title: Transition from Superlithiophobicity to Superlithiophilicity of Garnet Solid-State Electrolyte.
abstract: All-solid-state Li-batteries using solid-state electrolytes (SSEs) offer enhanced safety over conventional Li-ion batteries with organic liquid electrolytes due to the nonflammable nature of SSEs. The superior mechanical strength of SSEs can also protect against Li dendrite penetration, which enables the use of the highest specific capacity (3861 mAh/g) and lowest redox potential (-3.04 V vs standard hydrogen electrode) anode: Li metal. However, contact between the Li metal and SSEs presents a major challenge, where a large polarization occurs at the Li metal/SSE interface. Here, the chemical properties of a promising oxide-based SSE (garnet) changed from "super-lithiophobicity" to "super-lithiophilicity" through an ultrathin coating of amorphous Si deposited by plasma-enhanced chemical vapor deposition (PECVD). The wettability transition is due to the reaction between Li and Si and the in situ formation of lithiated Si. As a result, symmetric cells composed of a Si-coated garnet-structured SSE and Li metal electrodes exhibited much smaller impedance and excellent stability upon plating/stripping cycles compared to cells using bare garnet SSE. Specifically, the interfacial resistance between Li and garnet dramatically decreased from 925 to 127 Ω cm(2) when lithiated Si was formed on the garnet. Our discovery of switchable lithiophobic-lithiophilic surfaces to improve the Li metal/SSE interface opens opportunities for improving many other SSEs.
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Wei
authors: W
authors: Luo
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Yunhui
authors: Y
authors: Gong
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Yizhou
authors: Y
authors: Zhu
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Kun Kelvin
authors: KK
authors: Fu
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Jiaqi
authors: J
authors: Dai
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Steven D
authors: SD
authors: Lacey
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Chengwei
authors: C
authors: Wang
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Boyang
authors: B
authors: Liu
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Xiaogang
authors: X
authors: Han
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Yifei
authors: Y
authors: Mo
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Eric D
authors: ED
authors: Wachsman
authors: Department of Materials Science and Engineering, ‡Department of Mechanical Engineering, and §University of Maryland Energy Research Center, University of Maryland , College Park, Maryland 20742, United States.
authors: Liangbing
authors: L
authors: Hu