Monothetic and conductive network and mechanical stress releasing layer on micron-silicon anode enabling high-energy solid-state battery

Silicon has ultrahigh capacity,dendrite-free alloy lithiation mechanism and low cost and has been regarded as a promising anode candidate for solid-state battery.Owing to the low infiltration of solid-state electrolyte(SSE),not the unstable solid-electrolyte interphase(SEI),but the huge stress during lithiation-and delithiation-induced particle fracture and conductivity lost tend to be the main issues.In this study,starting with micron-Si,a novel monothetic carbon conductive framework and a MgO coating layer are designed,which serve as electron pathway across the whole electrode and stress releasing layer,respectively.In addition,the in situ reaction between Si and SSE helps to form a LiF-rich and mechanically stable SEI layer.As a result,the mechanical stability and charge transfer kinetics of the uniquely designed Si anode are significantly improved.Consequently,high initial Coulombic efficiency,high capacity and durable cycling stability can be achieved by applying the Si@MgO@C anode in SSB.For example,high specific capacity of 3224.6 mAh·g^(-1)and long cycling durability of 200 cycles are achieved.This work provides a new concept for designing alloy-type anode that combines surface coating on particle and electrode structure design.

Liquid metal welding enabling high loading binder/carbon-free layered oxide cathode toward high-performance liquid and solid-state battery

High loading cathode with high active material proportion is a practical demand but far below the desirable value to achieve high energy density lithium-ion batteries(LIBs).Normally,the Li^(+)/electron transport between active materials and electrolyte/c arbon,however,it is poor and areal resistance is extremely high for a high loading/thick cathode.In this manuscript,taking high-voltage lithium cobalt oxide LiCoO_(2)(LCO)as an example,we design a facile liquid metal welding method enabled by a low melting-point indium-tin oxide In_(2)O_(3)/SnO_(2)(ITO)during a thermal treatment process,the strongly adhesion active particles show robust mechanical property for the free-standing LCO cathode with a pellet architecture.We also demonstrate that the O_(2)atmosphere plays a critical role on the interfacial property,that is preventing the layered structure to rock-salt Co_(3)O_(4)as well as further enhancing the interfacial mechanical integration.As expected,the LCO-ITO free-standing cathode not only shows robust mechanical property with densely packed configuration but also provides a fast Li^(+)/electron pathway at the interface.Consequently,the LCO-ITO composite cathode exhibits excellent electrochemical cycling performance in both liquid and solid-state cells.For example,even at a high active material mass of 56 mg·cm^(-2),the LCO cathode still delivers a specific capacity of 151 mAh·g^(-1)and maintains132.5 mAh·g^(-1)(corresponding to 7.4 mAh·cm^(-2))after 80cycles.The LCO-ITO-O_(2)cathode is also applicable to a solidstate cell,which exhibits a high capacity of 100.4 mAh·g^(-1)after 200 cycles of long-term cycling.The excellent electrochemical of the LCO-ITO-O_(2)reveals the successful engineering mechanical architecture and interfacial carriers transport,which may be expected as an alternative approach to achieve high energy density LIBs.