Strongly Solvating Ether Electrolytes for High-Voltage Lithium Metal Batteries,ACS Applied Materials & Interfaces

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Strongly Solvating Ether Electrolytes for High-Voltage Lithium Metal Batteries
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-01 , DOI: 10.1021/acsami.3c00165
Shunqiang Chen ₁ , Weiduo Zhu ₂ , Lijiang Tan ₁ , Digen Ruan ₁ , JiaJia Fan ₁ , Yunhua Chen ₃ , Xianhui Meng ₃ , Qingshun Nian ₁ , Xin Zhao ₁ , Jinyu Jiang ₁ , Zihong Wang ₁ , Shuhong Jiao ₁ , Xiaojun Wu ₁ , Xiaodi Ren ₁

Affiliation

Ethers are promising electrolytes for lithium (Li) metal batteries (LMBs) because of their unique stability with Li metal. Although intensive research on designing anion-enriched electrolyte solvation structures has greatly improved their electrochemical stabilities, ether electrolytes are approaching an anodic bottleneck. Herein, we reveal the strong correlation between electrolyte solvation structure and oxidation stability. In contrast to previous designs of weakly solvating solvents for enhanced anion reactivities, the triglyme (G3)-based electrolyte with the largest Li⁺ solvation energy among different linear ethers demonstrates greatly improved stability on Ni-rich cathodes under an ultrahigh voltage of 4.7 V (93% capacity retention after 100 cycles). Ether electrolytes with a stronger Li⁺ solvating ability could greatly suppress deleterious oxidation side reactions by decreasing the lifetime of free labile ether molecules. This study provides critical insights into the dynamics of the solvation structure and its significant influence on the interfacial stability for future development of high-efficiency electrolytes for high-energy-density LMBs.

中文翻译：

用于高压锂金属电池的强溶剂化醚电解质

醚是锂 (Li) 金属电池 (LMB) 的有前途的电解质，因为它们与锂金属具有独特的稳定性。尽管对设计富含阴离子的电解质溶剂化结构的深入研究大大提高了它们的电化学稳定性，但醚类电解质正接近阳极瓶颈。在此，我们揭示了电解质溶剂化结构与氧化稳定性之间的强相关性。与之前为增强阴离子反应性而设计的弱溶剂化溶剂相比，在不同线性醚中具有最大 Li ⁺溶剂化能的三甘醇二甲醚 (G3) 基电解质在 4.7 V 的超高电压下表现出在富镍阴极上的稳定性大大提高（ 100 次循环后容量保持率为 93%）。具有更强 Li ^{+ 的醚类电解质}溶剂化能力可以通过降低游离不稳定醚分子的寿命来极大地抑制有害的氧化副反应。这项研究为溶剂化结构的动力学及其对界面稳定性的重大影响提供了重要的见解，从而为高能量密度 LMB 的高效电解质的未来发展提供了重要的见解。

更新日期：2023-03-01

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