期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-14848-2
关键词
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资金
- China Ministry of Science and Technology [2017YFA0208300, 2017YFA0402800]
- National Natural Science Foundation of China [21471143, 21533007, 11621063]
- Fundamental Research Funds for the Central Universities [KY2310000020, WK2340000076, WK2060030029]
- Youth Innovation Promotion Association CAS [CX2310000091]
Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt-support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H2SO4 and 46 mV in 1.0 M NaOH at 10 mA cm(-2), and long-term durability in wide-pH electrolytes.
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