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Radially distributed charging time constants at an electrode-solution interface

Author

Listed:
  • Ben Niu

    (Nanjing University)

  • Ruo-Chen Xie

    (Nanjing University)

  • Bin Ren

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM))

  • Yi-Tao Long

    (Nanjing University)

  • Wei Wang

    (Nanjing University)

Abstract

An electrochemically homogeneous electrode-solution interface should be understood as spatially invariant in both terms of intrinsic reactivity for the electrode side and electrical resistance mainly for the solution side. The latter remains presumably assumed in almost all cases. However, by using optical microscopy to spatially resolve the classic redox electrochemistry occurring at the whole surface of a gold macroelectrode, we discover that the electron transfer occurs always significantly sooner (by milliseconds), rather than faster in essence, at the radial coordinates closer to the electrode periphery than the very center. So is the charging process when there is no electron transfer. Based on optical measurements of the interfacial impedance, this spatially unsynchronized electron transfer is attributed to a radially non-uniform distribution of solution resistance. We accordingly manage to eliminate the heterogeneity by engineering the solution resistance distribution. The revealed spatially-dependent charging time ‘constant’ (to be questioned) would help paint our overall fundamental picture of electrode kinetics.

Suggested Citation

  • Ben Niu & Ruo-Chen Xie & Bin Ren & Yi-Tao Long & Wei Wang, 2024. "Radially distributed charging time constants at an electrode-solution interface," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50028-2
    DOI: 10.1038/s41467-024-50028-2
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    References listed on IDEAS

    as
    1. Ben Niu & Wenxuan Jiang & Bo Jiang & Mengqi Lv & Sa Wang & Wei Wang, 2022. "Determining the depth of surface charging layer of single Prussian blue nanoparticles with pseudocapacitive behaviors," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Qian Cheng & Lu Wei & Zhe Liu & Nan Ni & Zhe Sang & Bin Zhu & Weiheng Xu & Meijie Chen & Yupeng Miao & Long-Qing Chen & Wei Min & Yuan Yang, 2018. "Operando and three-dimensional visualization of anion depletion and lithium growth by stimulated Raman scattering microscopy," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
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