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Continuous transition from double-layer to Faradaic charge storage in confined electrolytes

Author

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  • Simon Fleischmann

    (North Carolina State University
    Université Paul Sabatier, CIRIMAT UMR CNRS 5085
    Helmholtz Institute Ulm (HIU)
    Karlsruhe Institute of Technology (KIT))

  • Yuan Zhang

    (INM—Leibniz Institute for New Materials
    Saarland University)

  • Xuepeng Wang

    (University of California)

  • Peter T. Cummings

    (Vanderbilt University)

  • Jianzhong Wu

    (University of California)

  • Patrice Simon

    (Université Paul Sabatier, CIRIMAT UMR CNRS 5085
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E))

  • Yury Gogotsi

    (Université Paul Sabatier, CIRIMAT UMR CNRS 5085
    Drexel University)

  • Volker Presser

    (INM—Leibniz Institute for New Materials
    Saarland University
    Saarene—Saarland Center for Energy Materials and Sustainability)

  • Veronica Augustyn

    (North Carolina State University)

Abstract

The capacitance of the electrochemical interface has traditionally been separated into two distinct types: non-Faradaic electric double-layer capacitance, which involves charge induction, and Faradaic pseudocapacitance, which involves charge transfer. However, the electrochemical interface in most energy technologies is not planar but involves porous and layered materials that offer varying degrees of electrolyte confinement. We suggest that understanding electrosorption under confinement in porous and layered materials requires a more nuanced view of the capacitive mechanism than that at a planar interface. In particular, we consider the crucial role of the electrolyte confinement in these systems to reconcile different viewpoints on electrochemical capacitance. We propose that there is a continuum between double-layer capacitance and Faradaic intercalation that is dependent on the specific confinement microenvironment. We also discuss open questions regarding electrochemical capacitance in porous and layered materials and how these lead to opportunities for future energy technologies.

Suggested Citation

  • Simon Fleischmann & Yuan Zhang & Xuepeng Wang & Peter T. Cummings & Jianzhong Wu & Patrice Simon & Yury Gogotsi & Volker Presser & Veronica Augustyn, 2022. "Continuous transition from double-layer to Faradaic charge storage in confined electrolytes," Nature Energy, Nature, vol. 7(3), pages 222-228, March.
  • Handle: RePEc:nat:natene:v:7:y:2022:i:3:d:10.1038_s41560-022-00993-z
    DOI: 10.1038/s41560-022-00993-z
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    Cited by:

    1. Chenxuan Xu & Jingdong Zhu & Dedi Li & Xu Qian & Gang Chen & Huachao Yang, 2022. "Unveiling the Effects of Solvent Polarity within Graphene Based Electric Double-Layer Capacitors," Energies, MDPI, vol. 15(24), pages 1-13, December.
    2. Kangkang Ge & Hui Shao & Encarnacion Raymundo-Piñero & Pierre-Louis Taberna & Patrice Simon, 2024. "Cation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Siraprapha Deebansok & Jie Deng & Etienne Calvez & Yachao Zhu & Olivier Crosnier & Thierry Brousse & Olivier Fontaine, 2024. "Capacitive tendency concept alongside supervised machine-learning toward classifying electrochemical behavior of battery and pseudocapacitor materials," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    4. Qiulong Wei & Xiaoqing Chang & Danielle Butts & Ryan DeBlock & Kun Lan & Junbin Li & Dongliang Chao & Dong-Liang Peng & Bruce Dunn, 2023. "Surface-redox sodium-ion storage in anatase titanium oxide," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    5. Mailis Lounasvuori & Yangyunli Sun & Tyler S. Mathis & Ljiljana Puskar & Ulrich Schade & De-En Jiang & Yury Gogotsi & Tristan Petit, 2023. "Vibrational signature of hydrated protons confined in MXene interlayers," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Tao Wang & Runtong Pan & Murillo L. Martins & Jinlei Cui & Zhennan Huang & Bishnu P. Thapaliya & Chi-Linh Do-Thanh & Musen Zhou & Juntian Fan & Zhenzhen Yang & Miaofang Chi & Takeshi Kobayashi & Jianz, 2023. "Machine-learning-assisted material discovery of oxygen-rich highly porous carbon active materials for aqueous supercapacitors," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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