Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

Yuhai Dou, Chun-Ting He, Lei Zhang, Huajie Yin, Mohammad Al-Mamun, Jianmin Ma and Huijun Zhao ()
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Yuhai Dou: Griffith University
Chun-Ting He: Jiangxi Normal University
Lei Zhang: Griffith University
Huajie Yin: Griffith University
Mohammad Al-Mamun: Griffith University
Jianmin Ma: Hunan University
Huijun Zhao: Griffith University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe2-DFe–VCo exhibits much higher catalytic activity than other defect-activated CoSe2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co2 site that is adjacent to the VCo-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔEOH) without changing ΔEO, and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.

Date: 2020
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DOI: 10.1038/s41467-020-15498-0

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