Unraveling the Intra and Intercycle Interfacial Evolution of Li6PS5Cl‐Based All‐Solid‐State Lithium Batteries. Issue 4 (10th December 2019)

• Record Type: Journal Article
• Authors: Zhang, Jun; Zheng, Chao; Li, Lujie; Xia, Yang; Huang, Hui; Gan, Yongping; Liang, Chu; He, Xinping; Tao, Xinyong; Zhang, Wenkui
• Is Part Of: Advanced energy materials. Volume 10:Issue 4(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2019-12-10
• Subjects: all‐solid‐state lithium batteries -- argyrodite Li6PS5Cl -- in situ characterizations -- interface evolution -- space charge layer; Energy harvesting -- Materials -- Periodicals; Energy conversion -- Materials -- Periodicals; Energy storage -- Materials -- Periodicals; Photovoltaics -- Periodicals; Fuel cells -- Periodicals; Thermoelectric materials -- Periodicals; 621.31
• DOI: 10.1002/aenm.201903311
• Languages: English
• ISSNs: 1614-6832

Abstract

Abstract: High‐performance rechargeable all‐solid‐state lithium metal batteries with high energy density and enhanced safety are attractive for applications like portable electronic devices and electric vehicles. Among the various solid electrolytes, argyrodite Li6 PS5 Cl with high ionic conductivity and easy processability is of great interest. However, the low interface compatibility between sulfide solid electrolytes and high capacity cathodes like nickel‐rich layered oxides requires many thorny issues to be resolved, such as the space charge layer (SCL) and interfacial reactions. In this work, in situ electrochemical impedance spectroscopy and in situ Raman spectroscopy measurements are performed to monitor the detailed interface evolutions in a LiNi0.8 Co0.1 Mn0.1 O2 (NCM)/Li6 PS5 Cl/Li cell. Combining with ex situ characterizations including scanning electron microscopy and X‐ray photoelectron spectroscopy, the evolution of the SCL and the chemical bond vibration at NCM/Li6 PS5 Cl interface during the early cycles is elaborated. It is found that the Li + ion migration, which varies with the potential change, is a very significant cause of these interface behaviors. For the long‐term cycling, the SCL, interfacial reactions, lithium dendrites, and chemo‐mechanical failure have an integrated effect on interfaces, further deteriorating the interfacial structure and electrochemical performance. This research provides a new insight on intra and intercycle interfacial evolution of solid‐state batteries. Abstract : Several in situ and ex situ measurements are used to monitor the interfacial evolutions in a LiNi0.8 Co0.1 Mn0.1 O2 (NCM)/Li6 PS5 Cl/Li cell. The detailed interfacial evolution shows very different behavior between inter and intracycles. The evolution of the space charge layer and the chemical bond vibration at NCM/Li6 PS5 Cl interface play key roles during the early cycles.