期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 17, 页码 7883-7888出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c01135
关键词
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资金
- Swiss Office of Energy (BFE) [SI/501598-01]
- ETH Career Seed Grant [SEED-15 19-2]
Ruthenium pyrochlores, that is, oxides of composition A(2)Ru(2)O(7-delta), have emerged recently as state-of-the-art catalysts for the oxygen evolution reaction (OER) in acidic conditions. Here, we demonstrate that the A-site substituent in yttrium ruthenium pyrochlores Y1.8M0.2Ru2O7-delta (M = Cu, Co, Ni, Fe, Y) controls the concentration of surface oxygen vacancies (V-O) in these materials whereby an increased concentration of V-O sites correlates with a superior OER activity. DFT calculations rationalize these experimental trends demonstrating that the higher OER activity and V-O surface density originate from a weakened strength of the M-O bond, scaling with the formation enthalpy of the respective MOx phases and the coupling between the M d states and O 2p states. Our work introduces a novel catalyst with improved OER performance, Y1.8M0.2Ru2O7-delta, and provides general guidelines for the design of active electrocatalysts.
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