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Understanding potential-dependent competition between electrocatalytic dinitrogen and proton reduction reactions

Author

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  • Changhyeok Choi

    (Korea Advanced Institute of Science and Technology (KAIST))

  • Geun Ho Gu

    (Korea Advanced Institute of Science and Technology (KAIST))

  • Juhwan Noh

    (Korea Advanced Institute of Science and Technology (KAIST))

  • Hyun S. Park

    (Korea Institute of Science and Technology (KIST))

  • Yousung Jung

    (Korea Advanced Institute of Science and Technology (KAIST))

Abstract

A key challenge to realizing practical electrochemical N2 reduction reaction (NRR) is the decrease in the NRR activity before reaching the mass-transfer limit as overpotential increases. While the hydrogen evolution reaction (HER) has been suggested to be responsible for this phenomenon, the mechanistic origin has not been clearly explained. Herein, we investigate the potential-dependent competition between NRR and HER using the constant electrode potential model and microkinetic modeling. We find that the H coverage and N2 coverage crossover leads to the premature decrease of NRR activity. The coverage crossover originates from the larger charge transfer in H+ adsorption than N2 adsorption. The larger charge transfer in H+ adsorption, which potentially leads to the coverage crossover, is a general phenomenon seen in various heterogeneous catalysts, posing a fundamental challenge to realize practical electrochemical NRR. We suggest several strategies to overcome the challenge based on the present understandings.

Suggested Citation

  • Changhyeok Choi & Geun Ho Gu & Juhwan Noh & Hyun S. Park & Yousung Jung, 2021. "Understanding potential-dependent competition between electrocatalytic dinitrogen and proton reduction reactions," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24539-1
    DOI: 10.1038/s41467-021-24539-1
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    Cited by:

    1. Jongyoun Kim & Taemin Lee & Hyun Dong Jung & Minkyoung Kim & Jungsu Eo & Byeongjae Kang & Hyeonwoo Jung & Jaehyoung Park & Daewon Bae & Yujin Lee & Sojung Park & Wooyul Kim & Seoin Back & Youngu Lee &, 2024. "Vitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. 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.

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