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在分子尺度上实现碳酸盐与醚的杂化用于高能高安全锂金属电池

Hybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries.

作者信息

Chen Jiawei, Zhang Daoming, Zhu Lei, Liu Mingzhu, Zheng Tianle, Xu Jie, Li Jun, Wang Fei, Wang Yonggang, Dong Xiaoli, Xia Yongyao

机构信息

Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai, 200433, China.

Sinopec Shanghai Research Institute of Petrochemical Technology Co., Ltd., Shanghai, 201208, China.

出版信息

Nat Commun. 2024 Apr 15;15(1):3217. doi: 10.1038/s41467-024-47448-5.

DOI:10.1038/s41467-024-47448-5
PMID:38622141
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11018806/
Abstract

Commonly-used ether and carbonate electrolytes show distinct advantages in active lithium-metal anode and high-voltage cathode, respectively. While these complementary characteristics hold promise for energy-dense lithium metal batteries, such synergy cannot be realized solely through physical blending. Herein, a linear functionalized solvent, bis(2-methoxyethyl) carbonate (BMC), is conceived by intramolecularly hybridizing ethers and carbonates. The integration of the electron-donating ether group with the electron-withdrawing carbonate group can rationalizes the charge distribution, imparting BMC with notable oxidative/reductive stability and relatively weak solvation ability. Furthermore, BMC also offers advantages including the ability to slightly dissolve LiNO, excellent thermostability and nonflammability. Consequently, the optimized BMC-based electrolyte, even with typical concentrations in the single solvent, demonstrates high-voltage tolerance (4.4 V) and impressive Li plating/stripping Coulombic efficiency (99.4%). Moreover, it fulfills practical lithium metal batteries with satisfactory cycling performance and exceptional tolerance towards thermal/mechanical abuse, showcasing its suitability for safe high-energy lithium metal batteries.

摘要

常用的醚类和碳酸酯类电解质分别在活性锂金属负极和高压正极方面展现出显著优势。虽然这些互补特性为高能量密度锂金属电池带来了希望,但这种协同效应无法仅通过物理混合来实现。在此,通过分子内杂化醚类和碳酸酯类设计了一种线性官能化溶剂,双(2-甲氧基乙基)碳酸酯(BMC)。供电子醚基与吸电子碳酸酯基的整合能够使电荷分布合理化,赋予BMC显著的氧化/还原稳定性和相对较弱的溶剂化能力。此外,BMC还具有包括能微溶LiNO、出色的热稳定性和不燃性等优点。因此,即使是单溶剂中典型浓度的优化BMC基电解质也表现出高电压耐受性(4.4 V)和令人印象深刻的锂电镀/剥离库仑效率(99.4%)。此外,它使实用的锂金属电池具有令人满意的循环性能以及对热/机械滥用的出色耐受性,展示了其适用于安全高能量锂金属电池的特性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/224574fcb04b/41467_2024_47448_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/55830fd164ad/41467_2024_47448_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/1cd28a5d35dd/41467_2024_47448_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/464e438061b6/41467_2024_47448_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/ae10fad971b5/41467_2024_47448_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/224574fcb04b/41467_2024_47448_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/55830fd164ad/41467_2024_47448_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/1cd28a5d35dd/41467_2024_47448_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/464e438061b6/41467_2024_47448_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/ae10fad971b5/41467_2024_47448_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a84/11018806/224574fcb04b/41467_2024_47448_Fig5_HTML.jpg

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