Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 5, Pages 2264-2271Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c10587
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- Office of Vehicle Technologies of the US Department of Energy under the eXtreme Fast Charge Cell Evaluation of Li-ion batteries (XCEL) program [34553]
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This study reveals the significant contribution of entropy change during the Li-ion desolvation process to the measured Li/Li+ electrode potential temperature coefficients. Relationships between electrode potential TCs and Li-ion solvation structures have been established and validated by ab initio molecular dynamics simulations, providing valuable insights for designing future electrolytes for Li-ion/Li metal batteries.
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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