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Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide

Author

Listed:
  • Wanyu Deng

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    Technical University of Denmark)

  • Peng Zhang

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University)

  • Brian Seger

    (Technical University of Denmark)

  • Jinlong Gong

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University)

Abstract

Electrochemical reduction of CO2 (CO2ER) has received significant attention due to its potential to sustainably produce valuable fuels and chemicals. However, the reaction mechanism is still not well understood. One vital debate is whether the rate-limiting step (RLS) is dominated by the availability of protons, the conversion of water molecules, or the adsorption of CO2. This paper describes insights into the RLS by investigating pH dependency and kinetic isotope effect with respect to the rate expression of CO2ER. Focusing on electrocatalysts geared towards two-electron transfer reactions, we find the generation rates of CO and formate to be invariant with either pH or deuteration of the electrolyte over Au, Ag, Sn, and In. We elucidate the RLS of two-electron transfer CO2ER to be the adsorption of CO2 onto the surface of electrocatalysts. We expect this finding to provide guidance for improving CO2ER activity through the enhancement of the CO2 adsorption processes by strategies such as surface modification of catalysts as well as careful control of pressure and interfacial electric field within reactors.

Suggested Citation

  • Wanyu Deng & Peng Zhang & Brian Seger & Jinlong Gong, 2022. "Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28436-z
    DOI: 10.1038/s41467-022-28436-z
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    Cited by:

    1. Wei Liu & Mengyang Xia & Chao Zhao & Ben Chong & Jiahe Chen & He Li & Honghui Ou & Guidong Yang, 2024. "Efficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Jiawei Li & Hongliang Zeng & Xue Dong & Yimin Ding & Sunpei Hu & Runhao Zhang & Yizhou Dai & Peixin Cui & Zhou Xiao & Donghao Zhao & Liujiang Zhou & Tingting Zheng & Jianping Xiao & Jie Zeng & Chuan X, 2023. "Selective CO2 electrolysis to CO using isolated antimony alloyed copper," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Xin Chen & Junxiang Chen & Huayu Chen & Qiqi Zhang & Jiaxuan Li & Jiwei Cui & Yanhui Sun & Defa Wang & Jinhua Ye & Lequan Liu, 2023. "Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Seung-Jae Shin & Hansol Choi & Stefan Ringe & Da Hye Won & Hyung-Suk Oh & Dong Hyun Kim & Taemin Lee & Dae-Hyun Nam & Hyungjun Kim & Chang Hyuck Choi, 2022. "A unifying mechanism for cation effect modulating C1 and C2 productions from CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    5. Stefan Ringe, 2023. "The importance of a charge transfer descriptor for screening potential CO2 reduction electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    6. Wanyu Deng & Peng Zhang & Yu Qiao & Georg Kastlunger & Nitish Govindarajan & Aoni Xu & Ib Chorkendorff & Brian Seger & Jinlong Gong, 2024. "Unraveling the rate-determining step of C2+ products during electrochemical CO reduction," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    7. Jing Xue & Xue Dong & Chunxiao Liu & Jiawei Li & Yizhou Dai & Weiqing Xue & Laihao Luo & Yuan Ji & Xiao Zhang & Xu Li & Qiu Jiang & Tingting Zheng & Jianping Xiao & Chuan Xia, 2024. "Turning copper into an efficient and stable CO evolution catalyst beyond noble metals," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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