Highly conductive polyacrylonitrile-based hybrid aqueous/ionic liquid solid polymer electrolytes with tunable passivation for Li-ion batteries

被引：0

作者：

Ludwig K.B. ^{[1
]}

Correll-Brown R. ^{[1
]}

Freidlin M. ^{[1
]}

Garaga M.N. ^{[2
]}

Bhattacharyya S. ^{[1
]}

Gonzales P.M. ^{[1
]}

Cresce A.V. ^{[3
]}

Greenbaum S. ^{[2
]}

Wang C. ^{[1
]}

Kofinas P. ^{[1
]}

机构：

[1] Department of Chemical & Biomolecular Engineering, University of Maryland, 4418 Stadium Dr., College Park, 20740, MD

[2] Department of Physics & Astronomy, Hunter College of the City University of New York, 695 Park Ave., New York, 10065, NY

[3] Combat Capabilities Development Command US Army Research Laboratory, 2800 Powder Mill Rd., Adelphi, 20783, MD

来源：

Electrochimica Acta | 2023年 / 453卷

基金：

美国国家科学基金会;

关键词：

Aqueous electrolytes; Ionic conductivity; Ionic liquids; Passivation; Polymer electrolytes;

D O I：

10.1016/j.electacta.2023.142349

中图分类号：

学科分类号：

摘要：

The rapid growth in demand for lithium-ion batteries that can deliver more energy and power has generated concerns over safety. Aqueous electrolytes are a strong candidate to alleviate this apprehension, however their ability to overcome the “cathodic challenge” is limited due to anion-dominated passivation at the anode. In this work, the recently developed “hybrid aqueous/nonaqueous” electrolyte (HANE) strategy was employed to tune the degree of passivation at the anode in solid polymer electrolytes (SPEs) by using various ionic liquids as the nonaqueous component. Whereas common HANE systems sacrifice ionic conductivity to create a more robust passivation layer at the cathodic limit, the “hybrid aqueous/ionic liquid” SPEs (HAILSPEs) investigated in this work do not. Two HAILSPE systems (H1, H2.5) were fabricated from a blend of polyacrylonitrile (PAN), water, lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), and either triethylsulfonium-TFSI (S2,2,2) or N-methyl-N-propylpyrrolidinium-TFSI (Pyr1,3). These HAILSPE systems demonstrated a remarkable improvement in transport properties compared to their predecessors, achieving room temperature ionic conductivities of up to 5.39 mS/cm. A reduction in apparent activation energy and nearly complete decoupling of ionic transport from polymer chain mobility were found to contribute to this increase. Stable and complete growth of a passivating layer at 2 V vs. Li/Li+ was also observed, which was tuned by changing the ionic liquid. The work presented here provides a potential route for overcoming the “cathodic challenge” in aqueous SPEs. © 2023 Elsevier Ltd

引用

共 66 条

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