The application of all-solid-state Li-metal batteries with solid oxide electrolytes is hindered by interfacial issues,especially the solid electrolyte/Li-metal interface.This work introduced a uniform indium film laye...The application of all-solid-state Li-metal batteries with solid oxide electrolytes is hindered by interfacial issues,especially the solid electrolyte/Li-metal interface.This work introduced a uniform indium film layer on the surface of Na^(+)super ionic conductor(NASICON)solid electrolyte Li_(1.5)Al_(0.5)Ge_(1.5)P_(3)O_(12)(LAGP),which promotes the intimate contact between Li metal and solid electrolyte and hinders the side reactions at the interface.Electrochemical impedance spectra show that the battery with coated solid electrolyte presents a smaller interfacial resistance and maintains stability after a long cycling time.By contrast,the baseline battery with a pure LAGP pellet shows a contact loss after cycling with the vibration of interfacial impedance.The Li symmetric cells with indium-modified solid electrolyte present stable cycling behavior over 400 h at 0.1 and 0.2 mA·cm^(−2).The all-solid-state Li-metal batteries with a Li anode,indium coating LAGP and two kinds of cathodes,namely carbon nanotubes(CNTs)and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),are prepared and tested.The CNTs cathode for Li-O2 and Li-air batteries has a higher specific capacity than traditional Li-ion battery cathodes.The Li-NCM811 batteries deliver an initial Coulombic efficiency of about 75%,with 82%capacity retention after 20 cycles.展开更多
Li1.5Al0.5Ge1.5(PO4)3(LAGP)is a solid-state electrolyte with high ionic conductivity and air stability but poor chemical stability and high interfacial impedance when directly contacted with Li metal.In this work,we d...Li1.5Al0.5Ge1.5(PO4)3(LAGP)is a solid-state electrolyte with high ionic conductivity and air stability but poor chemical stability and high interfacial impedance when directly contacted with Li metal.In this work,we develop an inorganic/polymer hybrid interlayer composed of Li bis(trifluoromethylsulfonyl)imide/poly(vinylene carbonate)polymer electrolyte and SiO2 submicrospheres to stabilize the Li/LAGP interface.The polymeric component renders high ionic conductance and low interfacial resistance,whereas the inorganic component imparts flame retardancy and a physical barrier to the known Li-LAGP side reaction,together enabling stable Li stripping/plating for more than 1,500 h at room temperature.With this interlayer at both electrodes,all-solid-state Li∥LiFePO4 full cells with stable cycling performance are also demonstrated.展开更多
文摘The application of all-solid-state Li-metal batteries with solid oxide electrolytes is hindered by interfacial issues,especially the solid electrolyte/Li-metal interface.This work introduced a uniform indium film layer on the surface of Na^(+)super ionic conductor(NASICON)solid electrolyte Li_(1.5)Al_(0.5)Ge_(1.5)P_(3)O_(12)(LAGP),which promotes the intimate contact between Li metal and solid electrolyte and hinders the side reactions at the interface.Electrochemical impedance spectra show that the battery with coated solid electrolyte presents a smaller interfacial resistance and maintains stability after a long cycling time.By contrast,the baseline battery with a pure LAGP pellet shows a contact loss after cycling with the vibration of interfacial impedance.The Li symmetric cells with indium-modified solid electrolyte present stable cycling behavior over 400 h at 0.1 and 0.2 mA·cm^(−2).The all-solid-state Li-metal batteries with a Li anode,indium coating LAGP and two kinds of cathodes,namely carbon nanotubes(CNTs)and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),are prepared and tested.The CNTs cathode for Li-O2 and Li-air batteries has a higher specific capacity than traditional Li-ion battery cathodes.The Li-NCM811 batteries deliver an initial Coulombic efficiency of about 75%,with 82%capacity retention after 20 cycles.
基金This work was supported by the US National Science Foundation(No.CBET-1903342)Y.R.H.acknowledges the exchange graduate student scholarship from the China Scholarship Council.Y.R.Z.acknowledges the Link Foundation Energy Fellowship.L.M.Q.acknowledges support from the Ministry of Science and Technology of China(No.2018YFA0703502)H.L.W.acknowledges the Sloan Research Fellowship.
文摘Li1.5Al0.5Ge1.5(PO4)3(LAGP)is a solid-state electrolyte with high ionic conductivity and air stability but poor chemical stability and high interfacial impedance when directly contacted with Li metal.In this work,we develop an inorganic/polymer hybrid interlayer composed of Li bis(trifluoromethylsulfonyl)imide/poly(vinylene carbonate)polymer electrolyte and SiO2 submicrospheres to stabilize the Li/LAGP interface.The polymeric component renders high ionic conductance and low interfacial resistance,whereas the inorganic component imparts flame retardancy and a physical barrier to the known Li-LAGP side reaction,together enabling stable Li stripping/plating for more than 1,500 h at room temperature.With this interlayer at both electrodes,all-solid-state Li∥LiFePO4 full cells with stable cycling performance are also demonstrated.