基金the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects[2023-XMDJ-00617107]Natural Science Foundation of Yunnan Province[202401AS070646]Natural Science Foundation of Jiangxi Provincial[20232BAB214038].
文摘Despite progress in suppressing polysulfide shuttling,this challenge persists in lithium-sulfur battery commercialization.While existing strategies emphasize polysulfide adsorption and catalytic conversion,the critical role of diffusion kinetics in conversion–deposition processes remains underexplored.We design an MXene-based array architecture integrating 2D structural advantages and strong polysulfide affinity to regulate diffusion pathways.Combined experimental and multiscale computational studies reveal diffusion-mediated conversion-deposition dynamics.The sodium alginate-constructed MXene array enables three synergistic mechanisms:(1)Enhanced ion/electron delocalization reduces diffusion barriers,(2)Continuous ion transport channels facilitate charge transfer,and(3)Exposed polar surfaces promote polysulfide aggregation/conversion.Synchrotron X-ray tomography coupled with comprehensive electrochemical analyses reveals distinct mechanistic differences between conversion and deposition processes arising from diffusion heterogeneity.In situ characterization techniques combined with DFT simulation calculations demonstrate that diffusion kinetics exerts differential regulatory effects on these coupled electrochemical processes,exhibiting particular sensitivity toward the deposition mechanism.This work provides fundamental insights that reshape our understanding of diffusion-mediated phase transformation in complex multi-step electrochemical systems,offering new perspectives for advanced electrode architecture design in next-generation energy storage technologies.
