7 results on '"H. L. Zhang"'
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2. Layered Pd oxide on PdSn nanowires for boosting direct H2O2 synthesis
- Author
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Hong-chao Li, Qiang Wan, Congcong Du, Jiafei Zhao, Fumin Li, Ying Zhang, Yanping Zheng, Mingshu Chen, Kelvin H. L. Zhang, Jianyu Huang, Gang Fu, Sen Lin, Xiaoqing Huang, and Haifeng Xiong
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Multidisciplinary ,General Physics and Astronomy ,General Chemistry ,General Biochemistry, Genetics and Molecular Biology - Abstract
Hydrogen peroxide (H2O2) has the wide range of applications in industry and living life. However, the development of the efficient heterogeneous catalyst in the direct H2O2 synthesis (DHS) from H2 and O2 remains a formidable challenge because of the low H2O2 producibility. Herein, we develop a two-step approach to prepare PdSn nanowire catalysts, which comprises Pd oxide layered on PdSn nanowires (PdL/PdSn-NW). The PdL/PdSn-NW displays superior reactivity in the DHS at zero Celcius, presenting the H2O2 producibility of 528 mol kgcat−1·h−1 and H2O2 selectivity of >95%. A layer of Pd oxide on the PdSn nanowire generates bi-coordinated Pd, leading to the different adsorption behaviors of O2, H2 and H2O2 on the PdL/PdSn-NW. Furthermore, the weak adsorption of H2O2 on the PdL/PdSn-NW contributes to the low activation energy and high H2O2 producibility. This surface engineering approach, depositing metal layer on metal nanowires, provides a new insight in the rational designing of efficient catalyst for DHS.
- Published
- 2022
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3. Reversible nano-structuring of SrCrO3-δ through oxidation and reduction at low temperature
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Yingge Du, Kelvin H. L. Zhang, Mark E. Bowden, Scott A. Chambers, Peter V. Sushko, and Robert J. Colby
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Multidisciplinary ,Materials science ,Nanostructure ,Diffusion ,Oxide ,General Physics and Astronomy ,chemistry.chemical_element ,Nanotechnology ,General Chemistry ,Epitaxy ,Crystallographic defect ,Oxygen ,General Biochemistry, Genetics and Molecular Biology ,Metal ,chemistry.chemical_compound ,chemistry ,Chemical physics ,visual_art ,visual_art.visual_art_medium ,Perovskite (structure) - Abstract
Oxygen vacancies are often present in complex oxides as point defects, and their effect on the electronic properties is typically uniform and isotropic. Exploiting oxygen deficiency in order to generate controllably novel structures and functional properties remains a challenging goal. Here we show that epitaxial strontium chromite films can be transformed, reversibly and at low temperature, from rhombohedral, semiconducting SrCrO(2.8) to cubic, metallic perovskite SrCrO(3-δ). Oxygen vacancies in SrCrO(2.8) aggregate and give rise to ordered arrays of {111}-oriented SrO(2) planes interleaved between layers of tetrahedrally coordinated Cr(4+) and separated by ~1 nm. First-principle calculations provide insight into the origin of the stability of such nanostructures and, consistent with the experimental data, predict that the barrier for O(2-) diffusion along these quasi-two-dimensional nanostructures is significantly lower than that in cubic SrCrO(3-δ). This property is of considerable relevance to solid oxide fuel cells in which fast O(2-) diffusion reduces the required operating temperature.
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- 2014
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4. Dynamic restructuring of nickel sulfides for electrocatalytic hydrogen evolution reaction
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Xingyu Ding, Da Liu, Pengju Zhao, Xing Chen, Hongxia Wang, Freddy E. Oropeza, Giulio Gorni, Mariam Barawi, Miguel García-Tecedor, Víctor A. de la Peña O’Shea, Jan P. Hofmann, Jianfeng Li, Jongkyoung Kim, Seungho Cho, Renbing Wu, and Kelvin H. L. Zhang
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Science - Abstract
Abstract Transition metal chalcogenides have been identified as low-cost and efficient electrocatalysts to promote the hydrogen evolution reaction in alkaline media. However, the identification of active sites and the underlying catalytic mechanism remain elusive. In this work, we employ operando X-ray absorption spectroscopy and near-ambient pressure X-ray photoelectron spectroscopy to elucidate that NiS undergoes an in-situ phase transition to an intimately mixed phase of Ni3S2 and NiO, generating highly active synergistic dual sites at the Ni3S2/NiO interface. The interfacial Ni is the active site for water dissociation and OH* adsorption while the interfacial S acts as the active site for H* adsorption and H2 evolution. Accordingly, the in-situ formation of Ni3S2/NiO interfaces enables NiS electrocatalysts to achieve an overpotential of only 95 ± 8 mV at a current density of 10 mA cm−2. Our work highlighted that the chemistry of transition metal chalcogenides is highly dynamic, and a careful control of the working conditions may lead to the in-situ formation of catalytic species that boost their catalytic performance.
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- 2024
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5. Generating active metal/oxide reverse interfaces through coordinated migration of single atoms
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Lina Zhang, Shaolong Wan, Congcong Du, Qiang Wan, Hien Pham, Jiafei Zhao, Xingyu Ding, Diye Wei, Wei Zhao, Jiwei Li, Yanping Zheng, Hui Xie, Hua Zhang, Mingshu Chen, Kelvin H. L. Zhang, Shuai Wang, Jingdong Lin, Jianyu Huang, Sen Lin, Yong Wang, Abhaya K. Datye, Ye Wang, and Haifeng Xiong
- Subjects
Science - Abstract
Abstract Identification of active sites in catalytic materials is important and helps establish approaches to the precise design of catalysts for achieving high reactivity. Generally, active sites of conventional heterogeneous catalysts can be single atom, nanoparticle or a metal/oxide interface. Herein, we report that metal/oxide reverse interfaces can also be active sites which are created from the coordinated migration of metal and oxide atoms. As an example, a Pd1/CeO2 single-atom catalyst prepared via atom trapping, which is otherwise inactive at 30 °C, is able to completely oxidize formaldehyde after steam treatment. The enhanced reactivity is due to the formation of a Ce2O3-Pd nanoparticle domain interface, which is generated by the migration of both Ce and Pd atoms on the atom-trapped Pd1/CeO2 catalyst during steam treatment. We show that the generation of metal oxide-metal interfaces can be achieved in other heterogeneous catalysts due to the coordinated mobility of metal and oxide atoms, demonstrating the formation of a new active interface when using metal single-atom material as catalyst precursor.
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- 2024
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6. Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
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Hailong Zhang, Peijie Han, Danfeng Wu, Congcong Du, Jiafei Zhao, Kelvin H. L. Zhang, Jingdong Lin, Shaolong Wan, Jianyu Huang, Shuai Wang, Haifeng Xiong, and Yong Wang
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Science - Abstract
Abstract The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu−1 h−1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement.
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- 2023
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7. Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
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Dong Li, Hongguang Wang, Kaifeng Li, Bonan Zhu, Kai Jiang, Dirk Backes, Larissa S. I. Veiga, Jueli Shi, Pinku Roy, Ming Xiao, Aiping Chen, Quanxi Jia, Tien-Lin Lee, Sarnjeet S. Dhesi, David O. Scanlon, Judith L. MacManus-Driscoll, Peter A. van Aken, Kelvin H. L. Zhang, and Weiwei Li
- Subjects
Science - Abstract
Abstract Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO6 octahedral rotations throughout LaCoO3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO3 films while suggesting potential applications toward low-power spintronic devices.
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- 2023
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