Examining the Electrochemical Properties of Hybrid Aqueous/Ionic Liquid Solid Polymer Electrolytes through the Lens of Composition-Function Relationships

Kyle B. Ludwig; Riordan Correll-Brown; Max FreidlinMounesha N. GaragaSahana BhattacharyyaPatricia M. GonzalesArthur V. CresceSteven GreenbaumChunsheng WangPeter Kofinas

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Examining the Electrochemical Properties of Hybrid Aqueous/Ionic Liquid Solid Polymer Electrolytes through the Lens of Composition-Function Relationships

机译：Examining the Electrochemical Properties of Hybrid Aqueous/Ionic Liquid Solid Polymer Electrolytes through the Lens of Composition-Function Relationships

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Solid polymer electrolytes (SPEs) have the potential to meet evolving Li-ionbattery demands, but for these electrolytes to satisfy growing power andenergy density requirements, both transport properties and electrochemicalstability must be improved. Unfortunately, improvement in one of theseproperties often comes at the expense of the other. To this end, a “hybridaqueous/ionic liquid” SPE (HAILSPE) which incorporatestriethylsulfonium-TFSI (S_(2,2,2)) or N-methyl-N-propylpyrrolidinium-TFSI (Pyr_(1,3))ionic liquid (IL) alongside H_2O and LiTFSI salt to simultaneously improvetransport and electrochemical stability is studied. This work focuses on theimpact of HAILSPE composition on electrochemical performance. Analysisshows that an increase in LiTFSI content results in decreased ionic mobility,while increasing IL and water content can offset its impact. pfg-NMR resultsreveal that preferential lithium-ion transport is present in HAILSPE systems.Higher IL concentrations are correlated with an increased degree ofpassivation against H_2O reduction. Compared to the Pyr_(1,3) systems, the S_(2,2,2)systems exhibit a stronger degree of passivation due to the formation of amulticomponent interphase layer, including LiF, Li_2CO_3, Li2S, and Li_3N. Theresults herein demonstrate the superior electrochemical stability of the S_(2,2,2)systems compared to Pyr_(1,3) and provide a path toward further enhancementof HAILSPE performance via composition optimization.

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《Advanced energy materials》 |2023年第31期|2301428.1-2301428.15|共15页
作者
Kyle B. Ludwig; Riordan Correll-Brown; Max FreidlinMounesha N. GaragaSahana BhattacharyyaPatricia M. GonzalesArthur V. CresceSteven GreenbaumChunsheng WangPeter Kofinas;
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作者单位

Department of Chemical & Biomolecular EngineeringUniversity of Maryland4418 Stadium Dr, College Park, MD 20740, USA;

Department of Physics & AstronomyHunter College of the City University of New York695 Park Ave, New York, NY 10065, USA;

Department of Materials Science & EngineeringUniversity of Maryland4418 Stadium Dr, College Park, MD 20740, USABattery Science Branch, Energy Science Division, Sensors and ElectronDevices DirectorateDEVCOM US Army Research Laboratory2800 Powder Mill Rd, Adelphi, MD 20783, USA;

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all-solid-state batteries; aqueous electrolytes; ionic liquid electrolytes; lithium-ion batteries; solid polymer electrolytes;

Examining the Electrochemical Properties of Hybrid Aqueous/Ionic Liquid Solid Polymer Electrolytes through the Lens of Composition-Function Relationships

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