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

Pokharel, Jyotshna; Cresce, Arthur; Pant, Bharat; Yang, Moon Young; Gurung, Ashim; He, Wei; Baniya, Abiral; Lamsal, Buddhi Sagar; Yang, Zhongjiu; Gent, Stephen; Xian, Xiaojun; Cao, Ye; Goddard III, William A.; Xu, Kang; Zhou, Yue

doi:10.1038/s41467-024-47521-z

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

Journal Article · 10 April 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-47521-z · OSTI ID:2335931

Pokharel, Jyotshna ^[1];

^[2];

^[3];

^[4]; Gurung, Ashim ^[5]; He, Wei ^[5]; Baniya, Abiral ^[5]; Lamsal, Buddhi Sagar ^[5];

^[6]; Gent, Stephen ^[5];

^[5];

^[3];

^[4];

^[7];

^[6]

Univ. of Texas at Dallas, Richardson, TX (United States); South Dakota State Univ., Brookings, SD (United States)
Army Research Lab., Adelphi, MD (United States)
Univ. of Texas, Arlington, TX (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)
South Dakota State Univ., Brookings, SD (United States)
Univ. of Texas at Dallas, Richardson, TX (United States)
Army Research Lab., Adelphi, MD (United States); SolidEnergy Systems LLC, Woburn, MA (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2335931

Alternate ID(s):: OSTI ID: 2470263

Journal Information:: Nature Communications, Vol. 15, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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