摘要：The polysulfide shuttling effect is the primary bottleneck restricting the industrial application of Li-S batteries,and the electrocatalytic sulfur reduction reaction(SRR)has emerged as an effective ***-based singleatom catalysts(SACs),which promotes SRR,show great potential in inhibiting the shuttling effect of ***,the optimization and rational design of such catalysts requires a deep understanding to the fundamental SRR mechanism and remains highly *** this work,we construct a comprehensive database of carbon-based SACs,covering different coordination patterns,heteroatoms,and transition *** SRR activities are determined using density functional theory calculations,revealing a synergistic effect between the p orbital of the heteroatom and the d orbital of the transition *** interplay underscores the critical importance of the coordination environment for SRR under the ortho-P_(2)C_(2)*** of the transition metal type,the ortho-P_(2)C_(2)coordination pattern significantly enhances the SRR performance of SACs,surpassing the widely reported N_(3)C_(1)and N_(4)coordinated graphene-based ***,heteroatoms with ortho-P_(2)C_(2)may exhibit SRR *** a word,by using this comprehensive dataset and data-driven framework,we propose a promising novel class of coordination structure(ortho-P_(2)C_(2)structure)and neglected design principle.

摘要：聚合物基固态电解质得益于其易加工性,最有希望应用于下一代固态锂金属电池.目前,聚合物基态电解质的离子电导率提升策略多为加入导锂陶瓷以构建离子传输通道,其提升程度有限.电场在锂离子输运过程中存在重要影响,目前研究中有关电场对锂离子传输的影响机制尚不明确.本文将兼具高离子电导率和高介电常数的铌酸锂嵌入聚偏氟乙烯基体中,设计了一种新型复合固态电解质.铌酸锂颗粒有效调节电解质内部电场结构,增强了离子输运方向电场强度,实现了离子电导率的大幅提升(7.39×10^(-4)S cm^(-1),25℃).该电解质匹配高镍正极和锂金属负极的固态电池可稳定循环1000次以上,容量保持率为72%.该研究为设计下一代固态锂电池用高离子电导复合固态电解质提供了新的策略.