Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction

Shi Fang, Xiaorong Zhu, Xiaokang Liu, Jian Gu, Wei Liu, Danhao Wang, Wei Zhang, Yue Lin, Junling Lu, Shiqiang Wei, Yafei Li and Tao Yao ()
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Shi Fang: University of Science and Technology of China
Xiaorong Zhu: Nanjing Normal University
Xiaokang Liu: University of Science and Technology of China
Jian Gu: University of Science and Technology of China
Wei Liu: University of Science and Technology of China
Danhao Wang: University of Science and Technology of China
Wei Zhang: University of Science and Technology of China
Yue Lin: University of Science and Technology of China
Junling Lu: University of Science and Technology of China
Shiqiang Wei: University of Science and Technology of China
Yafei Li: Nanjing Normal University
Tao Yao: University of Science and Technology of China

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract 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.

Date: 2020
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DOI: 10.1038/s41467-020-14848-2

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