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

• Published in: Nature communications Vol. 15; no. 1; p. 3085
• Main Authors: 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, William A., Xu, Kang, Zhou, Yue
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 10.04.2024; Nature Publishing Group; Nature Portfolio
• Subjects: 140/146; 147/135; 147/3; 639/301/299/161; 639/4077/4079/891; Concentration gradient; Dendrites; Diffusion; Diffusion barriers; Diffusion layers; Electrodes; Electrolytes; Electrolytic cells; Humanities and Social Sciences; Interphase; Ion transport; Lithium; Lithium batteries; Mechanical properties; Metals; multidisciplinary; Science; Science (multidisciplinary); Solid electrolytes; Transport phenomena
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-47521-z

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 Li 0 ) 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 Li 3 N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li + across the SEI. Compared with a polycrystalline Li 3 N SEI obtained from conventional practice, the phase-pure/single crystalline Li 3 N-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 Li 3 N-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. Constructing an artificial solid electrolyte interphase to protect the lithium metal electrode is promising but challenging. Here, authors report a facile approach to form a layer to simultaneously overcome diffusion and advection-limited ion transport to achieve dendrite-free Li plating/stripping.