5f covalency synergistically boosting oxygen evolution of UCoO4 catalyst
學年 110
學期 1
出版(發表)日期 2022-01-03
作品名稱 5f covalency synergistically boosting oxygen evolution of UCoO4 catalyst
著者 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
著錄名稱、卷期、頁數 Journal of the American Chemical Society 144(1), p.416-423
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.
語言 en_US
ISSN 0002-7863;1520-5126
期刊性質 國外
收錄於 SCI
國別 USA
出版型式 ,電子版

機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/124073 )