Jiahang Chen , Yang Zhang , Huichao Lu , Juan Ding , Xingchao Wang , Yudai Huang , Huiyang Ma , Jiulin Wang
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引用次数: 2
Abstract
Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li+ coordination structure via electrolyte solvation chemistry. Nitrate anions are aggregated in the solvation sheath, even at low concentration in a solvent with moderate solvation ability, which promotes Li+ desolvation and constructs a nitrate anion-tuned interphase. Meanwhile, a high-donor-number solvent is introduced as an additive to strongly coordinate with Li+, which accelerates the ion-transfer kinetics and rate performance. This not only results in micro-sized lithium deposition and a high CE of 99.5% over 3500 h, but also enables superior anode stability even under 50% depth plating/stripping and with a lean electrolyte of 3 g Ah−1 at 50 °C. A lithium–sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%. A full battery using 1x excess lithium exhibits a high capacity near 1600 mAh gS−1 for 100 cycles without capacity loss. Moreover, a 0.55 Ah pouch cell delivers a reversible energy density of 423 Wh kg−1 based on these electrodes and electrolyte.
锂金属电池被认为是有前途的下一代储能系统。然而,不稳定的阳极界面导致枝晶生长和不可逆的锂消耗,且库仑效率(CE)低。在此,我们通过电解质溶剂化化学合理地设计了Li+配位结构。在中等溶剂化能力的溶剂中,即使在低浓度下,硝酸盐阴离子也会聚集在溶剂鞘中,促进Li+的脱溶,构建硝酸盐阴离子调质间相。同时,引入高给体数溶剂作为添加剂,与Li+强配位,加快了离子转移动力学和速率性能。这不仅导致了微尺寸的锂沉积和在3500小时内99.5%的高CE,而且在50°C下,即使在50%深度电镀/剥离和3 g Ah−1的稀薄电解质下,也能实现卓越的阳极稳定性。锂硫电池的寿命延长至2000次循环,平均CE为100%。使用1倍多余锂的完整电池在100次循环中具有接近1600 mAh gS−1的高容量,而不会出现容量损失。此外,基于这些电极和电解质,0.55 Ah的袋状电池可提供423 Wh kg−1的可逆能量密度。