstrates a highest photocatalytic H-2 rate of 13 mmol g(-1) h(-1) under simulated solar light, and possesses a stable cycling activity without obvious decrease after five cycles. Such high H-2 production performance can be attributed to both the phase-juncted Pt/PtO providing more active sites while PtO suppresses the undesirable hydrogen back reaction, and the special hierarchically porous TiO2 network with inner-particle mesopores presenting short diffusion path lengths for photogenerated electrons and enhanced light harvesting efficiency. This work suggests that Pt/PtO phase-juncted cocatalyst on hierarchically porous TiO2 nanostructures is a promising strategy for advanced photocatalytic H-2 production.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.504
Times cited: 18
DOI: 10.1021/ACSAMI.7B07226
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“Chemistry of trimethyl aluminum: a spontaneous route to thermally stable 3D crystalline macroporous alumina foams with a hierarchy of pore sizes”. Li Y, Yang X-Y, Tian G, Vantomme A, Yu J, Van Tendeloo G, Su B-L, Chemistry of materials 22, 3251 (2010). http://doi.org/10.1021/cm100491r
Abstract: A simple and spontaneous one-pot self-formation procedure that is easy to scale up has been developed based on the chemistry of trimethylaluminum (TMA), leading to thermally stable macroporous crystalline alumina with a very unique and unprecedented three-dimensional (3D) hierarchical pore structure consisting of well-defined wormlike mesopores. TMA is the precursor of both product and porogene (viz, two working functions within the same molecule (2 in 1)). The materials obtained have been intensively characterized by powder X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), N2 adsorption−desorption, and mercury porosimetry. The open cagelike macrocavities are self-constructed by mesoporous nanorods (diameter of ca. 40−70 nm), which are themselves formed by a random assembly of fibrous nanoparticles 5−6 nm in size. Optical microscopy (OM) has been used in situ to follow the synthesis procedure, which led to the proposal of the formation mechanism. Methane molecules as porogens, which were instantaneously released because of the fast hydrolysis of the chemical precursor, were the key factor in producing these 3D structures with uniform co-continuous macropores that interconnected directly with the wormlike mesopores. The important characteristic of this procedure is the concurrent formation of a multiscaled porous network. The material exhibits great thermal stability. The hierarchically mesoporous−macroporous Al2O3 obtained is quite attractive for a myriad of applications, from catalysis to biomedicine. The present work illustrates that the one-pot self-formation concept, based on the chemistry of alkyl metals, is a versatile method to design industrially valuable hierarchically porous materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 38
DOI: 10.1021/cm100491r
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“Characterization and optimization of \beta-galactosidase immobilization process on a mixed-matrix membrane”. Jochems P, Satyawali Y, van Roy S, Doyen W, Diels L, Dejonghe W, Enzyme and microbial technology 49, 580 (2011). http://doi.org/10.1016/J.ENZMICTEC.2011.06.010
Abstract: β-Galactosidase is an important enzyme catalyzing not only the hydrolysis of lactose to the monosaccharides glucose and galactose but also the transgalactosylation reaction to produce galacto-oligosaccharides (GOS). In this study, β-galactosidase was immobilized by adsorption on a mixed-matrix membrane containing zirconium dioxide. The maximum β-galactosidase adsorbed on these membranes was 1.6 g/m2, however, maximal activity was achieved at an enzyme concentration of around 0.5 g/m2. The tests conducted to investigate the optimal immobilization parameters suggested that higher immobilization can be achieved under extreme parameters (pH and temperature) but the activity was not retained at such extreme operational parameters. The investigations on immobilized enzymes indicated that no real shift occurred in its optimal temperature after immobilization though the activity in case of immobilized enzyme was better retained at lower temperature (5 °C). A shift of 0.5 unit was observed in optimal pH after immobilization (pH 6.5 to 7). Perhaps the most striking results are the kinetic parameters of the immobilized enzyme; while the Michaelis constant (Km) value increased almost eight times compared to the free enzyme, the maximum enzyme velocity (Vmax) remained almost constant.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.ENZMICTEC.2011.06.010
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“Characterization and analysis of the adsorption immobilization mechanism of \beta-galactosidase on metal oxide powders”. Satyawali Y, Van Roy S, Roevens A, Meynen V, Mullens S, Jochems P, Doyen W, Cauwenberghs L, Dejonghe W, RSC advances 3, 24054 (2013). http://doi.org/10.1039/C3RA45107K
Abstract: Immobilization of the enzymes plays a vital role in enhancing their applicability in a wide range of applications, thus ensuring the use of sustainable enzymatic processes over the conventional chemical processes on an industrial scale. This study provides the background information for the selection and screening of inorganic metal oxide (MO) powders for their use as fillers in mixed matrix membranes for enzyme immobilization as the future aim. A total of 13 MOs, ranging in size from 0.01 μm to <5 μm, were tested for their performance as a support for enzyme (β-galactosidase) immobilization via adsorption. Alumina appeared to be the best performing MO with the amount and activity of the immobilized enzyme being 64 mg g−1 and up to 288 U g−1, respectively. The amount of immobilized enzyme on alumina (α-Al2O3 C and γ-Al2O3) was >3 times higher than ZrO2 (used as a reference MO in this study). Upon heat treatment at 900 °C, up to 15%, 52% and 42% decline was observed in the amount of immobilized enzyme in case of alumina metal oxides (MOs), ZrO2 and TiO2, respectively. The results suggested that both isoelectric point and surface area of the MO influence the immobilization. The most important observation in this study was that the bonding of the enzyme to the MO surface seems to be mediated by the bonding/interaction of the buffer to the enzyme.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1039/C3RA45107K
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“Blue-edge slow photons promoting visible-light hydrogen production on gradient ternary 3DOM TiO 2 -Au-CdS photonic crystals”. Zhao H, Hu Z, Liu J, Li Y, Wu M, Van Tendeloo G, Su B-L, Nano energy 47, 266 (2018). http://doi.org/10.1016/j.nanoen.2018.02.052
Abstract: The slow photon effect, a structural effect of photonic crystal photocatalyst, is very efficient in the enhancement of photocatalytic reactions. However, slow photons in powdered photonic crystal photocatalyst have rarely been discussed because they are usually randomly oriented when the photocatalytic reaction happens in solution under constant stirring. In this work, for the first time we design a gradient ternary TiO2-Au-CdS photonic crystal based on three-dimensionally ordered macroporous (3DOM) TiO2 as skeleton, Au as electron transfer medium and CdS as active material for photocatalytic H2 production under visible-light. As a result, this gradient ternary photocatalyst is favorable to simultaneously enhance light absorption, extend the light responsive region and reduce the recombination rate of the charge carriers. In particular, we found that slow photons at blue-edge exhibit much higher photocatalytic activity than that at red-edge. The photonic crystal photocatalyst with a macropore size of 250 nm exhibits the highest visible-light H2 production rate of 3.50 mmolh⁻¹g⁻¹ due to the slow photon energy at the blue-edge to significantly enhance the incident photons utilization. This work verifies that slow photons at the blue-edge can largely enhance light harvesting and sheds a light on designing the powdered photonic crystal photocatalyst to promote the photocatalytic H2 production via slow photon effect.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.343
Times cited: 33
DOI: 10.1016/j.nanoen.2018.02.052
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“BiVo4/3DOM TiO2 nanocomposites : effect of BiVO4 as highly efficient visible light sensitizer for highly improved visible light photocatalytic activity in the degradation of dye pollutants”. Zalfani M, Hu Z-Y, Yu W-B, Mahdouani M, Bourguiga R, Wu M, Li Y, Van Tendeloo G, Djoued Y, Su B-L, Applied catalysis : B : environmental 205, 121 (2017). http://doi.org/10.1016/J.APCATB.2016.12.019
Abstract: A series of BiVO4/3DOM TiO2 nanocomposites have been synthesized and their photocatalytic activity was investigated under visible light irradiation using the RhB dye as model pollutant molecule in an aqueous solution. The effect of the amount of BiVO4 as visible light sensitizer on the photocatalytic activity of BiVO4/3DOM TiO2 nanocomposites was highlighted. The heterostructured composite system leads to much higher photocatalytic efficiencies than bare 3DOM TiO2 and BiVO4 nanoparticles. As the proportion of BiVO4 in BiVO4/3DOM TiO2 nanocomposites increases from 0.04 to 0.6, the photocatalytic performance of the BiVO4/3DOM TiO2 nanocomposites increases and then decreases after reaching a maximum at 0.2. This improvement in photocatalytic perfomance is related to 1) the interfacial electron transfer efficiency between the coupled materials, 2) the 3DOM TiO2 inverse opal structure with interconnected pores providing an easy mass transfer of the reactant molecules and high accessibility to the active sites and large surface area and 3) the effect of light sensitizer of BiVO4. Intensive studies on structural, textural, optical and surface properties reveal that the electronic interactions between BiVO4 and TiO2 lead to an improved charge separation of the coupled BiVO4/TiO2 system. The photogenerated charge carrier densities increase with increasing the BiVO4 content, which acts as visible light sensitizer to the TiO2 and is responsible for the enhancement in the rate of photocatalytic degradation. However, the photocatalytic activity is reduced when the BiVO4 amount is much higher than that of 3DOM TiO2. Two reasons could account for this behavior. First, with increasing BiVO4 content, the photogenerated electron/hole pairs are accumulated at the surface of the BiVO4 nanoparticles and the recombination rate increases as shown by the PL results. Second, decreasing the amount of 3DOM TiO2 in the nanocomposite decreases the surface area as shown by the BET results. Moreover, the poor adsorptive properties of the BiVO4 photocatalyst also affect the photocatalytic performance, in particular at higher BiVO4 content. The present work demonstrates that BiVO4/3DOM TiO2 is a very promising heterojunction system for visible light photocatalytic applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.446
Times cited: 52
DOI: 10.1016/J.APCATB.2016.12.019
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“BiVO4/3DOM TiO2 nanocomposites: Effect of BiVO4 as highly efficient visible light sensitizer for highly improved visible light photocatalytic activity in the degradation of dye pollutants”. Zalfani M, Hu Z-Y, Yu W-B, Mahdouani M, Bourguig R, Wu M, Li Y, Van Tendeloo G, Djoued Y, Su B-L, Applied Catalysis B-Environmental 205, 121 (2016). http://doi.org/10.1016/j.apcatb.2016.12.019
Abstract: A series of BiVO4/3DOM TiO2 nanocomposites have been synthesized and their photocatalytic activity was investigated under visible light irradiation using the RhB dye as model pollutant molecule in an aqueous solution. The effect of the amount of BiVO4 as visible light sensitizer on the photocatalytic activity of BiVO4/3DOM TiO2 nanocomposites was highlighted. The heterostructured composite system leads to much higher photocatalytic efficiencies than bare 3DOM TiO2 and BiVO4 nanoparticles. As the proportion of BiVO4 in BiVO4/3DOM TiO2 nanocomposites increases from 0.04 to 0.6, the photocatalytic performance of the BiVO4/3DOM TiO2 nanocomposites increases and then decreases after reaching a maximum at 0.2. This improvement in photocatalytic perfomance is related to 1) the interfacial electron transfer efficiency between the coupled materials, 2) the 3DOM TiO2 inverse opal structure with interconnected pores providing an easy mass transfer of the reactant molecules and high accessibility to the active sites and large surface area and 3) the effect of light sensitizer of BiVO4. Intensive studies on structural, textural, optical and surface properties reveal that the electronic interactions between BiVO4 and TiO2 lead to an improved charge separation of the coupled BiVO4/TiO2 system. The photogenerated charge carrier densities increase with increasing the BiVO4 content, which acts as visible light sensitizer to the TiO2 and is responsible for the enhancement in the rate of photocatalytic degradation. However, the photocatalytic activity is reduced when the BiVO4 amount is much higher than that of 3DOM TiO2. Two reasons could account for this behavior. First, with increasing BiVO4 content, the photogenerated electron/hole pairs are accumulated at the surface of the BiVO4 nanoparticles and the recombination rate increases as shown by the PL results. Second, decreasing the amount of 3DOM TiO2 in the nanocomposite decreases the surface area as shown by the BET results. Moreover, the poor adsorptive properties of the BiVO4 photocatalyst also affect the photocatalytic performance, in particular at higher BiVO4 content. The present work demonstrates that BiVO4/3DOM TiO2 is a very promising heterojunction system for visible light photocatalytic applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.446
Times cited: 52
DOI: 10.1016/j.apcatb.2016.12.019
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“Bioinspired noncyclic transfer pathway electron donors for unprecedented hydrogen production”. Liu J, Wang C, Yu W, Zhao H, Hu Z-Y, Liu F, Hasan T, Li Y, Van Tendeloo G, Li C, Su B-L, CCS chemistry 5, 1470 (2023). http://doi.org/10.31635/CCSCHEM.022.202202071
Abstract: Electron donors are widely exploited in visible-light photocatalytic hydrogen production. As a typical electron donor pair and often the first choice for hydrogen production, the sodium sulfide-sodium sulfite pair has been extensively used. However, the resultant thiosulfate ions consume the photogenerated electrons to form an undesirable pseudocyclic electron transfer pathway during the photocatalytic process, strongly limiting the solar energy conversion efficiency. Here, we report novel and bioinspired electron donor pairs offering a noncyclic electron transfer pathway that provides more electrons without the consumption of the photogenerated electrons. Compared to the state-of-the-art electron donor pair Na2S-Na2SO3, these novel Na2S-NaH2PO2 and Na2S-NaNO2 electron donor pairs enable an unprecedented enhancement of up to 370% and 140% for average photocatalytic H-2 production over commercial CdS nanoparticles, and they are versatile for a large series of photocatalysts for visible-light water splitting. The discovery of these novel electron donor pairs can lead to a revolution in photocatalysis and is of great significance for industrial visible-light-driven H-2 production. [GRAPHICS] .
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.31635/CCSCHEM.022.202202071
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“Behavior of Ni-doped MgMoO4 single-phase catalysts for synthesis of multiwalled carbon nanotube bundles”. Li Y, Zhang X, Geise HJ, Van Tendeloo G, Chemical vapor deposition 13, 30 (2007). http://doi.org/10.1002/cvde.200606531
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.333
Times cited: 4
DOI: 10.1002/cvde.200606531
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“An elliptical blade is not a true ellipse, but a superellipse : evidence from two Michelia species”. Li Y, Niklas KJ, Gielis J, Niinemets Ü, Schrader J, Wang R, Shi P, Journal of forestry research 33, 1341 (2022). http://doi.org/10.1007/S11676-021-01385-X
Abstract: The shape of leaf laminae exhibits considerable diversity and complexity that reflects adaptations to environmental factors such as ambient light and precipitation as well as phyletic legacy. Many leaves appear to be elliptical which may represent a ‘default’ developmental condition. However, whether their geometry truly conforms to the ellipse equation (EE), i.e., (x/a)2 + (y/b)2 = 1, remains conjectural. One alternative is described by the superellipse equation (SE), a generalized version of EE, i.e., |x/a|n +|y/b|n = 1. To test the efficacy of EE versus SE to describe leaf geometry, the leaf shapes of two Michelia species (i.e., M. cavaleriei var. platypetala, and M. maudiae), were investigated using 60 leaves from each species. Analysis shows that the majority of leaves (118 out of 120) had adjusted root-mean-square errors of < 0.05 for the nonlinear fitting of SE to leaf geometry, i.e., the mean absolute deviation from the polar point to leaf marginal points was smaller than 5% of the radius of a hypothesized circle with its area equaling leaf area. The estimates of n for the two species were ˂ 2, indicating that all sampled leaves conformed to SE and not to EE. This study confirms the existence of SE in leaves, linking this to its potential functional advantages, particularly the possible influence of leaf shape on hydraulic conductance.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3
DOI: 10.1007/S11676-021-01385-X
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“Active site titration of immobilized beta-galactosidase for the determination of active enzymes”. Jochems P, Mueller T, Satyawali Y, Diels L, Dejonghe W, Hanefeld U, Biochemical engineering journal 93, 137 (2015). http://doi.org/10.1016/J.BEJ.2014.10.007
Abstract: In the present study, an active site titration method is demonstrated, to determine the amount of active enzyme (beta-galactosidase), immobilized on a support. Two types of supports were investigated, viz, amino acrylic resin and a mixed matrix membrane. Furthermore, 2',4'-dinitrophenyl 2-deoxy-2-fluoro-beta-D-galactopyranoside was used as an inhibitor for the active site titration of immobilized beta-galactosidase obtained from Kluyveromyces lactis. Using the active site titration, approximately 8.3 mg of active enzyme was found on 1 g of dried commercially available SPRIN imibond, which is an amino acrylic resin with covalently bound beta-galactosidase obtained from K. lactis. However, this method, in its present form, was not effective on the mixed matrix membranes due to the irreversible partial adsorption of the leaving group (2',4'-dinitrophenolate) by the membrane. This observation implied that it is important to investigate interactions between the support and the used inhibitor and leaving group. (C) 2014 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.BEJ.2014.10.007
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“A superellipse with deformation and its application in describing the cross-sectional shapes of a square bamboo”. Huang W, Li Y, Niklas KJ, Gielis J, Ding Y, Cao L, Shi P, Symmetry-Basel 12, 2073 (2020). http://doi.org/10.3390/SYM12122073
Abstract: Many cross-sectional shapes of plants have been found to approximate a superellipse rather than an ellipse. Square bamboos, belonging to the genus Chimonobambusa (Poaceae), are a group of plants with round-edged square-like culm cross sections. The initial application of superellipses to model these culm cross sections has focused on Chimonobambusa quadrangularis (Franceschi) Makino. However, there is a need for large scale empirical data to confirm this hypothesis. In this study, approximately 750 cross sections from 30 culms of C. utilis were scanned to obtain cross-sectional boundary coordinates. A superellipse exhibits a centrosymmetry, but in nature the cross sections of culms usually deviate from a standard circle, ellipse, or superellipse because of the influences of the environment and terrain, resulting in different bending and torsion forces during growth. Thus, more natural cross-sectional shapes appear to have the form of a deformed superellipse. The superellipse equation with a deformation parameter (SEDP) was used to fit boundary data. We find that the cross-sectional shapes (including outer and inner rings) of C. utilis can be well described by SEDP. The adjusted root-mean-square error of SEDP is smaller than that of the superellipse equation without a deformation parameter. A major finding is that the cross-sectional shapes can be divided into two types of superellipse curves: hyperellipses and hypoellipses, even for cross sections from the same culm. There are two proportional relationships between ring area and the product of ring length and width for both the outer and inner rings. The proportionality coefficients are significantly different, as a consequence of the two different superellipse types (i.e., hyperellipses and hypoellipses). The difference in the proportionality coefficients between hyperellipses and hypoellipses for outer rings is greater than that for inner rings. This work informs our understanding and quantifying of the longitudinal deformation of plant stems for future studies to assess the influences of the environment on stem development. This work is also informative for understanding the deviation of natural shapes from a strict rotational symmetry.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.7
DOI: 10.3390/SYM12122073
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“A hidden single-stage martensitic transformation from B2 parent phase to B19 ' martensite phase in an aged Ni51Ti49 alloy”. Zeng CY, Cao S, Li YY, Zhao ZX, Yao XY, Ma X, Zhang XP, Materials letters 253, 99 (2019). http://doi.org/10.1016/J.MATLET.2019.06.055
Abstract: The aged Ni-rich NiTi shape memory alloys (SMAs) exhibit the multi-stage martensitic transformation (MMT), which has important influences on functional properties and practical applications of the NiTi SMAs. A hidden single-stage martensitic transformation from B2 parent phase to B19' martensite phase is found in an aged Ni51Ti49 alloy, which happens concurrently with a commonly observed two-stage martensitic transformation B2-R-B19' (R: martensite phase) and actually composes one stage of a multi-stage martensitic transformation (MMT) together with the two-stage one. B2-B19' martensitic transformation occurs in the NiTi matrix containing Ni4Ti3 precipitates with relatively large inter-particle space, while B2-R-B19' transformation takes place in the NiTi matrix with Ni4Ti3 precipitates having relatively small inter-particle space. (C) 2019 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.572
DOI: 10.1016/J.MATLET.2019.06.055
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