Unraveling the mechanism for paired electrocatalysis of organics with water as a feedstock

Ganceng Yang, Yanqing Jiao, Haijing Yan (), Ying Xie, Chungui Tian, Aiping Wu, Yu Wang and Honggang Fu ()
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Ganceng Yang: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Yanqing Jiao: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Haijing Yan: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Ying Xie: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Chungui Tian: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Aiping Wu: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Yu Wang: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University
Honggang Fu: Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China, Heilongjiang University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Paired electroreduction and electrooxidation of organics with water as a feedstock to produce value-added chemicals is meaningful. A comprehensive understanding of reaction mechanism is critical for the catalyst design and relative area development. Here, we have systematically studied the mechanism of the paired electroreduction and electrooxidation of organics on Fe-Mo-based phosphide heterojunctions. It is shown that active H* species for organic electroreduction originate from water. As for organic electrooxidation, among various oxygen species (OH*, OOH*, and O*), OH* free radicals derived from the first step of water dissociation are identified as active species. Furthermore, explicit reaction pathways and their paired advantages are proposed based on theoretical calculations. The paired electrolyzer powered by a solar cell shows a low voltage of 1.594 V at 100 mA cm−2, faradaic efficiency of ≥99%, and remarkable cycle stability. This work provides a guide for sustainable synthesis of various value-added chemicals via paired electrocatalysis.

Date: 2022
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DOI: 10.1038/s41467-022-30495-1

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