Lanthanum lithium titanate is one of the promising electrolytes for solid-state lithium-ion batteries due to its high bulk ionic conductivity up to∼10^(−3) S/cm.However,the practical application of this material has ...Lanthanum lithium titanate is one of the promising electrolytes for solid-state lithium-ion batteries due to its high bulk ionic conductivity up to∼10^(−3) S/cm.However,the practical application of this material has been bottlenecked by high grain boundary(GB)resistance,while the underlying mechanism is still under debate.Here we report a comprehensive study with direct evidence to reveal the origin of high GB resistance in La_(2/3)–xLi_(3x)TiO_(3)(LLTO).Atomic-scale observations via advanced scanning transmission electron microscopy show that the GBs are uniformly subject to subsurface segregation of La atoms to compensate for the excess surface charges.The La segregation leads to an abrupt decrease of charge carrier concentration neighboring GBs and hence is supposed to have deleterious effect on GB conductivity.The findings suggest a novel mechanism of space-charge-induced cation segregation,which shed lights on the intrinsic origin of low GB ionic conductivity in LLTO.展开更多
基金Project(E2013402056)supported by the Natural Science Foundation of Hebei Province,ChinaProject(QN2014002)supported by the Science and Technology Research Foundation of Hebei Education Department for Young Teachers in University,ChinaProject(51601053)supported by the National Natural Science Foundation of China
基金This work was supported by the National Natural Science Foundation of China(U2030206,22075003).
文摘Lanthanum lithium titanate is one of the promising electrolytes for solid-state lithium-ion batteries due to its high bulk ionic conductivity up to∼10^(−3) S/cm.However,the practical application of this material has been bottlenecked by high grain boundary(GB)resistance,while the underlying mechanism is still under debate.Here we report a comprehensive study with direct evidence to reveal the origin of high GB resistance in La_(2/3)–xLi_(3x)TiO_(3)(LLTO).Atomic-scale observations via advanced scanning transmission electron microscopy show that the GBs are uniformly subject to subsurface segregation of La atoms to compensate for the excess surface charges.The La segregation leads to an abrupt decrease of charge carrier concentration neighboring GBs and hence is supposed to have deleterious effect on GB conductivity.The findings suggest a novel mechanism of space-charge-induced cation segregation,which shed lights on the intrinsic origin of low GB ionic conductivity in LLTO.