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通过与钴铁层状双氢氧化物的电子耦合促进单原子钌的析氧反应

Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides.

作者信息

Li Pengsong, Wang Maoyu, Duan Xinxuan, Zheng Lirong, Cheng Xiaopeng, Zhang Yuefei, Kuang Yun, Li Yaping, Ma Qing, Feng Zhenxing, Liu Wen, Sun Xiaoming

机构信息

State Key Laboratory of Chemical Resource Engineering, College of Energy, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

Department of Chemistry and Energy Sciences Institute, Yale University, West Haven, CT, 06516, USA.

出版信息

Nat Commun. 2019 Apr 12;10(1):1711. doi: 10.1038/s41467-019-09666-0.

Abstract

Single atom catalyst, which contains isolated metal atoms singly dispersed on supports, has great potential for achieving high activity and selectivity in hetero-catalysis and electrocatalysis. However, the activity and stability of single atoms and their interaction with support still remains a mystery. Here we show a stable single atomic ruthenium catalyst anchoring on the surface of cobalt iron layered double hydroxides, which possesses a strong electronic coupling between ruthenium and layered double hydroxides. With 0.45 wt.% ruthenium loading, the catalyst exhibits outstanding activity with overpotential 198 mV at the current density of 10 mA cm and a small Tafel slope of 39 mV dec for oxygen evolution reaction. By using operando X-ray absorption spectroscopy, it is disclosed that the isolated single atom ruthenium was kept under the oxidation states of 4+ even at high overpotential due to synergetic electron coupling, which endow exceptional electrocatalytic activity and stability simultaneously.

摘要

单原子催化剂包含孤立的金属原子,这些原子单独分散在载体上,在多相催化和电催化中实现高活性和选择性方面具有巨大潜力。然而,单原子的活性和稳定性及其与载体的相互作用仍是一个谜。在此,我们展示了一种稳定的单原子钌催化剂,它锚定在钴铁层状双氢氧化物表面,钌与层状双氢氧化物之间存在强电子耦合。在钌负载量为0.45 wt.%时,该催化剂在析氧反应中表现出优异的活性,在电流密度为10 mA cm时过电位为198 mV,塔菲尔斜率为39 mV dec。通过使用原位X射线吸收光谱,揭示出即使在高过电位下,由于协同电子耦合,孤立的单原子钌仍保持在4+的氧化态,这同时赋予了其优异的电催化活性和稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9441/6461613/220ceaaf18e5/41467_2019_9666_Fig1_HTML.jpg

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