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DOI | 10.1073/pnas.2004576117 |
Designing electrolytes with polymerlike glass-forming properties and fast ion transport at low temperatures | |
Zhao Q.; Liu X.; Zheng J.; Deng Y.; Warren A.; Zhang Q.; Archer L. | |
发表日期 | 2020 |
ISSN | 0027-8424 |
起始页码 | 26053 |
结束页码 | 26060 |
卷号 | 117期号:42 |
英文摘要 | In the presence of Lewis acid salts, the cyclic ether, dioxolane (DOL), is known to undergo ring-opening polymerization inside electrochemical cells to form solid-state polymer batteries with good interfacial charge-transport properties. Here we report that LiNO3, which is unable to ring-open DOL, possesses a previously unknown ability to coordinate with and strain DOL molecules in bulk liquids, completely arresting their crystallization. The strained DOL electrolytes exhibit physical properties analogous to amorphous polymers, including a prominent glass transition, elevated moduli, and low activation entropy for ion transport, but manifest unusually high, liquidlike ionic conductivities (e.g., 1 mS/cm) at temperatures as low as -50 °C. Systematic electrochemical studies reveal that the electrolytes also promote reversible cycling of Li metal anodes with high Coulombic efficiency (CE) on both conventional planar substrates (1 mAh/cm2 over 1,000 cycles with 99.1% CE; 3 mAh/cm2over 300 cycles with 99.2% CE) and unconventional, nonplanar/three-dimensional (3D) substrates (10 mAh/cm2over 100 cycles with 99.3% CE). Our finding that LiNO3promotes reversibility of Li metal electrodes in liquid DOL electrolytes by a physical mechanism provides a possible solution to a longstanding puzzle in the field about the versatility of LiNO3salt additives for enhancing reversibility of Li metal electrodes in essentially any aprotic liquid electrolyte solvent. As a first step toward understanding practical benefits of these findings, we create functional Lijjlithium iron phosphate (LFP) batteries in which LFP cathodes with high capacity (5 to 10 mAh/cm2) are paired with thin (50 μm) lithium metal anodes, and investigate their galvanostatic electrochemical cycling behaviors. © 2020 National Academy of Sciences. All rights reserved. |
英文关键词 | Coupled dynamics; Electrolytes; Ion transport; Lithium batteries; Thermal transition |
语种 | 英语 |
scopus关键词 | electrolyte; lithium; lithium nitrate; polymer; solvent; unclassified drug; Article; conductance; controlled study; crystallization; dynamics; electrochemical analysis; ion transport; low temperature; priority journal; thermal analysis |
来源期刊 | Proceedings of the National Academy of Sciences of the United States of America |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/160207 |
作者单位 | Zhao, Q., Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States; Liu, X., Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States; Zheng, J., Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, United States; Deng, Y., Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, United States; Warren, A., Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States; Zhang, Q., Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States; Archer, L., Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States, Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, United States |
推荐引用方式 GB/T 7714 | Zhao Q.,Liu X.,Zheng J.,et al. Designing electrolytes with polymerlike glass-forming properties and fast ion transport at low temperatures[J],2020,117(42). |
APA | Zhao Q..,Liu X..,Zheng J..,Deng Y..,Warren A..,...&Archer L..(2020).Designing electrolytes with polymerlike glass-forming properties and fast ion transport at low temperatures.Proceedings of the National Academy of Sciences of the United States of America,117(42). |
MLA | Zhao Q.,et al."Designing electrolytes with polymerlike glass-forming properties and fast ion transport at low temperatures".Proceedings of the National Academy of Sciences of the United States of America 117.42(2020). |
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