Su Long, Gao Xinpei, Mariani Alessandro, Liu Xu, Passerini Stefano, Gao Yanan, Zheng Liqiang
Key Laboratory of Colloid and Interface Chemistry, Shandong University, Ministry of Education, Jinan, 250100, P. R. China.
Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources, Hainan University, No 58, Renmin Avenue, Haikou 570228, P. R. China.
J Phys Chem Lett. 2022 Jan 13;13(1):105-111. doi: 10.1021/acs.jpclett.1c03605. Epub 2021 Dec 28.
Ionic liquids (ILs) are promising designer solvents for multivalent electrolytes, enabling the modulation of molecular-level interactions of solvate species. The molecular mechanism of multivalent-ion clustering and its impact on electrolytes properties is far less studied than that of ion pairs. Herein, we explore the effect of ion clusters on the transport and electrochemical behavior of IL-based electrolytes for Mg batteries. Simulation and small-angle X-ray scattering results indicate that ILs with higher denticity effectively suppress ion agglomeration and parasitic reactions of the Mg electrolytes. Although ion clustering reduces the diffusivity of Mg, the Coulombic efficiency for the reversible Mg deposition/stripping process is improved, highlighting the importance of microstructural and dynamical heterogeneities in the rational design of enhanced multivalent electrolytes.
离子液体（ILs）是用于多价电解质的有前景的定制溶剂，能够调节溶剂化物物种的分子水平相互作用。与离子对相比，多价离子聚集的分子机制及其对电解质性质的影响研究得要少得多。在此，我们探讨离子簇对镁电池中基于离子液体的电解质的传输和电化学行为的影响。模拟和小角X射线散射结果表明，具有更高配位数的离子液体能有效抑制镁电解质的离子团聚和寄生反应。尽管离子簇降低了镁的扩散率，但可逆镁沉积/剥离过程的库仑效率得到了提高，这突出了微观结构和动力学不均匀性在合理设计增强型多价电解质中的重要性。
