Статья

Correlating Li-Ion Solvation Structures and Electrode Potential Temperature Coefficients

Hansen WangDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesSang Cheol KimDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesTomás RojasDepartment of Chemical Engineering, University of Illinois at Chicago, Chicago, Illinois 60607, United StatesYangying ZhuDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesYanbin LiDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesLin MaEnergy & Biotechnology Division, Sensors and Electron Devices Directorate, US Army Research Laboratory, Adelphi, Maryland 20783, United StatesKang XuEnergy & Biotechnology Division, Sensors and Electron Devices Directorate, US Army Research Laboratory, Adelphi, Maryland 20783, United StatesAnh T. NgoDepartment of Chemical Engineering, University of Illinois at Chicago, Chicago, Illinois 60607, United StatesYi CuiDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States

2021en

ABI

Аннотация

Temperature coefficients (TCs) for either electrochemical cell voltages or potentials of individual electrodes have been widely utilized to study the thermal safety and cathode/anode phase changes of lithium (Li)-ion batteries. However, the fundamental significance of single electrode potential TCs is little known. In this work, we discover that the Li-ion desolvation process during Li deposition/intercalation is accompanied by considerable entropy change, which significantly contributes to the measured Li/Li+ electrode potential TCs. To explore this phenomenon, we compare the Li/Li+ electrode potential TCs in a series of electrolyte formulations, where the interaction between Li-ion and solvent molecules occurs at varying strength as a function of both solvent and anion species as well as salt concentrations. As a result, we establish correlations between electrode potential TCs and Li-ion solvation structures and further verify them by ab initio molecular dynamics simulations. We show that measurements of Li/Li+ electrode potential TCs provide valuable knowledge regarding the Li-ion solvation environments and could serve as a screening tool when designing future electrolytes for Li-ion/Li metal batteries.

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Идентификаторы

DOI: 10.1021/jacs.0c10587

Цитирования и источники

Цитирований: 3Использованных источников: 0

Показатели — AkademScholar