Determining the Oxidation Stability of Electrolytes for Lithium-Ion Batteries Using Quantum Chemistry and Molecular Dynamics | Sciact - CRIS-система Института катализа

Determining the Oxidation Stability of Electrolytes for Lithium-Ion Batteries Using Quantum Chemistry and Molecular Dynamics Научная публикация

Журнал

Electrochem
ISSN: 2673-3293

Вых. Данные

Год: 2024, Том: 5, Номер: 1, Страницы: 107-123 Страниц : 17 DOI: 10.3390/electrochem5010007

Ключевые слова

liquid electrolytes; lithium-ion batteries; cationic complexes; anionic complexes; molecular dynamics simulation; quantum chemical calculations; oxidative stability of complexes

Авторы

Evshchik Elizaveta Y. ¹ , Borisevich Sophia S. ^1,2 , Ilyina Margarita G. ^2,3 , Khamitov Edward M. ³ , Chernyak Alexander V. ^1,4 , Pugacheva Tatiana A. ¹ , Kolmakov Valery G. ¹ , Bushkova Olga V. ⁵ , Dobrovolsky Yuri A. ^1,6

Организации

1	Federal Research Center for Problems of Chemical Physics and Medical Chemistry RAS, 142432 Chernogolovka, Russia
2	Institute of Intelligent Cybernetic Systems, National Research Nuclear University MEPI, 115409 Moscow, Russia
3	Ufa Institute of Chemistry, Ural Federal Research Center, Russian Academy of Sciences, 450054 Ufa, Russia
4	Scientific Center of the Institute of Solid-State Physics RAS, 142432 Chernogolovka, Russia
5	Institute of Solid State Chemistry, Ural Branch of the Russian Academy of Sciences, 620108 Yekaterinburg, Russia
6	CHT AFC Sistema, 125009 Moscow, Russia

Determining the oxidation potential (OP) of lithium-ion battery (LIB) electrolytes using theoretical methods will significantly speed up and simplify the process of creating a new generation high-voltage battery. The algorithm for calculating OP should be not only accurate but also fast. Our work proposes theoretical principles for evaluating the OP of LIB electrolytes by considering LiDFOB solutions with different salt concentrations in EC/DMC solvent mixtures. The advantage of the new algorithm compared to previous versions of the theoretical determination of the oxidation potential of electrolyte solutions used in lithium-ion batteries for calculations of statistically significant complexes, the structure of which was determined by the molecular dynamics method. This approach significantly reduces the number of atomic–molecular systems whose geometric parameters need to be optimized using quantum chemical methods. Due to this, it is possible to increase the speed of calculations and reduce the power requirements of the computer performing the calculations. The theoretical calculations included a set of approaches based on the methods of classical molecular mechanics and quantum chemistry. To select statistically significant complexes that can make a significant contribution to the stability of the electrochemical system, a thorough analysis of molecular dynamics simulation trajectories was performed. Their geometric parameters (including oxidized forms) were optimized by QM methods. As a result, oxidation potentials were assessed, and their dependence on salt concentration was described. Here, we once again emphasize that it is difficult to obtain, by calculation methods, the absolute OP values that would be equal (or close) to the OP values estimated by experimental methods. Nevertheless, a trend can be identified. The results of theoretical calculations are in full agreement with the experimental ones

Evshchik E.Y. , Borisevich S.S. , Ilyina M.G. , Khamitov E.M. , Chernyak A.V. , Pugacheva T.A. , Kolmakov V.G. , Bushkova O.V. , Dobrovolsky Y.A.
Determining the Oxidation Stability of Electrolytes for Lithium-Ion Batteries Using Quantum Chemistry and Molecular Dynamics
Electrochem. 2024. V.5. N1. P.107-123. DOI: 10.3390/electrochem5010007 OpenAlex

Поступила в редакцию:	9 нояб. 2023 г.
Принята к публикации:	21 февр. 2024 г.
Опубликована в печати:	4 мар. 2024 г.
Опубликована online:	4 мар. 2024 г.

OpenAlex:

W4392382298

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