Abstract
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. 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.
Original language | English |
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Pages (from-to) | 51806-51814 |
Number of pages | 9 |
Journal | ACS Applied Materials and Interfaces |
Volume | 15 |
Issue number | 44 |
DOIs | |
State | Published - Nov 8 2023 |
Funding
This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC05-00OR22725. Part of this work was conducted at the Center for Nanophase Materials Sciences (CNMS), which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, US Department of Energy, managed by UT-Battelle, LLC, for the United States. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE) and supported by the DOE Office of Fossil Energy. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC05-00OR22725. Part of this work was conducted at the Center for Nanophase Materials Sciences (CNMS), which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, US Department of Energy, managed by UT-Battelle, LLC, for the United States. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE) and supported by the DOE Office of Fossil Energy. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).
Keywords
- atom transfer radical polymerization
- carbon nanosphere
- lithium metal batteries
- particle brush
- poly(ionic liquid)s