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

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

doi:10.1002/advs.202106032

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

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

Materials & Chemistry Group

Research output: Contribution to journal › Article › peer-review

25 Scopus citations

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 ((Formula presented.) = 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.

Original language	English
Article number	2106032
Journal	Advanced Science
Volume	9
Issue number	16
DOIs	https://doi.org/10.1002/advs.202106032
State	Published - Jun 3 2022

Funding

Initial results were supported by a CSUN Research, Scholarship, and Creative Activity (RSCA) award. Subsequent experiments and results were supported by the National Science Foundation under Grant No. 2137973 (LEAPS-MPS). The collaboration between CSUN, SNL, and LLNL was supported in part by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS) under the Visiting Faculty Program (VFP). A portion of this work was supported by the Laboratory Directed Research and Development (LDRD) program within the Savannah River National Laboratory (SRNL). This work was produced by Battelle Savannah River Alliance, LLC under Contract No. 89303321CEM000080 with the U.S. Department of Energy. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under Contract No. DE-NA-0003525. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344 LLNL-JRNL-829954. Publisher acknowledges the U.S. Government license to provide public access under the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). Initial results were supported by a CSUN Research, Scholarship, and Creative Activity (RSCA) award. Subsequent experiments and results were supported by the National Science Foundation under Grant No. 2137973 (LEAPS\u2010MPS). The collaboration between CSUN, SNL, and LLNL was supported in part by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS) under the Visiting Faculty Program (VFP). A portion of this work was supported by the Laboratory Directed Research and Development (LDRD) program within the Savannah River National Laboratory (SRNL). This work was produced by Battelle Savannah River Alliance, LLC under Contract No. 89303321CEM000080 with the U.S. Department of Energy. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under Contract No. DE\u2010NA\u20100003525. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE\u2010AC52\u201007NA27344 LLNL\u2010JRNL\u2010829954. Publisher acknowledges the U.S. Government license to provide public access under the DOE Public Access Plan ( http://energy.gov/downloads/doe\u2010public\u2010access\u2010plan ).

Keywords

electrochromic window
gel polymer electrolyte
lithium closo-borate
lithium metal electrode

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10.1002/advs.202106032

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title = "Closo-Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window",

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 ((Formula presented.) = 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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AU - Hanna, Lauren

AU - Marple, Maxwell A.T.

AU - Fessler, Kimberly Alicia Strange

AU - Jones, Willis B.

AU - Stavila, Vitalie

AU - Ward, Patrick A.

AU - Teprovich, Joseph A.

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N2 - 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 ((Formula presented.) = 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.

AB - 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 ((Formula presented.) = 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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Closo-Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window

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