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“Control of the interfacial wettability to synthesize highly dispersed PtPd nanocrystals for efficient oxygen reduction reaction”. Wei H, Hu Z-Y, Xiao Y-X, Tian G, Ying J, Van Tendeloo G, Janiak C, Yang X-Y, Su B-L, Chemistry: an Asian journal 13, 1119 (2018). http://doi.org/10.1002/ASIA.201800191
Abstract: Highly dispersed PtPd bimetallic nanocrystals with enhanced catalytic activity and stability were prepared by adjusting the interfacial wettability of the reaction solution on a commercial carbon support. This approach holds great promise for the development of high-performance and low-cost catalysts for practical applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.083
Times cited: 3
DOI: 10.1002/ASIA.201800191
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“A facile synthesis of Ag@PdAg core-shell architecture for efficient purification of ethene feedstock”. Ma R, He Y, Feng J, Hu Z-Y, Van Tendeloo G, Li D, Journal of catalysis 369, 440 (2019). http://doi.org/10.1016/J.JCAT.2018.11.037
Abstract: Precise control of elemental configurations within multimetallic nanoparticles could enable access to functional nanomaterials with significant performance benefits. Here, we present a one-pot synthesis of supported Ag@PdAg core-shell catalyst with an ordered PdAg alloy shell and an Ag core. Both the relative reduction potential and ratio of metal precursors are essential for this synthesis strategy. The distinguished properties of Ag@PdAg, particularly the electronic structure, indicates the existence of electron modification not only between Pd and Ag on PdAg shell, but between Ag core and alloy shell. The Ag@PdAg catalyst displays 97% ethene yield in the partial hydrogenation of acetylene, which is 2.0 and 8.1 times that of over PdAg alloy and pure Pd catalysts, and this is the most selective catalyst reported to data under industrial evaluation conditions. Moreover, this core-shell structure exhibits preferable stability with comparison to PdAg alloy catalyst. The facile synthesis of core-shell architecture with alloy shell structure provides a new platform for efficient catalytic transfer of chemical resource. (C) 2018 Elsevier Inc. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.1016/J.JCAT.2018.11.037
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“Nano-single crystal coalesced PtCu nanospheres as robust bifunctional catalyst for hydrogen evolution and oxygen reduction reactions”. Li W, Hu Z-Y, Zhang Z, Wei P, Zhang J, Pu Z, Zhu J, He D, Mu S, Van Tendeloo G, Journal of catalysis 375, 164 (2019). http://doi.org/10.1016/J.JCAT.2019.05.031
Abstract: Because of high electrocatalytic activity, Pt based metal nanospheres (NSs) have attracted a lot of attention. Hence, multi-particle nano-single crystal coalesced PtCu NSs are designed and successfully synthesized by a cost-effective aqueous solution method. The formed PtCu NS catalyst exhibits a superior hydrogen evolution reaction (HER) electrocatalytic activity with an ultralow onset potential of 18 mV at the current density of 2 mA/cm(2) and high mass activity of 1.08 A/mg(pt) (7.2 times higher than that of commercial Pt/C catalysts). Also, it shows an enhancement of 3.2 and 2.7 times in the mass and specific activities toward oxygen reduction reaction (ORR) compared to that of Pt/C. Moreover, it possesses an excellent catalytic durability for both ORR and HER. Even after 10,000 cycles, its ORR mass activity retains 87% of its initial value. The density functional theory (DFT) calculations demonstrate that by introducing Cu atoms into the Pt lattice, a downshift of the D-band center and favorable hydrogen adsorption free energy of approaching to zero (Delta G) occur, indicating the increased electrocatalytic activity of Pt electrocatalysts. (C) 2019 Elsevier Inc. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.844
Times cited: 25
DOI: 10.1016/J.JCAT.2019.05.031
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“Hierarchical zeolite single-crystal reactor for excellent catalytic efficiency”. Sun M-H, Zhou J, Hu Z-Y, Chen L-H, Li L-Y, Wang Y-D, Xie Z-K, Turner S, Van Tendeloo G, Hasan T, Su B-L, Matter 3, 1226 (2020). http://doi.org/10.1016/J.MATT.2020.07.016
Abstract: As a size- and shape-selective catalyst, zeolites are widely used in petroleum and fine-chemicals processing. However, their small micropores severely hinder molecular diffusion and are sensitive to coke formation. Hierarchically porous zeolite single crystals with fully interconnected, ordered, and tunable multimodal porosity at macro-, meso-, and microlength scale, like in leaves, offer the ideal solution. However, their synthesis remains highly challenging. Here, we report a versatile confined zeolite crystallization process to achieve these superior properties. Such zeolite single crystals lead to significantly improved mass transport properties by shortening the diffusion length while maintaining shape-selective properties, endowing them with a high efficiency of zeolite crystals, enhanced catalytic activities and lifetime, highly reduced coke formation, and reduced deactivation rate in bulky-molecule reactions and methanol-to-olefins process. Their industrial utilization can lead to the design of innovative and intensified reactors and processes with highly enhanced efficiency and minimum energy consumption.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.1016/J.MATT.2020.07.016
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“Atomic defects, functional groups and properties in MXenes”. Cui W, Hu Z-Y, Unocic RR, Van Tendeloo G, Sang X, Chinese Chemical Letters 32, 339 (2021). http://doi.org/10.1016/J.CCLET.2020.04.024
Abstract: MXenes, a new family of functional two-dimensional (2D) materials, have shown great potential for an extensive variety of applications within the last decade. Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties. In this review, we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes, and how to control them to directly influence various properties (e.g., electron transport, Li' adsorption, hydrogen evolution reaction (HER) activity, and magnetism) of 2D MXenes materials. Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed. The review thus provides perspectives on property optimization through atomic defect engineering, and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes. (C) 2020 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.932
DOI: 10.1016/J.CCLET.2020.04.024
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“Size effect of bifunctional gold in hierarchical titanium oxide-gold-cadmium sulfide with slow photon effect for unprecedented visible-light hydrogen production”. Zhao H, Li C-F, Hu Z-Y, Liu J, Li Y, Hu J, Van Tendeloo G, Chen L-H, Su B-L, Journal Of Colloid And Interface Science 604, 131 (2021). http://doi.org/10.1016/J.JCIS.2021.06.167
Abstract: Gold nanoparticles (Au NPs) with surface plasmonic resonance (SPR) effect and excellent internal electron transfer ability have widely been combined with semiconductors for photocatalysis. However, the in-depth effects of Au NPs in multicomponent photocatalysts have not been completely understood. Herein, ternary titanium oxide-gold-cadmium sulfide (TiO2-Au-CdS, TAC) photocatalysts, based on hierarchical TiO2 inverse opal photonic crystal structure with different Au NPs sizes have been designed to reveal the SPR effect and internal electron transfer of Au NPs in the presence of slow photon effect. It appears that the SPR effect and internal electron transfer ability of Au NPs, depending on their sizes, play a synergistic effect on the photocatalytic enhancement. The ternary TAC-10 photocatalyst with – 10 nm Au NPs demonstrates an unprecedented hydrogen evolution rate of 47.6 mmolh-1g 1 under visible-light, demonstrating- 48% enhancement comparing to the sample without slow photon effect. In particular, a 9.83% apparent quantum yield under 450 nm monochromatic light is achieved for TAC-10. A model is proposed and finite-difference time-domain (FDTD) simulations reveal the size influence of Au NPs in ternary TAC photocatalysts. This work suggests that the rational design of bifunctional Au NPs coupling with slow photon effect could largely promote hydrogen production from visible-light driven water splitting. (c) 2021 Elsevier Inc. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.233
DOI: 10.1016/J.JCIS.2021.06.167
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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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“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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“Hierarchical zeolites containing embedded Cd0.2Zn0.8S as a photocatalyst for hydrogen production from seawater”. Yuan Y, Wu F-J, Xiao S-T, Wang Y-T, Yin Z-W, Van Tendeloo G, Chang G-G, Tian G, Hu Z-Y, Wu S-M, Yang X-Y, Chemical communications 59, 7275 (2023). http://doi.org/10.1039/D3CC01409F
Abstract: Uncovering an efficient and stable photocatalytic system for seawater splitting is a highly desirable but challenging goal. Herein, Cd0.2Zn0.8S@Silicalite-1 (CZS@S-1) composites, in which CZS is embedded in the hierarchical zeolite S-1, were prepared and show remarkably high activity, stability and salt resistance in seawater.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.9
DOI: 10.1039/D3CC01409F
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