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Direct observation of ion dynamics in supercapacitor electrodes using in situ diffusion NMR spectroscopy

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  • Alexander C. Forse

    (University of Cambridge
    † Present addresses: Department of Chemistry, Department of Chemical and Biomolecular Engineering, and Berkeley Energy and Climate Institute, University of California, Berkeley 94720, USA (A.C.F.); Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK (J.M.G.).)

  • John M. Griffin

    (University of Cambridge
    † Present addresses: Department of Chemistry, Department of Chemical and Biomolecular Engineering, and Berkeley Energy and Climate Institute, University of California, Berkeley 94720, USA (A.C.F.); Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK (J.M.G.).)

  • Céline Merlet

    (University of Cambridge)

  • Javier Carretero-Gonzalez

    (University of Cambridge)

  • Abdul-Rahman O. Raji

    (University of Cambridge
    Cambridge Graphene Centre, University of Cambridge)

  • Nicole M. Trease

    (University of Cambridge)

  • Clare P. Grey

    (University of Cambridge)

Abstract

Ionic transport inside porous carbon electrodes underpins the storage of energy in supercapacitors and the rate at which they can charge and discharge, yet few studies have elucidated the materials properties that influence ion dynamics. Here we use in situ pulsed field gradient NMR spectroscopy to measure ionic diffusion in supercapacitors directly. We find that confinement in the nanoporous electrode structures decreases the effective self-diffusion coefficients of ions by over two orders of magnitude compared with neat electrolyte, and in-pore diffusion is modulated by changes in ion populations at the electrode/electrolyte interface during charging. Electrolyte concentration and carbon pore size distributions also affect in-pore diffusion and the movement of ions in and out of the nanopores. In light of our findings we propose that controlling the charging mechanism may allow the tuning of the energy and power performances of supercapacitors for a range of different applications.

Suggested Citation

  • Alexander C. Forse & John M. Griffin & Céline Merlet & Javier Carretero-Gonzalez & Abdul-Rahman O. Raji & Nicole M. Trease & Clare P. Grey, 2017. "Direct observation of ion dynamics in supercapacitor electrodes using in situ diffusion NMR spectroscopy," Nature Energy, Nature, vol. 2(3), pages 1-7, March.
    • Handle: RePEc:nat:natene:v:2:y:2017:i:3:d:10.1038_nenergy.2016.216
    DOI: 10.1038/nenergy.2016.216
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    Cited by:

    1. Pal, Bhupender & Yasin, Amina & Kaur, Rupinder & Tebyetekerwa, Mike & Zabihi, Fatemeh & Yang, Shengyuan & Yang, Chun-Chen & Sofer, Zděnek & Jose, Rajan, 2021. "Understanding electrochemical capacitors with in-situ techniques," Renewable and Sustainable Energy Reviews, Elsevier, vol. 149(C).
    2. Kunwar, Ria & Pal, Bhupender & Izwan Misnon, Izan & Daniyal, Hamdan & Zabihi, Fatemeh & Yang, Shengyuan & Sofer, Zděnek & Yang, Chun-Chen & Jose, Rajan, 2023. "Characterization of electrochemical double layer capacitor electrode using self-discharge measurements and modeling," Applied Energy, Elsevier, vol. 334(C).
    3. Choudhary, Ram Bilash & Ansari, Sarfaraz & Majumder, Mandira, 2021. "Recent advances on redox active composites of metal-organic framework and conducting polymers as pseudocapacitor electrode material," Renewable and Sustainable Energy Reviews, Elsevier, vol. 145(C).
    4. Xiao-Ting Yin & En-Ming You & Ru-Yu Zhou & Li-Hong Zhu & Wei-Wei Wang & Kai-Xuan Li & De-Yin Wu & Yu Gu & Jian-Feng Li & Bing-Wei Mao & Jia-Wei Yan, 2024. "Unraveling the energy storage mechanism in graphene-based nonaqueous electrochemical capacitors by gap-enhanced Raman spectroscopy," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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