A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)i...A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)ion,1-aza-12-crown-4-ether(A12C4)with cavity size well matched manganese(Ⅱ)ion is used in this work as electrolyte additive.Theoretical and experimental results show that stable complex forms between A12C4 and manganese(II)ions in the electrolyte,which does not affect the solvation of Li ions.The strong binding effect of A12C4 additive reduces the charge density of manganese(II)ion and inhibits its destruction of the PF_(6)^(-)structure in the electrolyte,leading to greatly improved thermal stability of manganese(II)ions-containing electrolyte.In addition to bulk electrolyte,A12C4 additive also shows capability in preventing Mn^(2+) from degrading SEI on graphite surface.Such bulk and interphasial stability introduced by A12C4 leads to significantly improved cycling performance of LIBs.展开更多
基金supported by the National Natural Science Foundation of China(21972049)the Guangdong Program for Distinguished Young Scholar(2017B030306013)the Science and Technology Planning Project of Guangdong Province(2017B090901020)。
文摘A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)ion,1-aza-12-crown-4-ether(A12C4)with cavity size well matched manganese(Ⅱ)ion is used in this work as electrolyte additive.Theoretical and experimental results show that stable complex forms between A12C4 and manganese(II)ions in the electrolyte,which does not affect the solvation of Li ions.The strong binding effect of A12C4 additive reduces the charge density of manganese(II)ion and inhibits its destruction of the PF_(6)^(-)structure in the electrolyte,leading to greatly improved thermal stability of manganese(II)ions-containing electrolyte.In addition to bulk electrolyte,A12C4 additive also shows capability in preventing Mn^(2+) from degrading SEI on graphite surface.Such bulk and interphasial stability introduced by A12C4 leads to significantly improved cycling performance of LIBs.