Dual‐Phase Single‐Ion Pathway Interfaces for Robust Lithium Metal in Working Batteries

• Published in: Advanced materials (Weinheim) Vol. 31; no. 19; pp. e1808392 - n/a
• Main Authors: Xu, Rui, Xiao, Ye, Zhang, Rui, Cheng, Xin‐Bing, Zhao, Chen‐Zi, Zhang, Xue‐Qiang, Yan, Chong, Zhang, Qiang, Huang, Jia‐Qi
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.05.2019
• Subjects: Anodes; Anodic protection; Batteries; Deformation; Dendritic structure; Deposition; Electric fields; Formability; Interfacial properties; Ion transport; Lithium; Lithium batteries; lithium‐metal anodes; Materials science; Metal surfaces; rechargeable batteries; single‐ion pathways; solid electrolyte interphase; Solid electrolytes; solid electrolyte interphase; single-ion pathways; rechargeable batteries; lithium-metal anodes
• DOI: 10.1002/adma.201808392
• ISSN: 0935-9648; 1521-4095

The lithium (Li) metal anode is confronted by severe interfacial issues that strongly hinder its practical deployment. The unstable interfaces directly induce unfavorable low cycling efficiency, dendritic Li deposition, and even strong safety concerns. An advanced artificial protective layer with single‐ion pathways holds great promise for enabling a spatially homogeneous ionic and electric field distribution over Li metal surface, therefore well protecting the Li metal anode during long‐term working conditions. Herein, a robust dual‐phase artificial interface is constructed, where not only the single‐ion‐conducting nature, but also high mechanical rigidity and considerable deformability can be fulfilled simultaneously by the rational integration of a garnet Al‐doped Li6.75La3Zr1.75Ta0.25O12‐based bottom layer and a lithiated Nafion top layer. The as‐constructed artificial solid electrolyte interphase is demonstrated to significantly stabilize the repeated cell charging/discharging process via regulating a facile Li‐ion transport and a compact Li plating behavior, hence contributing to a higher coulombic efficiency and a considerably enhanced cyclability of lithium metal batteries. This work highlights the significance of rational manipulation of the interfacial properties of a working Li metal anode and affords fresh insights into achieving dendrite‐free Li deposition behavior in a working battery. A single‐ion‐conducting interface consisting of dual‐layer architecture is proposed to regulate a homogeneous ionic and electric field distribution while achieving a superior mechanical feature at the surface of a lithium‐metal anode simultaneously, synergistically enabling a highly efficient cell performance of working lithium‐metal batteries.