Nan Li, Kun Gao, Ke Fan, Li Ma, Zihao Li, Baoluo He, Chao Shen, Qian Ye, Keyu Xie and Haitao Huang
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引用次数: 0
Abstract
Regulating the nanoscale interfacial solvation structure involving ion coordination in the electric double layer is of significant importance for the construction of a stable and rapid ion-transport solid–electrolyte interface for revolutionary lithium metal batteries (LMBs) operated under low-temperature serving conditions. Herein, an efficient strategy involving the use of PMETAC polymer brushes to regulate the nanoscale interfacial solvation structure is proposed, which is universal to different electrolyte chemistries and operating temperatures. Combined attenuated total reflection analysis and theoretical simulations revealed the unique interfacial solvation structure and the underlying synergistic mechanism. Owing to the electrostatic interaction between the quaternary amino nitrogen of the polymer brushes and electrolyte anions, as well as the unique steric hindrance effect originating from the polymer brushes, solvent molecules were excluded from the first inner solvation shell and more anions entered the electric double layer to participate in Li-ion coordination, thus prompting the formation of a stable inorganic-rich SEI with favorable ion transport. With the unique nanoscale interfacial solvation structure, the assembled LMBs achieved stable operation at room temperature for over 1.7 years and at a low temperature of −20 °C. More excitingly, the strategy could support the industrial manufacturing of Ah-level anode-free Li metal pouch cells. This work reveals the importance of regulating the nanoscale interfacial solvation structure, promoting the realistic applications of high-energy LMBs for operation under various service conditions.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).