Facile Strategy to Prepare Poly(ionic liquid)-Coated Solid Polymer Electrolytes through Layer-by-Layer Assembly

Wang, Zongyu; Thapaliya, Bishnu P.; Popovs, Ilja; Wang, Yangyang; Wang, Tao; Chen, Jihua; Arnould, Mark A.; Mahurin, Shannon M.; Dai, Sheng

doi:10.1021/acsami.3c11418

Title: Facile Strategy to Prepare Poly(ionic liquid)-Coated Solid Polymer Electrolytes through Layer-by-Layer Assembly

Journal Article · 24 October 2023 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.3c11418 · OSTI ID:2217709

Wang, Zongyu ^[1];

^[1];

^[2]; Wang, Tao ^[1]; Chen, Jihua ^[2]; Arnould, Mark A. ^[2];

^[1];

^[3]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); University of Tennessee, Knoxville, TN (United States)

The inability of solid polymer electrolytes to preserve strong mechanical strength with high ionic conductivity hinders the commercialization of lithium metal batteries (LMBs). The success of fabricating layer-by-layer (LbL)-assembled electrolytes has realized the application of flexible solid polymer electrolytes in electrochemical devices. Here, we demonstrate a rational strategy to construct solid electrolytes coated with multiple ultrathin layers of polyanions (poly(sodium 4-styrenesulfonate)) and polycations (linear poly(1-butyl-3-(4-vinylbenzyl)-1H-imidazolium chloride) (BVIC)/linear poly(PEG₄-VIC)/SiO₂-g-poly(PEG₄-VIC)) using an LbL assembly method. Poly(ionic liquid) backbones and PEG side groups are employed to facilitate the transport of lithium ions via the segmental motion of the macromolecular matrix. The fabricated free-standing membranes exhibited good ionic conductivities of 9.03–10 × 10^–4 S cm^–1. Furthermore, a Li/LiFePO₄ cell assembled with the LbL-membrane electrolytes exhibits an initial high discharge capacity of 143–158 mAhg^–1 at 60 °C with high columbic efficiency. In conclusion, this approach, which combines polymer synthesis and LbL self-assembly, is an effective and facile route to fabricate solid polymer electrolyte membranes with superior ionic conductivity and mechanical robustness, which are useful for electrochemical devices and high-voltage battery applications.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Fossil Energy and Carbon Management (FECM)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2217709

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 44 Vol. 15; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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