Grain‐Boundary‐Free Glassy Solid Electrolytes based on Sulfide Materials: Effects of Oxygen and Nitrogen Doping on Electrochemical Performance. Issue 11 (22nd September 2022)

• Record Type: Journal Article
• Authors: Zhao, Ran; Hu, Guantai; Kmiec, Steven; Wheaton, Jacob; Torres, Victor M.; Martin, Steve W.
• Is Part Of: Batteries & supercaps. Volume 5:Issue 11(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-09-22
• Subjects: grain-boundary-free -- lithium battery -- mixed glass former -- solid state electrolyte -- sulfide glass; Electrochemistry -- Periodicals; Electrodes -- Periodicals; Electric batteries -- Periodicals; 621.31242
• DOI: 10.1002/batt.202100356
• Languages: English
• ISSNs: 2566-6223

Abstract

Abstract: While much of the current research on glassy solid electrolytes (GSEs) has focused on the binary Li2 S+P2 S5 system, compositions with Si are of interest because Si promotes stronger glass formation and allows low‐cost melt‐quenching (MQ) synthesis under ambient pressure. Another advantage is that they can be formed in homogeneous and continuous glass forms, as a result they are free of grain boundaries. In this work, we have examined the structures and electrochemical properties of bulk glass pieces of sulfide and oxy‐sulfide GSE compositions and have also expanded the study by using LiPON glass as a dopant to produce an entirely new class of nitrogen doped mixed oxy‐sulfide nitride (MOSN) GSEs. Upon doping with oxygen and nitrogen, the solid electrolyte interface (SEI) is stabilized and the doped MOSN GSE exhibits a critical current density (CCD) of 1.8 mA cm −2 at 100 °C. We also report on improving the glass quality, the SEI engineering and its limitations, and future plans of improving the electrochemical performance of these homogeneous MQ MOSN GSEs. These fundamental results can help to understand the structures and doping effects of the bulk GSEs, and as such can provide a guide to design improved homogeneous grain‐boundary‐free GSEs. Abstract : Grain‐boundary‐free glassy solid electrolytes are successfully synthesized and the doping effects of oxygen and nitrogen in the sulfide dense glass electrolytes are investigated for the first time. The doped sample exhibits a critical current density of 1.8 mA cm −2 at 100 °C, and the strategies of further improving the electrochemical performance and glass quality are also disscussed, which provide a guide to design superior homogeneous glassy solid electrolyte that can be used in large scale batteries.