Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries

Abstract The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials...

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Main Authors: Eun Mi Kim, Jinseok Han, Guk-Tae Kim, Huan Li, Meng Yang Cui, Ganghwan Park, Dong-Ho Baek, Bo Jin, Sang Mun Jeong, Jae-Kwang Kim
Format: Article
Language:English
Published: Nature Portfolio 2024-09-01
Series:NPG Asia Materials
Online Access:https://doi.org/10.1038/s41427-024-00568-2
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author Eun Mi Kim
Jinseok Han
Guk-Tae Kim
Huan Li
Meng Yang Cui
Ganghwan Park
Dong-Ho Baek
Bo Jin
Sang Mun Jeong
Jae-Kwang Kim
author_facet Eun Mi Kim
Jinseok Han
Guk-Tae Kim
Huan Li
Meng Yang Cui
Ganghwan Park
Dong-Ho Baek
Bo Jin
Sang Mun Jeong
Jae-Kwang Kim
author_sort Eun Mi Kim
collection DOAJ
description Abstract The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries.
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spelling doaj-art-ae2420edf4da44478f3fcada24d58d8f2025-01-19T12:28:28ZengNature PortfolioNPG Asia Materials1884-40572024-09-0116111310.1038/s41427-024-00568-2Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteriesEun Mi Kim0Jinseok Han1Guk-Tae Kim2Huan Li3Meng Yang Cui4Ganghwan Park5Dong-Ho Baek6Bo Jin7Sang Mun Jeong8Jae-Kwang Kim9Department of Chemical Engineering, Chungbuk National UniversityDepartment of Energy Convergence Engineering, Cheongju UniversityDepartment of Energy Convergence Engineering, Cheongju UniversitySchool of Materials Science and Engineering, Guilin University of Electronic TechnologyKey Laboratory of Automobile Materials, Ministry of Education, and College of Materials Science and Engineering, Jilin UniversityDepartment of Energy Convergence Engineering, Cheongju UniversityDepartment of Energy Convergence Engineering, Cheongju UniversityKey Laboratory of Automobile Materials, Ministry of Education, and College of Materials Science and Engineering, Jilin UniversityDepartment of Chemical Engineering, Chungbuk National UniversityDepartment of Energy Convergence Engineering, Cheongju UniversityAbstract The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries.https://doi.org/10.1038/s41427-024-00568-2
spellingShingle Eun Mi Kim
Jinseok Han
Guk-Tae Kim
Huan Li
Meng Yang Cui
Ganghwan Park
Dong-Ho Baek
Bo Jin
Sang Mun Jeong
Jae-Kwang Kim
Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
NPG Asia Materials
title Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
title_full Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
title_fullStr Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
title_full_unstemmed Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
title_short Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries
title_sort sulfur reduced graphite oxide and dual anion solid polymer electrolyte integrated structure for high loading practical all solid state lithium sulfur batteries
url https://doi.org/10.1038/s41427-024-00568-2
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