Pivotal role of reversible NiO6 geometric conversion in oxygen evolution

Xiaopeng Wang, Shibo Xi (), Pengru Huang, Yonghua Du, Haoyin Zhong, Qing Wang, Armando Borgna, Yong-Wei Zhang, Zhenbo Wang, Hao Wang (), Zhi Gen Yu (), Wee Siang Vincent Lee () and Junmin Xue ()
Additional contact information
Xiaopeng Wang: National University of Singapore
Shibo Xi: Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research
Pengru Huang: National University of Singapore
Yonghua Du: Brookhaven National Laboratory
Haoyin Zhong: National University of Singapore
Qing Wang: National University of Singapore
Armando Borgna: Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research
Yong-Wei Zhang: Agency for Science, Technology and Research
Zhenbo Wang: Harbin Institute of Technology, Heilongjiang Sheng
Hao Wang: National University of Singapore
Zhi Gen Yu: Agency for Science, Technology and Research
Wee Siang Vincent Lee: National University of Singapore
Junmin Xue: National University of Singapore

Nature, 2022, vol. 611, issue 7937, 702-708

Abstract: Abstract Realizing an efficient electron transfer process in the oxygen evolution reaction by modifying the electronic states around the Fermi level is crucial in developing high-performing and robust electrocatalysts1–3. Typically, electron transfer proceeds solely through either a metal redox chemistry (an adsorbate evolution mechanism (AEM), with metal bands around the Fermi level) or an oxygen redox chemistry (a lattice oxygen oxidation mechanism (LOM), with oxygen bands around the Fermi level), without the concurrent occurrence of both metal and oxygen redox chemistries in the same electron transfer pathway1–15. Here we report an electron transfer mechanism that involves a switchable metal and oxygen redox chemistry in nickel-oxyhydroxide-based materials with light as the trigger. In contrast to the traditional AEM and LOM, the proposed light-triggered coupled oxygen evolution mechanism requires the unit cell to undergo reversible geometric conversion between octahedron (NiO6) and square planar (NiO4) to achieve electronic states (around the Fermi level) with alternative metal and oxygen characters throughout the oxygen evolution process. Utilizing this electron transfer pathway can bypass the potential limiting steps, that is, oxygen–oxygen bonding in AEM and deprotonation in LOM1–5,8. As a result, the electrocatalysts that operate through this route show superior activity compared with previously reported electrocatalysts. Thus, it is expected that the proposed light-triggered coupled oxygen evolution mechanism adds a layer of understanding to the oxygen evolution research scene.

Date: 2022
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DOI: 10.1038/s41586-022-05296-7

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