Optimization of chlorine content in Li7-xPS6-xClx solid electrolytes for high-performance all-solid-state batteries
In the context of the rapid development of all-solid-state batteries,the argyrodite-type electrolyte Li6PS5Cl has attracted significant attention due to its high ionic conductivity and favorable processing characteristics.The chlorine substitution level in the electrolyte significantly influences its ionic conductivity and stability,yet research on the effects of chlorine content on interfacial interactions remains incomplete.In this study,Li7-xPS6-xClx electrolytes with x ranging from 1.0 to 1.5 were synthesized using a solid-state sintering method,evaluating the impact of x=1.0-1.5 related chlorine content(Cl content from 25%-37.5%,mole fraction)on their physicochemical properties.Additionally,based on the performance of the electrolyte in various battery components,a systematic evaluation of the influence of chlorine content on interfacial interactions and performance was conducted,integrating techniques such as X-ray photoelectron spectroscopy and the distribution of impedance relaxation times.The material Li5.7PS4.7Cl1.3 exhibits superior rate performance in the cathode.However,electrolyte layers with high chlorine content Li5.5PS4.5Cl1.5 lead to degradation at both anode and cathode interfaces,reducing cycle performance.By adjusting the chlorine content,a balance between ionic conductivity and interfacial reactions can be achieved,enhancing the overall battery performance.The assembled LiNi0.8Co0.1Mn0.1O2@Li5.7PS4.7Cl1.3|Li6PS5Cl|LiIn battery maintains a specific capacity of 132.8 mA∙h/g after 300 cycles at loading of 20 mg/cm2 and rate of 0.5C.
sulfide solid electrolytesLi7-xPS6-xClxall-solid-state batterieschlorine substitutiondistribution of relaxation times