Xinyu Zheng, Yanbin Qiu, Jing Luo, Sisheng Yang, Yan Yu, Zheyuan Liu, Ran Zhang, Chengkai Yang
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引用次数: 0
摘要
调节界面电化学是缓解锂枝晶生长和提高电池性能的常用方法。然而,虽然大多数添加剂都具有抑制特性,但其对界面电化学的加速作用却很少受到关注。在这项研究中,全氟吗啉(PFM)具有促进动力学特性,可优先吸附在锂金属界面上。PFM 分子会破坏 Li+ 的溶解结构,并增强 Li+ 的迁移。与三氟甲苯相结合,形成了一个协同加速-抑制系统。对松散的外层溶胶团簇和关键的吸附-沉积步骤进行的 ab initio 分子动力学(AIMD)和密度泛函理论(DFT)计算,支持了以 C─F 和 C─H 基团为加速填充模式的快速扩散和稳定的界面电化学。这种方法可实现均匀的锂沉积。在锂||锂对称电池中实现了优异的循环性能,即使在锂||NCM811全电池中循环 200 次后,仍能保持 80% 的容量。这项研究阐明了界面的加速电化学过程,并拓展了锂金属电池加速含氟添加剂的设计策略。
Perfluorinated Amines: Accelerating Lithium Electrodeposition by Tailoring Interfacial Structure and Modulated Solvation for High-Performance Batteries.
Modulating interfacial electrochemistry represents a prevalent approach for mitigating lithium dendrite growth and enhancing battery performance. Nevertheless, while most additives exhibit inhibitory characteristics, the accelerating effects on interfacial electrochemistry have garnered limited attention. In this work, perfluoromorpholine (PFM) with facilitated kinetics is utilized to preferentially adsorb on the lithium metal interface. The PFM molecules disrupt the solvation structure of Li+ and enhance the migration of Li+. Combined with the benzotrifluoride, a synergistic acceleration-inhibition system is formed. The ab initio molecular dynamics (AIMD) and density functional theory (DFT) calculation of the loose outer solvation clusters and the key adsorption-deposition step supports the fast diffusion and stable interface electrochemistry with an accelerated filling mode with C─F and C─H groups. The approach induces the uniform lithium deposition. Excellent cycling performance is achieved in Li||Li symmetric cells, and even after 200 cycles in Li||NCM811 full cells, 80% of the capacity is retained. This work elucidates the accelerated electrochemical processes at the interface and expands the design strategies of acceleration fluorinated additives for lithium metal batteries.
期刊介绍:
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