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Charge transfer kinetics at the solid–solid interface in porous electrodes

Author

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  • Peng Bai

    (Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA)

  • Martin Z. Bazant

    (Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
    Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA)

Abstract

Interfacial charge transfer is widely assumed to obey the Butler–Volmer kinetics. For certain liquid–solid interfaces, the Marcus–Hush–Chidsey theory is more accurate and predictive, but it has not been applied to porous electrodes. Here we report a simple method to extract the charge transfer rates in carbon-coated LiFePO4 porous electrodes from chronoamperometry experiments, obtaining curved Tafel plots that contradict the Butler–Volmer equation but fit the Marcus–Hush–Chidsey prediction over a range of temperatures. The fitted reorganization energy matches the Born solvation energy for electron transfer from carbon to the iron redox site. The kinetics are thus limited by electron transfer at the solid–solid (carbon-LixFePO4) interface rather than by ion transfer at the liquid–solid interface, as previously assumed. The proposed experimental method generalizes Chidsey’s method for phase-transforming particles and porous electrodes, and the results show the need to incorporate Marcus kinetics in modelling batteries and other electrochemical systems.

Suggested Citation

  • Peng Bai & Martin Z. Bazant, 2014. "Charge transfer kinetics at the solid–solid interface in porous electrodes," Nature Communications, Nature, vol. 5(1), pages 1-7, May.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms4585
    DOI: 10.1038/ncomms4585
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    1. Gangbin Yan & Jialiang Wei & Emory Apodaca & Suin Choi & Peter J. Eng & Joanne E. Stubbs & Yu Han & Siqi Zou & Mrinal K. Bera & Ronghui Wu & Evguenia Karapetrova & Hua Zhou & Wei Chen & Chong Liu, 2024. "Identifying critical features of iron phosphate particle for lithium preference," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Kotub Uddin & Alessandro Picarelli & Christopher Lyness & Nigel Taylor & James Marco, 2014. "An Acausal Li-Ion Battery Pack Model for Automotive Applications," Energies, MDPI, vol. 7(9), pages 1-26, August.
    3. Igor Iwakiri & Tiago Antunes & Helena Almeida & João P. Sousa & Rita Bacelar Figueira & Adélio Mendes, 2021. "Redox Flow Batteries: Materials, Design and Prospects," Energies, MDPI, vol. 14(18), pages 1-45, September.

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