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 outs...

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Main Authors: 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 Jr.
Format: Article
Language:English
Published: Wiley 2022-05-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202106032
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author 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 Jr.
author_facet 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 Jr.
author_sort Matthew Green
collection DOAJ
description 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 (tLi+$t_{{ m{Li}}}^ + $ = 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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spelling doaj.art-d12e0dbe593c4902878cbccc1f2e56982022-12-22T02:37:13ZengWileyAdvanced Science2198-38442022-05-01916n/an/a10.1002/advs.202106032Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature WindowMatthew Green0Katty Kaydanik1Miguel Orozco2Lauren Hanna3Maxwell A. T. Marple4Kimberly Alicia Strange Fessler5Willis B. Jones6Vitalie Stavila7Patrick A. Ward8Joseph A. Teprovich Jr.9Department of Chemistry and Biochemistry California State University Northridge 18111 Nordhoff St. Northridge CA 91330 USADepartment of Chemistry and Biochemistry California State University Northridge 18111 Nordhoff St. Northridge CA 91330 USADepartment of Chemistry and Biochemistry California State University Northridge 18111 Nordhoff St. Northridge CA 91330 USAAdvanced Manufacturing and Energy Science Savannah River National Laboratory Aiken SC 29803 USAPhysical and Life Sciences Directorate Lawrence Livermore National Laboratory Livermore CA 94551 USASpectroscopy Separations and Material Characterization Savannah River National Laboratory Aiken SC 29803 USASpectroscopy Separations and Material Characterization Savannah River National Laboratory Aiken SC 29803 USAEnergy Nanomaterials Sandia National Laboratory Livermore CA 94551 USAAdvanced Manufacturing and Energy Science Savannah River National Laboratory Aiken SC 29803 USADepartment of Chemistry and Biochemistry California State University Northridge 18111 Nordhoff St. Northridge CA 91330 USAAbstract 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 (tLi+$t_{{ m{Li}}}^ + $ = 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.https://doi.org/10.1002/advs.202106032electrochromic windowgel polymer electrolytelithium closo‐boratelithium metal electrode
spellingShingle 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 Jr.
Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
Advanced Science
electrochromic window
gel polymer electrolyte
lithium closo‐borate
lithium metal electrode
title Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
title_full Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
title_fullStr Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
title_full_unstemmed Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
title_short Closo‐Borate Gel Polymer Electrolyte with Remarkable Electrochemical Stability and a Wide Operating Temperature Window
title_sort closo borate gel polymer electrolyte with remarkable electrochemical stability and a wide operating temperature window
topic electrochromic window
gel polymer electrolyte
lithium closo‐borate
lithium metal electrode
url https://doi.org/10.1002/advs.202106032
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