Jiahang Chen , Yang Zhang , Huichao Lu , Juan Ding , Xingchao Wang , Yudai Huang , Huiyang Ma , Jiulin Wang
{"title":"Electrolyte solvation chemistry to construct an anion-tuned interphase for stable high-temperature lithium metal batteries","authors":"Jiahang Chen , Yang Zhang , Huichao Lu , Juan Ding , Xingchao Wang , Yudai Huang , Huiyang Ma , Jiulin Wang","doi":"10.1016/j.esci.2023.100135","DOIUrl":null,"url":null,"abstract":"<div><p>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<sup>+</sup> 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<sup>+</sup> desolvation and constructs a nitrate anion-tuned interphase. Meanwhile, a high-donor-number solvent is introduced as an additive to strongly coordinate with Li<sup>+</sup>, 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<sup>−1</sup> 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 g<sub>S</sub><sup>−1</sup> for 100 cycles without capacity loss. Moreover, a 0.55 Ah pouch cell delivers a reversible energy density of 423 Wh kg<sup>−1</sup> based on these electrodes and electrolyte.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":42.9000,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"2","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"eScience","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2667141723000605","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ELECTROCHEMISTRY","Score":null,"Total":0}
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。