Diffusion-free Grotthuss topochemistry for high-rate and long-life proton batteries

Xianyong Wu; Jessica J. Hong; Woochul Shin; Lu Ma; Tongchao Liu; Xuanxuan Bi; Yifei Yuan; Yitong Qi; T. Wesley Surta; Wenxi Huang; Joerg Neuefeind; Tianpin Wu; P. Alex Greaney; Jun Lu; Xiulei Ji

doi:10.1038/s41560-018-0309-7

Diffusion-free Grotthuss topochemistry for high-rate and long-life proton batteries

Xianyong Wu, Jessica J. Hong, Woochul Shin, Lu Ma, Tongchao Liu, Xuanxuan Bi, Yifei Yuan, Yitong Qi, T. Wesley Surta, Wenxi Huang, Joerg Neuefeind, Tianpin Wu, P. Alex Greaney, Jun Lu, Xiulei Ji

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469 Scopus citations

Abstract

The design of Faradaic battery electrodes that exhibit high rate capability and long cycle life equivalent to those of the electrodes of electrical double-layer capacitors is a big challenge. Here we report a strategy to fill this performance gap using the concept of Grotthuss proton conduction, in which proton transfer takes place by means of concerted cleavage and formation of O–H bonds in a hydrogen-bonding network. We show that in a hydrated Prussian blue analogue (Turnbull’s blue) the abundant lattice water molecules with a contiguous hydrogen-bonding network facilitate Grotthuss proton conduction during redox reactions. When using it as a battery electrode, we find high-rate behaviours at 4,000 C (380 A g ⁻¹ , 508 mA cm ⁻² ), and a long cycling life of 0.73 million cycles. These results for diffusion-free Grotthuss topochemistry of protons, in contrast to orthodox battery electrochemistry, which requires ion diffusion inside electrodes, indicate a potential direction to revolutionize electrochemical energy storage for high-power applications.

Original language	English
Pages (from-to)	123-130
Number of pages	8
Journal	Nature Energy
Volume	4
Issue number	2
DOIs	https://doi.org/10.1038/s41560-018-0309-7
State	Published - Feb 1 2019

Funding

This work was supported by the US National Science Foundation, Award Number 1551693. J.L. gratefully acknowledges support from the US DOE, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. Argonne National Laboratory is operated for DOE Office of Science by UChicago Argonne, LLC, under contract DE-AC02-06CH11357. This research used resources of the APS (9-BM and 11-ID-D), a US DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract DE-AC02-06CH11357. The work used the XSEDE, which is supported by National Science Foundation grant ACI-1548562. Through XSEDE, computing was performed on Stambede2 at the Texas Advanced Computing Centre through allocation TG-DMR130046. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
DOE Office of Science
US National Science Foundation	1551693
XSEDE
National Science Foundation	ACI-1548562
U.S. Department of Energy
Office of Energy Efficiency and Renewable Energy	DE-AC02-06CH11357
Argonne National Laboratory
American Pain Society	11-ID-D

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title = "Diffusion-free Grotthuss topochemistry for high-rate and long-life proton batteries",

abstract = " The design of Faradaic battery electrodes that exhibit high rate capability and long cycle life equivalent to those of the electrodes of electrical double-layer capacitors is a big challenge. Here we report a strategy to fill this performance gap using the concept of Grotthuss proton conduction, in which proton transfer takes place by means of concerted cleavage and formation of O–H bonds in a hydrogen-bonding network. We show that in a hydrated Prussian blue analogue (Turnbull{\textquoteright}s blue) the abundant lattice water molecules with a contiguous hydrogen-bonding network facilitate Grotthuss proton conduction during redox reactions. When using it as a battery electrode, we find high-rate behaviours at 4,000 C (380 A g −1 , 508 mA cm −2 ), and a long cycling life of 0.73 million cycles. These results for diffusion-free Grotthuss topochemistry of protons, in contrast to orthodox battery electrochemistry, which requires ion diffusion inside electrodes, indicate a potential direction to revolutionize electrochemical energy storage for high-power applications.",

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AU - Qi, Yitong

AU - Surta, T. Wesley

AU - Huang, Wenxi

AU - Neuefeind, Joerg

AU - Wu, Tianpin

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AU - Lu, Jun

AU - Ji, Xiulei

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Diffusion-free Grotthuss topochemistry for high-rate and long-life proton batteries

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