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In situ NMR metrology reveals reaction mechanisms in redox flow batteries

Author

Listed:
  • Evan Wenbo Zhao

    (University of Cambridge)

  • Tao Liu

    (University of Cambridge
    Tongji University)

  • Erlendur Jónsson

    (University of Cambridge
    Chalmers University of Technology)

  • Jeongjae Lee

    (University of Cambridge
    Seoul National University)

  • Israel Temprano

    (University of Cambridge)

  • Rajesh B. Jethwa

    (University of Cambridge)

  • Anqi Wang

    (Imperial College London)

  • Holly Smith

    (University of Cambridge)

  • Javier Carretero-González

    (Institute of Polymer Science and Technology, ICTP-CSIC)

  • Qilei Song

    (Imperial College London)

  • Clare P. Grey

    (University of Cambridge)

Abstract

Large-scale energy storage is becoming increasingly critical to balancing renewable energy production and consumption1. Organic redox flow batteries, made from inexpensive and sustainable redox-active materials, are promising storage technologies that are cheaper and less environmentally hazardous than vanadium-based batteries, but they have shorter lifetimes and lower energy density2,3. Thus, fundamental insight at the molecular level is required to improve performance4,5. Here we report two in situ nuclear magnetic resonance (NMR) methods of studying redox flow batteries, which are applied to two redox-active electrolytes: 2,6-dihydroxyanthraquinone (DHAQ) and 4,4′-((9,10-anthraquinone-2,6-diyl)dioxy) dibutyrate (DBEAQ). In the first method, we monitor the changes in the 1H NMR shift of the liquid electrolyte as it flows out of the electrochemical cell. In the second method, we observe the changes that occur simultaneously in the positive and negative electrodes in the full electrochemical cell. Using the bulk magnetization changes (observed via the 1H NMR shift of the water resonance) and the line broadening of the 1H shifts of the quinone resonances as a function of the state of charge, we measure the potential differences of the two single-electron couples, identify and quantify the rate of electron transfer between the reduced and oxidized species, and determine the extent of electron delocalization of the unpaired spins over the radical anions. These NMR techniques enable electrolyte decomposition and battery self-discharge to be explored in real time, and show that DHAQ is decomposed electrochemically via a reaction that can be minimized by limiting the voltage used on charging. We foresee applications of these NMR methods in understanding a wide range of redox processes in flow and other electrochemical systems.

Suggested Citation

  • Evan Wenbo Zhao & Tao Liu & Erlendur Jónsson & Jeongjae Lee & Israel Temprano & Rajesh B. Jethwa & Anqi Wang & Holly Smith & Javier Carretero-González & Qilei Song & Clare P. Grey, 2020. "In situ NMR metrology reveals reaction mechanisms in redox flow batteries," Nature, Nature, vol. 579(7798), pages 224-228, March.
  • Handle: RePEc:nat:nature:v:579:y:2020:i:7798:d:10.1038_s41586-020-2081-7
    DOI: 10.1038/s41586-020-2081-7
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    Citations

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    Cited by:

    1. Dominic Hey & Rajesh B. Jethwa & Nadia L. Farag & Bernardine L. D. Rinkel & Evan Wenbo Zhao & Clare P. Grey, 2023. "Identifying and preventing degradation in flavin mononucleotide-based redox flow batteries via NMR and EPR spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Chunchun Ye & Anqi Wang & Charlotte Breakwell & Rui Tan & C. Grazia Bezzu & Elwin Hunter-Sellars & Daryl R. Williams & Nigel P. Brandon & Peter A. A. Klusener & Anthony R. Kucernak & Kim E. Jelfs & Ne, 2022. "Development of efficient aqueous organic redox flow batteries using ion-sieving sulfonated polymer membranes," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    3. Rémy Richard Jacquemond & Maxime van der Heijden & Emre Burak Boz & Eric Ricardo Carreón Ruiz & Katharine Virginia Greco & Jeffrey Adam Kowalski & Vanesa Muñoz Perales & Fikile Richard Brushett & Kitt, 2024. "Quantifying concentration distributions in redox flow batteries with neutron radiography," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    4. Sanat Vibhas Modak & Wanggang Shen & Siddhant Singh & Dylan Herrera & Fairooz Oudeif & Bryan R. Goldsmith & Xun Huan & David G. Kwabi, 2023. "Understanding capacity fade in organic redox-flow batteries by combining spectroscopy with statistical inference techniques," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    5. Li Jin & Xiaoyuan Zhou & Fang Wang & Xiang Ning & Yujie Wen & Benteng Song & Changju Yang & Di Wu & Xiaokang Ke & Luming Peng, 2022. "Insights into memory effect mechanisms of layered double hydroxides with solid-state NMR spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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