Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ...Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ability to suppress Li dendrite growth at high current densities.This study addresses both issues by incorporating two-dimensional oxygenated carbon nitride(2D OCN)into a polyvinylidene fluoride(PVDF)-based composite polymer electrolyte and modifying the Li anode with OCN.The OCN nanosheets incorporated PVDF electrolyte exhibits a high ionic conductivity(1.6×10^(-4)S cm^(-1)at 25℃)and Li+transference number(0.62),wide electrochemical window(5.3),and excellent fire resistance.Furthermore,the OCN-modified Li anode in situ generates a protective layer of Li_(3)N during cycling,preventing undesirable reactions with PVDF electrolyte and effectively suppressing Li dendrite growth.Symmetric cells using the upgraded PVDF polymer electrolyte and modified Li anode demonstrate long cycling stability over 2500 h at 0.1 mA cm^(-2).Full cells with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode exhibit high energy density and long-term cycling stability,even at a high loading of 8.2 mg cm^(-2).Incorporating 2D OCN nanosheets into the PVDF-based electrolyte and Li-metal anode provides an effective strategy for achieving safe and high-energy-density Li-metal batteries.展开更多
基金National Key Research and Development Program of China,Grant/Award Number:2023YFB2503801National Natural Science Foundation of China,Grant/Award Numbers:52302253,5202780089+2 种基金Fundamental Research Funds for the Central Universities,Grant/Award Number:HUST:2172020kfyXJJS089Key R&D Program of Hubei Province,Grant/Award Number:2023BAB028Key Program of the National Natural Science Foundation of China,Grant/Award Number:52231009。
文摘Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ability to suppress Li dendrite growth at high current densities.This study addresses both issues by incorporating two-dimensional oxygenated carbon nitride(2D OCN)into a polyvinylidene fluoride(PVDF)-based composite polymer electrolyte and modifying the Li anode with OCN.The OCN nanosheets incorporated PVDF electrolyte exhibits a high ionic conductivity(1.6×10^(-4)S cm^(-1)at 25℃)and Li+transference number(0.62),wide electrochemical window(5.3),and excellent fire resistance.Furthermore,the OCN-modified Li anode in situ generates a protective layer of Li_(3)N during cycling,preventing undesirable reactions with PVDF electrolyte and effectively suppressing Li dendrite growth.Symmetric cells using the upgraded PVDF polymer electrolyte and modified Li anode demonstrate long cycling stability over 2500 h at 0.1 mA cm^(-2).Full cells with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode exhibit high energy density and long-term cycling stability,even at a high loading of 8.2 mg cm^(-2).Incorporating 2D OCN nanosheets into the PVDF-based electrolyte and Li-metal anode provides an effective strategy for achieving safe and high-energy-density Li-metal batteries.
