Modifying Ionogel Solid-Electrolytes for Complex Electrochemical Systems

Ashby, David S.; Cardenas, Jorge; Bhandarkar, Austin Suhas; Cook, Adam W.; Talin, A. Alec

doi:10.1021/acsaem.2c02085

Modifying Ionogel Solid-Electrolytes for Complex Electrochemical Systems

Journal Article · Mon Oct 03 00:00:00 EDT 2022 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.2c02085· OSTI ID:1894602

^[1]; Cardenas, Jorge ^[2]; Bhandarkar, Austin Suhas ^[1]; Cook, Adam W. ^[2]; ^[1]

Sandia National Laboratories (SNL-CA), Livermore, CA (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

The solution processability of ionogel solid electrolytes has recently garnered attention in the Li-ion battery community as a means to address the interface and fabrication issues commonly associated with most solid electrolytes. However, the trapped ionic liquid (ILE) component has hindered the electrochemical performance. In this report we present a process to tune the properties by replacing the ILE in a silica-based ionogel after fabrication with a liquid component befitting the desired application. Electrochemical cycling under various conditions showcases gels containing different liquid components incorporated into LiFePO4 (LFP)/gel/Li cells: high power (455 W kg^–1 at a 1 C discharge) systems using carbonates, low temperatures (-40 °C) using ethers, or high temperatures (100 °C) using ionic liquids. Fabrication of additive-manufactured cells utilizing the exchanged carbonate-based system is demonstrated in a planar LFP/Li₄Ti₅O₁₂ (LTO) system, where a marked improvement over an ionogel is found in terms of rate capability, capacity, and cycle stability (118 vs 41 mA h g^–1 at C/4). This process represents a promising route to create a separator-less cell, potentially in complex architectures, where the electrolyte properties can be facilely tuned to meet the required conditions for a wide range of battery chemistries while maintaining a uniform electrolyte access throughout cast electrodes.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-CA), Livermore, CA (United States); Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: NA0003525

OSTI ID:: 1894602

Report Number(s):: SAND2022-13226J; 710291

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 10 Vol. 5; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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