<br>库仑交联支持的两性离子聚合物离子凝胶电解质：碱金属阳离子特性的影响,The Journal of Physical Chemistry B

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库仑交联支持的两性离子聚合物离子凝胶电解质：碱金属阳离子特性的影响
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2024-03-26 , DOI: 10.1021/acs.jpcb.3c08144
Mossab K Alsaedi ₁ , Meron Y Tadesse ₂ , Venkat Ganesan ₂ , Matthew J Panzer ₁

Affiliation

两性离子 (ZI) 聚合物能够在离子液体电解质 (ILE) 内形成非共价交联，从而形成不易燃、机械坚固且高导电性的离子凝胶电解质。在这项研究中，ZI 均聚物聚（2-甲基丙烯酰氧基乙基磷酰胆碱）[聚（MPC）]支架在锂和/或钠盐基 ILE 内原位合成，以构建一系列含有 3 至 15 wt% 聚（ MPC）。发现这些离子凝胶的室温离子电导率值在约 1.3 至 2.2 mS cm ^–1之间变化。对于仅含钠和含有 6 wt% 聚（MPC）的 1:1 锂/钠等摩尔混合盐离子凝胶，由于 ZI 支架的存在，与纯 ILE 相比，离子电导率提高了 14%。此外，比较含锂离子凝胶与含钠离子凝胶的弹性模量值，发现差异高达 1 个数量级 [对于 3 wt% 聚（MPC），分别为 10.6 kPa 与 111 kPa]。离子凝胶前体溶液的分子动力学模拟通过证明所形成的锂/ZI单体和钠/ZI单体簇尺寸分布的差异证实了实验结果，假设这会影响光聚合时获得的支架网络交联密度。这项工作深入了解了为什么与开发更安全的锂离子和钠离子电池电解质相关的 ZI 聚合物支持的离子凝胶特性取决于碱金属阳离子的化学特性。

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Zwitterionic Polymer Ionogel Electrolytes Supported by Coulombic Cross-Links: Impacts of Alkali Metal Cation Identity

Zwitterionic (ZI) polymers enable the formation of noncovalent cross-links within ionic liquid electrolytes (ILEs) to create nonflammable, mechanically robust, and highly conductive ionogel electrolytes. In this study, ZI homopolymer poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] scaffolds are synthesized in situ within lithium and/or sodium salt-based ILEs to construct a series of ionogels that contain between 3 and 15 wt % poly(MPC). Room-temperature ionic conductivity values of these ionogels are found to vary between approximately 1.3 and 2.2 mS cm^–1. For sodium only and 1:1 lithium/sodium equimolar mixed salt ionogels containing 6 wt % poly(MPC), the ionic conductivity is found to improve by 14% compared to the neat ILE due to the presence of the ZI scaffold. Moreover, comparing the elastic modulus values of lithium- versus sodium-containing ionogels revealed a difference of up to 1 order of magnitude [10.6 vs 111 kPa, respectively, for 3 wt % poly(MPC)]. Molecular dynamics simulations of ionogel precursor solutions corroborate the experimental results by demonstrating differences in the lithium/ZI monomer and sodium/ZI monomer cluster size distributions formed, which is hypothesized to influence the scaffold network cross-link density obtained upon photopolymerization. This work provides insights into why ZI polymer-supported ionogel properties that are relevant for the development of safer electrolytes for lithium-ion and sodium-ion batteries depend upon the chemical identity of the alkali metal cation.

更新日期：2024-03-26

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