Closo ‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window

Green, Matthew; Kaydanik, Katty; Orozco, Miguel; Hanna, Lauren; Marple, Maxwell A. T.; Fessler, Kimberly Alicia Strange; Jones, Willis B.; Stavila, Vitalie; Ward, Patrick A.; Teprovich, Jr., Joseph A.

doi:10.1002/advs.202106032

Title: Closo ‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window

Journal Article · Thu Apr 07 00:00:00 UTC 2022 · Advanced Science

DOI: https://doi.org/10.1002/advs.202106032 · OSTI ID:1862050

Green, Matthew ^[1]; Kaydanik, Katty ^[1]; Orozco, Miguel ^[1]; Hanna, Lauren ^[2]; Marple, Maxwell A. T. ^[3]; Fessler, Kimberly Alicia Strange ^[4]; Jones, Willis B. ^[4]; Stavila, Vitalie ^[5]; Ward, Patrick A. ^[2];

^[1]

Department of Chemistry and Biochemistry California State University Northridge 18111 Nordhoff St. Northridge CA 91330 USA
Advanced Manufacturing and Energy Science Savannah River National Laboratory Aiken SC 29803 USA
Physical and Life Sciences Directorate Lawrence Livermore National Laboratory Livermore CA 94551 USA
Spectroscopy Separations and Material Characterization Savannah River National Laboratory Aiken SC 29803 USA
Energy Nanomaterials Sandia National Laboratory Livermore CA 94551 USA

Abstract A major challenge in the pursuit of higher‐energy‐density lithium batteries for carbon‐neutral‐mobility is electrolyte compatibility with a lithium metal electrode. This study demonstrates the robust and stable nature of a closo ‐borate based gel polymer electrolyte (GPE), which enables outstanding electrochemical stability and capacity retention upon extensive cycling. The GPE developed herein has an ionic conductivity of 7.3 × 10 ⁻⁴ S cm ⁻² at room temperature and stability over a wide temperature range from −35 to 80 °C with a high lithium transference number ( = 0.51). Multinuclear nuclear magnetic resonance and Fourier transform infrared are used to understand the solvation environment and interaction between the GPE components. Density functional theory calculations are leveraged to gain additional insight into the coordination environment and support spectroscopic interpretations. The GPE is also established to be a suitable electrolyte for extended cycling with four different active electrode materials when paired with a lithium metal electrode. The GPE can also be incorporated into a flexible battery that is capable of being cut and still functional. The incorporation of a closo ‐borate into a gel polymer matrix represents a new direction for enhancing the electrochemical and physical properties of this class of materials.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Savannah River National Lab (SRNL), Aiken, SC (United States); Savannah River Site (SRS), Aiken, SC (United States)

Sponsoring Organization:: USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Environmental Management (EM)

Grant/Contract Number:: 89303321CEM000080; AC52-07NA27344; NA0003525

OSTI ID:: 1862050

Report Number(s):: LLNL-JRNL-829954; SRNL-STI-2021-00505; 2106032

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 16 Vol. 9; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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PMDETA as an efficient catalyst for bulk reversible complexation mediated polymerization (RCMP) in the absence of additional metal salts and deoxygenation Wang, Wenxiang; Bai, Liangjiu; Chen, Hou RSC Advances, Vol. 6, Issue 99 https://doi.org/10.1039/C6RA20164D	journal	January 2016
Polymer electrolytes for lithium polymer batteries Long, Lizhen; Wang, Shuanjin; Xiao, Min Journal of Materials Chemistry A, Vol. 4, Issue 26 https://doi.org/10.1039/C6TA02621D	journal	January 2016
A highly stable sodium solid-state electrolyte based on a dodeca/deca-borate equimolar mixture Duchêne, L.; Kühnel, R. -S.; Rentsch, D. Chemical Communications, Vol. 53, Issue 30 https://doi.org/10.1039/C7CC00794A	journal	January 2017
Li-Ion solvation in propylene carbonate electrolytes determined by molecular rotational measurements Jiang, Haotian; Zhang, Qi; Zhang, Yutong Physical Chemistry Chemical Physics, Vol. 21, Issue 20 https://doi.org/10.1039/C8CP07552B	journal	January 2019
4 V room-temperature all-solid-state sodium battery enabled by a passivating cathode/hydroborate solid electrolyte interface Asakura, Ryo; Reber, David; Duchêne, Léo Energy & Environmental Science, Vol. 13, Issue 12 https://doi.org/10.1039/D0EE01569E	journal	January 2020
Li2B12H12·7NH3: a new ammine complex for ammonia storage or indirect hydrogen storage Huang, Zhenguo; Gallucci, Judith; Chen, Xuenian Journal of Materials Chemistry, Vol. 20, Issue 14 https://doi.org/10.1039/b923829h	journal	January 2010
Dehydriding reaction of metal hydrides and alkali borohydrides enhanced by microwave irradiation Nakamori, Yuko; Orimo, Shin-ichi; Tsutaoka, Takanori Applied Physics Letters, Vol. 88, Issue 11 https://doi.org/10.1063/1.2185079	journal	March 2006
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Ion Transport Properties of Six Lithium Salts Dissolved in γ-Butyrolactone Studied by Self-Diffusion and Ionic Conductivity Measurements Aihara, Yuichi; Bando, Toshinori; Nakagawa, Hiroe Journal of The Electrochemical Society, Vol. 151, Issue 1 https://doi.org/10.1149/1.1630592	journal	January 2004
Lithium Closoborane Electrolytes Johnson, Jack W. Journal of The Electrochemical Society, Vol. 129, Issue 10 https://doi.org/10.1149/1.2123477	journal	January 1982
Dodekahydro-closo-Dodekaborat-Halogenide der schweren Alkalimetalle mit der Formel M ₃ X[B ₁₂ H ₁₂ ] (M = K – Cs, NH ₄ ; X = Cl und Br) / Dodecahydro-closo-dodecaborate Halides of the Heavy Alkali Metals with the Formula M ₃ X[B ₁₂ H ₁₂ ] (M = K – Cs, NH ₄ ; X = Cl and Br) Tiritiris, Ioannis; Weidlein, Johann; Schleid, Thomas Zeitschrift für Naturforschung B, Vol. 60, Issue 6 https://doi.org/10.1515/znb-2005-0605	journal	June 2005
Infiltrated and Isostatic Laminated NCM and LTO Electrodes with Plastic Crystal Electrolyte Based on Succinonitrile for Lithium-Ion Solid State Batteries Coeler, Matthias; van Laack, Vanessa; Langer, Frederieke Batteries, Vol. 7, Issue 1 https://doi.org/10.3390/batteries7010011	journal	February 2021

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