How do super concentrated electrolytes push the Li-ion batteries and supercapacitors beyond their thermodynamic and electrochemical limits?

Sayah, Simon; Ghosh, Arunabh; Baazizi, Mariam; Amine, Rachid; Dahbi, Mouad; Amine, Youssef; Ghamouss, Fouad; Amine, Khalil

doi:10.1016/j.nanoen.2022.107336

How do super concentrated electrolytes push the Li-ion batteries and supercapacitors beyond their thermodynamic and electrochemical limits?

Journal Article · Wed May 04 00:00:00 EDT 2022 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2022.107336· OSTI ID:1874048

Sayah, Simon ^[1]; Ghosh, Arunabh ^[1]; Baazizi, Mariam ^[2]; Amine, Rachid ^[3]; ^[4]; Amine, Youssef ^[5]; Ghamouss, Fouad ^[2]; Amine, Khalil ^[6]

University of Tours (France)
University of Tours (France); Mohammed VI Polytechnic University, Ben Guerir (Morocco)
Argonne National Lab. (ANL), Lemont, IL (United States)
Mohammed VI Polytechnic University, Ben Guerir (Morocco)
Swiss Federal Institute of Technology, Lausanne (Switzerland)
Mohammed VI Polytechnic University, Ben Guerir (Morocco); Argonne National Lab. (ANL), Lemont, IL (United States); Stanford Univ., CA (United States)

Increasing the energy density of energy storage devices is currently the key target of many battery and supercapacitor research activities. For both types of devices, the electrochemical stability window (ESW) determines the effective energy density of the device. ESWs are defined by the effective oxidation and reduction potentials of the electrolyte, which are controlled by many various factors, including the HOMO/LUMO (highest/lowest unoccupied molecular orbital) energies of the electrolyte molecules, the nature of the electrode/electrolyte interphases, and other physicochemical properties. The concentration of the electrolyte would affect the HOMO/ LUMO levels thus also change the ESW. A higher concentration of salt induces specific arrangements among the anion, cation, and solvent molecules of an electrolyte, altering the bulk behavior of the electrolyte, resulting in drastic change in the electrode interfaces. These uniquely modified physicochemical properties extend the ESW in several different ways, including the enhancement in the kinetic stability of the electrodes, as well as the thermodynamic and Nernst shifts of the oxidation/reduction potentials of the electrolyte. For organic electrolytes, it is the reduced amount of free solvent molecules that plays the key role in such changes; whereas for aqueous electrolytes, it is the scarcity of free water molecules and the reduced water activity that control the key properties of the electrolyte. Here, we focus on elucidating the fundamental structural changes occurring within an electrolyte system with increasing salt concentrations. The underlying mechanisms which not only facilitates the extension of the ESW, but also enables higher rate capabilities and mitigates aluminum dissolution for batteries with organic electrolytes, are meticulously explained. Further, we thoroughly discuss the importance of high-voltage stability in aqueous battery systems by exploiting the changed properties observed with higher concentrations of salts. To finish, high-voltage supercapacitors enabled by superconcentrated electrolytes are also explored.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office. Battery Materials Research (BMR) Program

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1874048

Journal Information:: Nano Energy, Journal Name: Nano Energy Vol. 98; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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High Voltage Stable Li Metal Batteries Enabled by Ether-Based Highly Concentrated Electrolytes at Elevated Temperatures Leng, Yongjun; Ge, Shanhai; Longchamps, Ryan S. Journal of The Electrochemical Society, Vol. 167, Issue 11 https://doi.org/10.1149/1945-7111/aba513	journal	July 2020
Review—Localized High-Concentration Electrolytes for Lithium Batteries Cao, Xia; Jia, Hao; Xu, Wu Journal of The Electrochemical Society, Vol. 168, Issue 1 https://doi.org/10.1149/1945-7111/abd60e	journal	January 2021
Highly Concentrated Electrolytes: Electrochemical and Physicochemical Characteristics of LiPF ₆ in Propylene Carbonate Solutions Åvall, Gustav; Wallenstein, Joachim; Cheng, Gang Journal of The Electrochemical Society, Vol. 168, Issue 5 https://doi.org/10.1149/1945-7111/abfdc3	journal	May 2021
Microporous Carbon-Based Electrical Double Layer Capacitor Operating at High Temperature in Ionic Liquid Electrolyte Largeot, C.; Taberna, P. L.; Gogotsi, Y. Electrochemical and Solid-State Letters, Vol. 14, Issue 12 https://doi.org/10.1149/2.013112esl	journal	January 2011
Corrosion/Passivation Behavior of Concentrated Ionic Liquid Electrolytes and Its Impact on the Li-Ion Battery Performance Liu, Qian; Dzwiniel, Trevor L.; Pupek, Krzysztof Z. Journal of The Electrochemical Society, Vol. 166, Issue 16 https://doi.org/10.1149/2.0161916jes	journal	January 2019
A Guide to Ethylene Carbonate-Free Electrolyte Making for Li-Ion Cells Ma, Lin; Glazier, S. L.; Petibon, R. Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0191701jes	journal	November 2016
Fast Charge/Discharge of Li Metal Batteries Using an Ionic Liquid Electrolyte Yoon, H.; Howlett, P. C.; Best, A. S. Journal of The Electrochemical Society, Vol. 160, Issue 10 https://doi.org/10.1149/2.022310jes	journal	January 2013
Electrolyte Solvation and Ionic Association II. Acetonitrile-Lithium Salt Mixtures: Highly Dissociated Salts Seo, Daniel M.; Borodin, Oleg; Han, Sang-Don Journal of The Electrochemical Society, Vol. 159, Issue 9 https://doi.org/10.1149/2.035209jes	journal	January 2012
LiTFSI Stability in Water and Its Possible Use in Aqueous Lithium-Ion Batteries: pH Dependency, Electrochemical Window and Temperature Stability Lux, S. F.; Terborg, L.; Hachmöller, O. Journal of The Electrochemical Society, Vol. 160, Issue 10 https://doi.org/10.1149/2.039310jes	journal	January 2013
Origin of the Electrochemical Stability of Aqueous Concentrated Electrolyte Solutions Yokoyama, Yuko; Fukutsuka, Tomokazu; Miyazaki, Kohei Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.0491814jes	journal	January 2018
“Water-in-Salt” for Supercapacitors: A Compromise between Voltage, Power Density, Energy Density and Stability Lannelongue, Pierre; Bouchal, Roza; Mourad, Eléonore Journal of The Electrochemical Society, Vol. 165, Issue 3 https://doi.org/10.1149/2.0951803jes	journal	January 2018
A safe and superior propylene carbonate-based electrolyte with high-concentration Li salt Ding, Yuanlei; Yun, Jiaojiao; Liu, Hongmei Pure and Applied Chemistry, Vol. 86, Issue 5 https://doi.org/10.1515/pac-2013-1120	journal	May 2014
Ionic liquids in supercapacitors Brandt, A.; Pohlmann, S.; Varzi, A. MRS Bulletin, Vol. 38, Issue 7 https://doi.org/10.1557/mrs.2013.151	journal	July 2013

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25 ENERGY STORAGE
Electrode-electrolyte interface
High voltage
Lithium based batteries
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Supercapacitors

How do super concentrated electrolytes push the Li-ion batteries and supercapacitors beyond their thermodynamic and electrochemical limits?

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