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Polymer-based electrolytes for all-solid-state lithium–sulfur batteries: from fundamental research to performance improvement

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Abstract

With the increasing demand for a higher energy density and a lower cost energy storage system, lithium–sulfur batteries have become one of the promising candidates to replace current Li-ion batteries. However, in liquid electrolyte systems, the lithium dendrite growth and the shuttle effect cause severe safety hazard as well as capacity decay, which hinders the commercialization of practical lithium–sulfur batteries. Polymer-based electrolytes provide a promising solution to these challenges. This type of electrolyte, including polymer and composite polymer electrolytes, demonstrates the capabilities to prevent polysulfide dissolution and suppress lithium dendrite growths, while ensuring good surface contact and high flame resistance. This review summarizes the most recent progress of polymer-based all-solid-state lithium–sulfur batteries (ASSLSB), which revealed mechanisms and challenges of electrolyte ionic conductivity, reaction mechanism, anode/electrolyte interface, and cathode/electrolyte interface. Based on these revealed principles, possible solutions to these challenges such as the addition of inorganic fillers, interface modification, utilization of different types of lithium salt and polymers are introduced. In addition, the state-of-the-art approaches with great performance improvement are highlighted in this review. Finally, we provide perspectives on research directions that can further the understanding and development of polymer-based ASSLSB.

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Figure 1
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Reproduced with permission from ref. [28], Copyright 2015, Royal Society of Chemistry

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Reproduced with permission from ref. [64], Copyright 2016, Elsevier Ltd. c Schematic illustration of the fast-ionic conduction pathway along the space charge regions. Reproduced with permission from ref. [65], Copyright 2018, American Chemical Society

Figure 5

Reproduced with permission from ref. [48], Copyright 2016, Elsevier B.V

Figure 6

Reproduced with permission from ref. [102], Copyright 2020, WILEY‐VCH

Figure 7

Reproduced with permission from ref. [105], Copyright 2006 Elsevier Ltd. b SEM images of lithium metal deposited onto bare stainless steel substrate in the electrolyte. i With the addition of only LiNO3 (1 wt%) and ii with the addition of both Li2S8 (0.18 M) and LiNO3 (1 wt%). (Scale bars in b, 20 μm.) Reproduced with permission from ref. [106], Copyright 2015, Nature Publishing Group

Figure 8

Reproduced with permission from ref. [107], Copyright 2017, American Chemical Society. c, d Top view c and cross-section view d of Li anode surface cycled with PEO/LiTFSI electrolyte. Reproduced with permission from ref. [108], Copyright 2019, American Chemical Society

Figure 9

Reproduced with permission from ref. [118], Copyright 2016, the Author(s)

Figure 10

Reproduced with permission from ref. [128], Copyright 2018, American Chemical Society

Figure 11

Reproduced with permission from ref. [135], Copyright 2018, WILEY‐VCH. b Schematic of the electrochemical deposition behavior of the Li metal anode with (left) the PLL solid electrolyte with immobilized anions and (right) the routine liquid electrolyte with mobile anions. c SEM images of Li metal plating on Cu foils with the presence of PEO-LiTFSI-LLZTO (PLL) and routine liquid electrolytes (1 M LiPF6-EC/DEC). (Scale bars in c, 10 μm.) Reproduced with permission from ref. [132], Copyright 2017, PNAS

Figure 12

Reproduced with permission from ref. [139], Copyright 2002, Elsevier Science B.V. c Synthesis route of PEG grafted graphene oxide cathode (GO-PEG@C/S). Reproduced with permission from ref. [144], Copyright 2017, Royal Society of Chemistry

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Acknowledgements

This work was supported in initial draft writing as part of the Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DESC0001160 and continued in manuscript writing and discussions supported by the U.S.-Israel Energy Center program managed by the U.S.-Israel Binational Industrial Research and Development (BIRD) Foundation.

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    Shoukang Hong, Yang Wang, Nam Kim & Sang Bok Lee

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Hong, S., Wang, Y., Kim, N. et al. Polymer-based electrolytes for all-solid-state lithium–sulfur batteries: from fundamental research to performance improvement. J Mater Sci 56, 8358–8382 (2021). https://doi.org/10.1007/s10853-021-05832-2

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