Eco-friendly electrolytes via a robust bond design for high-energy Li metal batteries,Energy & Environmental Science

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Eco-friendly electrolytes via a robust bond design for high-energy Li metal batteries
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2022-09-02 , DOI: 10.1039/d2ee01756c
Yiqiang Huang ₁ , Ruhong Li ₁ , Suting Weng ₂ , Haikuo Zhang ₁ , Chunnan Zhu ₁ , Di Lu ₁ , Chuangchao Sun ₁ , Xiaoteng Huang ₁ , Tao Deng ₃ , Liwu Fan ₄ , Lixin Chen _{1,

5} , Xuefeng Wang _{2,

6} , Xiulin Fan ₁

Affiliation

Electrolyte innovation that enables the formation of an anion-derived inorganic-rich solid electrolyte interphase (SEI) on electrodes and possesses wide electrochemical stability is critical for the commercialization of Li metal batteries (LMBs). While recent breakthroughs have improved the battery performance, no eco-friendly and economical less-fluorinated electrolytes can yet meet the practical requirements. Herein, we report a family of siloxane solvents, in which Si–O bonds confer high compatibility to Li metal anodes and high oxidation stability to cathodes simultaneously. The 1.5 M LiFSI in a dimethyldimethoxysilane electrolyte without any additives/cosolvents enables Li metal to achieve a high plating/stripping Coulombic efficiency (CE) of ∼99.8% as well as high-voltage LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) and LiCoO₂ (LCO) to achieve a high CE of >99.9%, allowing 4.5 V LiCoO₂ (3 mA h cm⁻²)||Li (20 μm) cells to retain 95% capacity after 200 cycles and 1.4 A h NCM811 (3.6 mA h cm⁻²)||Li (20 μm) pouch cells with 2.5 g A h⁻¹ lean electrolyte to achieve 96% capacity retention after 140 cycles. This work represents a deviation from the highly fluorinated electrolyte pathway for LMBs that not only benefits practical and sustainable LMBs but also highlights the possibility of bond design for developing high-performance electrolyte solutions.

中文翻译：

通过坚固的键合设计为高能锂金属电池提供环保电解质

能够在电极上形成阴离子衍生的富含无机的固体电解质界面 (SEI) 并具有广泛的电化学稳定性的电解质创新对于锂金属电池 (LMB) 的商业化至关重要。虽然最近的突破提高了电池的性能，但还没有一种环保且经济的低氟化电解质能够满足实际要求。在此，我们报道了一系列硅氧烷溶剂，其中 Si-O 键同时赋予锂金属负极高相容性和正极高氧化稳定性。在没有任何添加剂/助溶剂的二甲基二甲氧基硅烷电解质中的 1.5 M LiFSI 使锂金属能够实现 99.8% 的高电镀/剥离库仑效率 (CE) 以及高电压 LiNi _0.8 Co _0.1Mn _0.1 O ₂ (NCM811) 和 LiCoO ₂ (LCO) 实现 >99.9% 的高 CE，允许 4.5 V LiCoO ₂ (3 mA h cm ^-2 )||Li (20 μm) 电池在使用后保持 95% 的容量200 次循环和 1.4 A h NCM811 (3.6 mA h cm ^-2 )||Li (20 μm) 软包电池和 2.5 g A h ^-1贫电解液在 140 次循环后实现了 96% 的容量保持率。这项工作代表了对 LMB 的高度氟化电解质途径的偏离，这不仅有利于实用和可持续的 LMB，而且还强调了键设计用于开发高性能电解质溶液的可能性。

更新日期：2022-09-02

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