Spin-polarized oxygen evolution reaction under magnetic field

Xiao Ren, Tianze Wu, Yuanmiao Sun, Yan Li, Guoyu Xian, Xianhu Liu, Chengmin Shen, Jose Gracia, Hong-Jun Gao, Haitao Yang () and Zhichuan J. Xu ()
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Xiao Ren: Chinese Academy of Science
Tianze Wu: Chinese Academy of Science
Yuanmiao Sun: Nanyang Technological University
Yan Li: Chinese Academy of Science
Guoyu Xian: Chinese Academy of Science
Xianhu Liu: Key Laboratory of Advanced Material Processing & Mold (Zhengzhou University), Ministry of Education
Chengmin Shen: Chinese Academy of Science
Jose Gracia: MagnetoCat SL
Hong-Jun Gao: Chinese Academy of Science
Haitao Yang: Chinese Academy of Science
Zhichuan J. Xu: Nanyang Technological University

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: Abstract The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O2 from singlet state species (OH- or H2O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. Here, we report that by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under a constant magnetic field, the OER can be enhanced. However, it does not applicable to non-ferromagnetic catalysts. We found that the spin polarization occurs at the first electron transfer step in OER, where coherent spin exchange happens between the ferromagnetic catalyst and the adsorbed oxygen species with fast kinetics, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O2. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.

Date: 2021
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DOI: 10.1038/s41467-021-22865-y

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