The intricate sulfur redox chemistry involves multiple electron transfers and complicated phase changes.Catalysts have been previously explored to overcome the kinetic barrier in lithium-sulfur batteries(LSBs).This wo...The intricate sulfur redox chemistry involves multiple electron transfers and complicated phase changes.Catalysts have been previously explored to overcome the kinetic barrier in lithium-sulfur batteries(LSBs).This work contributes to closing the knowledge gap and examines electrocatalysis for enhancing LSB kinetics.With a strong chemical affinity for polysulfides,the electrocatalyst enables efficient adsorption and accelerated electron transfer reactions.Resulting cells with catalyzed cathodes exhibit improved rate capability and excellent stability over 500 cycles with 91.9%capacity retention at C/3.In addition,cells were shown to perform at high rates up to 2C and at high sulfur loadings up to 6 mg cm^(-2).Various electrochemical,spectroscopic,and microscopic analyses provide insights into the mechanism for retaining high activity,coulombic efficiency,and capacity.This work delves into crucial processes identifying pivotal reaction steps during the cycling process at commercially relevant areal capacities and rates.展开更多
基金financial support from Lion Battery Technologies IncThe computational works used Bridges-2 at Pittsburgh Supercomputing Center through allocation Discover MAT230033 from the Advanced Cyberinfrastructure Coordination Ecosystem:Services&Support(ACCESS)program,which is supported by National Science Foundation grants#2138259,#2138286,#2138307,#2137603,and#2138296The Bridges-2 system is supported by NSF award number ACI-1928147,at the Pittsburgh Supercomputing Center(PSC)。
文摘The intricate sulfur redox chemistry involves multiple electron transfers and complicated phase changes.Catalysts have been previously explored to overcome the kinetic barrier in lithium-sulfur batteries(LSBs).This work contributes to closing the knowledge gap and examines electrocatalysis for enhancing LSB kinetics.With a strong chemical affinity for polysulfides,the electrocatalyst enables efficient adsorption and accelerated electron transfer reactions.Resulting cells with catalyzed cathodes exhibit improved rate capability and excellent stability over 500 cycles with 91.9%capacity retention at C/3.In addition,cells were shown to perform at high rates up to 2C and at high sulfur loadings up to 6 mg cm^(-2).Various electrochemical,spectroscopic,and microscopic analyses provide insights into the mechanism for retaining high activity,coulombic efficiency,and capacity.This work delves into crucial processes identifying pivotal reaction steps during the cycling process at commercially relevant areal capacities and rates.
