Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries

Jyotshna Pokharel, Arthur Cresce, Bharat Pant, Moon Young Yang, Ashim Gurung, Wei He, Abiral Baniya, Buddhi Sagar Lamsal, Zhongjiu Yang, Stephen Gent, Xiaojun Xian, Ye Cao (), William A. Goddard (), Kang Xu () and Yue Zhou ()
Additional contact information
Jyotshna Pokharel: The University of Texas at Dallas
Arthur Cresce: U.S. CCDC Army Research Laboratory
Bharat Pant: University of Texas at Arlington
Moon Young Yang: California Institute of Technology
Ashim Gurung: South Dakota State University
Wei He: South Dakota State University
Abiral Baniya: South Dakota State University
Buddhi Sagar Lamsal: South Dakota State University
Zhongjiu Yang: The University of Texas at Dallas
Stephen Gent: South Dakota State University
Xiaojun Xian: South Dakota State University
Ye Cao: University of Texas at Arlington
William A. Goddard: California Institute of Technology
Kang Xu: U.S. CCDC Army Research Laboratory
Yue Zhou: The University of Texas at Dallas

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrodes is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0) and low Coulombic efficiency that plague development of lithium metal batteries, but how Li+ transport behavior in the SEI is coupled with mechanical properties remains unknown. We demonstrate here a facile and scalable solution-processed approach to form a Li3N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+ across the SEI. Compared with a polycrystalline Li3N SEI obtained from conventional practice, the phase-pure/single crystalline Li3N-rich SEI constitutes an interphase of high mechanical strength and low Li+ diffusion barrier. We elucidate the correlation among Li+ transference number, diffusion behavior, concentration gradient, and the stability of the lithium metal electrode by integrating phase field simulations with experiments. We demonstrate improved reversibility and charge/discharge cycling behaviors for both symmetric cells and full lithium-metal batteries constructed with this Li3N-rich SEI. These studies may cast new insight into the design and engineering of an ideal artificial SEI for stable and high-performance lithium metal batteries.

Date: 2024
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DOI: 10.1038/s41467-024-47521-z

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