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

Author

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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)

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.

Suggested Citation

  • Ganceng Yang & Yanqing Jiao & Haijing Yan & Ying Xie & Chungui Tian & Aiping Wu & Yu Wang & Honggang Fu, 2022. "Unraveling the mechanism for paired electrocatalysis of organics with water as a feedstock," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30495-1
    DOI: 10.1038/s41467-022-30495-1
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    References listed on IDEAS

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    1. Ming Yang & Yimin Jiang & Chung-Li Dong & Leitao Xu & Yutong Huang & Shifan Leng & Yandong Wu & Yongxiang Luo & Wei Chen & Ta Thi Thuy Nga & Shuangyin Wang & Yuqin Zou, 2024. "A self-reactivated PdCu catalyst for aldehyde electro-oxidation with anodic hydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Ke Liu & Mengna Lei & Xin Li & Xuemei Zhang & Ying Zhang & Weigang Fan & Man-Bo Li & Sheng Zhang, 2024. "Paired electrocatalysis unlocks cross-dehydrogenative coupling of C(sp3)-H bonds using a pentacoordinated cobalt-salen catalyst," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Lin Chen & Chang Yu & Xuedan Song & Junting Dong & Jiawei Mu & Jieshan Qiu, 2024. "Integrated electrochemical and chemical system for ampere-level production of terephthalic acid alternatives and hydrogen," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Qiqi Mao & Xu Mu & Wenxin Wang & Kai Deng & Hongjie Yu & Ziqiang Wang & You Xu & Liang Wang & Hongjing Wang, 2023. "Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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