QC and MD Modelling for Predicting the Electrochemical Stability Window of Electrolytes: New Estimating Algorithm
Source abstract
Abstract
The electrolyte is an important component of lithium-ion batteries, especially when it comes to cycling high-voltage cathode materials. In this paper, we propose an algorithm for estimating both the oxidising and reducing potential of electrolytes using molecular dynamics and quantum chemistry techniques. This algorithm can help to determine the composition and structure of the solvate complexes formed when a salt is dissolved in a mixture of solvents. To develop and confirm the efficiency of the algorithm, LiBF4 solutions in binary mixtures of ethylene carbonate (EC)/dimethyl carbonate (DMC) and sulfolane (SL)/dimethyl carbonate (DMC) were studied. The structure and composition of the complexes formed in these systems were determined according to molecular dynamics. Quantum chemical estimation of the thermodynamic and oxidative stability of solvate complexes made it possible to establish which complexes make the most significant contribution to the electrochemical stability of the electrolyte system. This method can also be used to determine the additive value of the oxidation and reduction potentials of the electrolyte, along with the contribution of each complex to the overall stability of the electrolyte. Theoretical calculations were confirmed experimentally in the course of studying electrolytes by step-by-step polarisation using inert electrodes. Thus, the main aim of the study is to demonstrate the possibility of using the developed algorithm to select the optimal composition and solvent ratio to achieve predicted redox stability.
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Research context
OpenAlex topics: Advanced Battery Technologies Research · Advancements in Battery Materials · Advanced Battery Materials and Technologies
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
CHT AFC Sistema, 125009 Moscow, Russia
Federal Research Center for Problems of Chemical Physics and Medical Chemistry RAS, 142432 Chernogolovka, Russia
Ufa Institute of Chemistry, Ural Federal Research Center, Russian Academy of Sciences, 450054 Ufa, Russia
Institute of Cyber Intelligence Systems, National Research Nuclear University MEPhI, 115409 Moscow, Russia
Center of Bio- and Chemoinformatics, First Moscow State Medical University I. M. Sechenov, 119048 Moscow, Russia
Institute of Solid-State Chemistry, Ural Branch of the Russian Academy of Sciences, 620108 Yekaterinburg, Russia
Funding
Russian Science Foundation
References (92)
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