淡江大學機構典藏:Item 987654321/124073
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    题名: 5f covalency synergistically boosting oxygen evolution of UCoO4 catalyst
    作者: X. Lin;Y. C. Huang;Z. Hu;L. Li;J. Zhou;Q. Zhao;H. Huang;J. Sun;C. W. Pao;Y. C. Chang;H. J. Lin;C. T. Chen;C. L Dong;J. Q. Wang;L. Zhang
    日期: 2021-12-08
    上传时间: 2023-05-12 12:08:34 (UTC+8)
    出版者: American Chemical Society
    摘要: Electronic structure modulation among multiple metal sites is key to the design of efficient catalysts. Most studies have focused on regulating 3d transition-metal active ions through other d-block metals, while few have utilized f-block metals. Herein, we report a new class of catalyst, namely, UCoO4 with alternative CoO6 and 5f-related UO6 octahedra, as a unique example of a 5f-covalent compound that exhibits enhanced electrocatalytic oxygen evolution reaction (OER) activity because of the presence of the U 5f–O 2p–Co 3d network. UCoO4 exhibits a low overpotential of 250 mV at 10 mA cm–2, surpassing other unitary cobalt-based catalysts ever reported. X-ray absorption spectroscopy revealed that the Co2+ ion in pristine UCoO4 was converted to high-valence Co3+/4+, while U6+ remained unchanged during the OER, indicating that only Co was the active site. Density functional theory calculations demonstrated that the OER activity of Co3+/4+ was synergistically enhanced by the covalent bonding of U6+-5f in the U 5f–O 2p–Co 3d network. This study opens new avenues for the realization of electronic structure manipulation via unique 5f involvement.
    關聯: Journal of the American Chemical Society 144(1), p.416-423
    DOI: 10.1021/jacs.1c10311
    显示于类别:[電機工程學系暨研究所] 期刊論文

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