Synergistic regulation of lithium nucleation and anion-rich solvation structure via silver trifluoroacetate additive for stable lithium metal anodes

Jing Bai, Wenjie Cheng, Tao Wang, Sheng Liu
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Abstract

Lithium (Li) metal, owing to its high theoretical specific capacity and low electrochemical potential, is considered one of the most promising anode materials for next-generation rechargeable batteries. However, interfacial instability severely hinders the practical application of Li anodes. Constructing a robust solid electrolyte interphase (SEI) with optimized chemical composition and structure has been recognized as an effective strategy to overcome this challenge. Here, we propose silver trifluoroacetate (AgTFA) as a multifunctional electrolyte additive that synergistically regulates Li nucleation and promotes the formation of an anion-rich solvation structure. Through a spontaneous in situ displacement reaction, uniformly distributed silver nanoparticles (Ag NPs) are generated on the Li surface, providing abundant lithiophilic nucleation sites to enable homogeneous Li deposition. Meanwhile, trifluoroacetate anions (TFA-) with an ultrahigh donor number, together with NO3- anions participating in Li+ solvation, markedly reduce the desolvation barrier and facilitate the formation of a LiF-Li3N-rich SEI. As a result, Li||Li symmetric cells exhibit remarkable cycling stability of up to 2,500 hours at 0.5 mA·cm-2/0.5 mAh·cm-2, while Li||LiFePO4 full cells deliver a high discharge capacity of 139.8 mAh·g-1 with an excellent capacity retention of 97.28% after 200 cycles at 1.0 C. This work demonstrates a feasible strategy for constructing durable SEI layers by coupling Li nucleation regulation with anion-rich solvation chemistry.
三氟乙酸银添加剂对锂成核和富阴离子溶剂化结构的协同调节
锂金属由于具有较高的理论比容量和较低的电化学电位,被认为是下一代可充电电池最有前途的负极材料之一。然而,界面不稳定性严重阻碍了锂阳极的实际应用。构建具有优化化学成分和结构的坚固固体电解质间相(SEI)是克服这一挑战的有效策略。在这里,我们提出三氟乙酸银(AgTFA)作为一种多功能电解质添加剂,协同调节Li成核并促进富阴离子溶剂化结构的形成。通过自发的原位位移反应,在锂表面生成均匀分布的银纳米粒子(Ag NPs),提供丰富的亲锂成核位点,使锂沉积均匀。同时,超高供体数的三氟乙酸阴离子(TFA-)与参与Li+溶剂化的NO3-阴离子一起,显著降低了脱溶屏障,促进了富lif - li3n SEI的形成。结果表明,Li||锂对称电池在0.5 mA·cm-2/0.5 mAh·cm-2下的循环稳定性可达2500小时,而Li||LiFePO4全电池在1.0 c下200次循环后的放电容量高达139.8 mAh·g-1,容量保持率高达97.28%。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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