文献类型：期刊文献

英文题名：Quantifying the Partitioning of Vehicular and Structural Lithium Transport in Binary Carbonate Electrolytes

作者：Charnay, Aaron P.[1];Charnay, Benjamin P.[1];Pan, Junkun[1];Zhang, Yan[2];Kanan, Matthew W.[1];Zheng, Weizhong[2];Fayer, Michael D.[1]

机构：[1]Stanford Univ, Dept Chem, Stanford, CA 94305 USA;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn & Low Carbon Technol, Shanghai 200237, Peoples R China

年份：2025

卷号：10

期号：11

起止页码：5885

外文期刊名：ACS ENERGY LETTERS

收录：;EI(收录号：20254419434224);WOS:【SCI-EXPANDED(收录号:WOS:001605889900001)】；

基金：Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-2026822. We thank Dr. Stephen Lynch for assistance with pfg-NMR experiments. A.P.C. and B.P.C. acknowledge the Center for Molecular Analysis and Design (CMAD) for their support.

语种：英文

外文关键词：Binary mixtures - Carbonation - Electrolytes - Infrared spectroscopy - Lithium - Lithium compounds - Lithium-ion batteries - Solvents

摘要：Lithium-ion batteries use mixed-solvent electrolytes, but the effect of solvent composition on the mechanism of lithium-ion transport is not well understood. Here, we quantify the partitioning between vehicular and structural Li+ transport mechanisms for binary mixtures of dimethyl carbonate (DMC) and propylene carbonate (PC) using a combination of 2D infrared spectroscopy and pulsed-field gradient NMR. The primary transport mechanism varies monotonically, with 65% vehicular transport in pure DMC and only 35% vehicular transport in pure PC. Li+ structural step lengths of 1.2-1.5 & Aring; were determined from the experimental data. The outcomes of this study are compared to previously described molecular dynamics simulations. The results presented here indicate that typical carbonate electrolytes cannot tailor structural transport and that new solvent chemistries may be required to enhance this diffusion pathway.