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On the importance of the electric double layer structure in aqueous electrocatalysis

Author

Listed:
  • Seung-Jae Shin

    (Korea Advanced Institute of Science and Technology)

  • Dong Hyun Kim

    (Gwangju Institute of Science and Technology)

  • Geunsu Bae

    (Gwangju Institute of Science and Technology)

  • Stefan Ringe

    (Daegu Gyeongbuk Institute of Science and Technology
    Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Hansol Choi

    (Gwangju Institute of Science and Technology)

  • Hyung-Kyu Lim

    (Kangwon National University)

  • Chang Hyuck Choi

    (Gwangju Institute of Science and Technology)

  • Hyungjun Kim

    (Korea Advanced Institute of Science and Technology)

Abstract

To design electrochemical interfaces for efficient electric-chemical energy interconversion, it is critical to reveal the electric double layer (EDL) structure and relate it with electrochemical activity; nonetheless, this has been a long-standing challenge. Of particular, no molecular-level theories have fully explained the characteristic two peaks arising in the potential-dependence of the EDL capacitance, which is sensitively dependent on the EDL structure. We herein demonstrate that our first-principles-based molecular simulation reproduces the experimental capacitance peaks. The origin of two peaks emerging at anodic and cathodic potentials is unveiled to be an electrosorption of ions and a structural phase transition, respectively. We further find a cation complexation gradually modifies the EDL structure and the field strength, which linearly scales the carbon dioxide reduction activity. This study deciphers the complex structural response of the EDL and highlights its catalytic importance, which bridges the mechanistic gap between the EDL structure and electrocatalysis.

Suggested Citation

  • Seung-Jae Shin & Dong Hyun Kim & Geunsu Bae & Stefan Ringe & Hansol Choi & Hyung-Kyu Lim & Chang Hyuck Choi & Hyungjun Kim, 2022. "On the importance of the electric double layer structure in aqueous electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-021-27909-x
    DOI: 10.1038/s41467-021-27909-x
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    Cited by:

    1. Chengcheng Zhu & Li Xu & Yazi Liu & Jiang Liu & Jin Wang & Hanjun Sun & Ya-Qian Lan & Chen Wang, 2024. "Polyoxometalate-based plasmonic electron sponge membrane for nanofluidic osmotic energy conversion," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Zesong Ma & Zhilong Yang & Wenchuan Lai & Qiyou Wang & Yan Qiao & Haolan Tao & Cheng Lian & Min Liu & Chao Ma & Anlian Pan & Hongwen Huang, 2022. "CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. 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.

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