Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_...Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_(5)Cl are especially promising due to their superior ionic conductivity.However,interfacial degradation between sulfide electrolytes and high-voltage cathodes,such as LiCoO_(2),limits long-term performance.This study demonstrates that a LiBF_(4)-derived F-rich coating on LiCoO_(2),applied by immersing LiCoO_(2) particles in a LiBF_(4) solution followed by annealing,can significantly enhance performance in Li_(6)PS_(5)Cl-based solid-state batteries.This coating enables stable high-voltage(4.5 V vs Li^(+)/Li)operation,achieving an initial specific capacity of 153.82 mAh g^(−1) and 87.1%capacity retention over 300 cycles at 0.5C.The enhanced performance stems from the F-rich coating,composed of multiple phases including LiF,CoF_(2),Li_(x)BF_(y)O_(z),and Li_(x)BO_(y),which effectively suppresses side reactions at the LiCoO_(2)|Li_(6)PS_(5)Cl interface and improves lithium-ion diffusivity,thereby enabling greater Li capacity utilization.Our findings provide a practical pathway for advancing solid-state batteries with high-voltage LiCoO_(2) cathodes,offering substantial promise for next-generation energy storage systems.展开更多
基金financial support under the scope of the COMET program within the K2 Center“Integrated Computational Material,Process and Product Engineering(IC-MPPE)”(Project ASSESS P1.10)financial support by the Austrian Federal Ministry for Digital and Economic Affairs,the National Foundation for Research,Technology and Development and the Christian Doppler Research Association(Christian Doppler Laboratory for Solid-State Batteries).
文摘Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_(5)Cl are especially promising due to their superior ionic conductivity.However,interfacial degradation between sulfide electrolytes and high-voltage cathodes,such as LiCoO_(2),limits long-term performance.This study demonstrates that a LiBF_(4)-derived F-rich coating on LiCoO_(2),applied by immersing LiCoO_(2) particles in a LiBF_(4) solution followed by annealing,can significantly enhance performance in Li_(6)PS_(5)Cl-based solid-state batteries.This coating enables stable high-voltage(4.5 V vs Li^(+)/Li)operation,achieving an initial specific capacity of 153.82 mAh g^(−1) and 87.1%capacity retention over 300 cycles at 0.5C.The enhanced performance stems from the F-rich coating,composed of multiple phases including LiF,CoF_(2),Li_(x)BF_(y)O_(z),and Li_(x)BO_(y),which effectively suppresses side reactions at the LiCoO_(2)|Li_(6)PS_(5)Cl interface and improves lithium-ion diffusivity,thereby enabling greater Li capacity utilization.Our findings provide a practical pathway for advancing solid-state batteries with high-voltage LiCoO_(2) cathodes,offering substantial promise for next-generation energy storage systems.