Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries

Dry electrode film fabrication technology, known for its environmental friendliness and low energy consumption, is recognized as an effective industrial approach for producing highly dense solid-state electrolytes and pore-free separators. It holds promise for applying thin lithium metal and Li meta...

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Main Authors: Haitao Zhou, Lianlu Wan, Jiacheng Han, Jian-Chun Wu, Yihong Deng, Jie Gu, Huanggang Wang, Hongquan Gao, Zilong Su
Format: Article
Language:English
Published: Elsevier 2025-03-01
Series:Chemical Engineering Journal Advances
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Online Access:http://www.sciencedirect.com/science/article/pii/S266682112400111X
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author Haitao Zhou
Lianlu Wan
Jiacheng Han
Jian-Chun Wu
Yihong Deng
Jie Gu
Huanggang Wang
Hongquan Gao
Zilong Su
author_facet Haitao Zhou
Lianlu Wan
Jiacheng Han
Jian-Chun Wu
Yihong Deng
Jie Gu
Huanggang Wang
Hongquan Gao
Zilong Su
author_sort Haitao Zhou
collection DOAJ
description Dry electrode film fabrication technology, known for its environmental friendliness and low energy consumption, is recognized as an effective industrial approach for producing highly dense solid-state electrolytes and pore-free separators. It holds promise for applying thin lithium metal and Li metal-free anodes in ultra-high energy density Li-ions batteries. However, the films produced by this method suffer from issues such as poor toughness, low strength, uneven thickness, and difficulties in rewinding, which limit its widespread adoption in the large-scale manufacturing of lithium batteries. In this study, we propose a hydrothermal process to introduce a chlorocatechol-based cross-linker onto the surface of highly crystalline polyphenylene sulfide (PPS) powder. By employing the dry electrode process, a PPS-based solid-state separator (PPS-SSS) is fabricated, featuring a thin profile (18±2 μm), a smoother surface, and a denser structure, significantly enhancing its mechanical properties. Moreover, the dense integration structure and chlorocatechol groups contribute to a higher Li+ transference number and more effectively inhibit the growth of Li dendrites. Li metal-free batteries, constructed with this separator, a Sn-plated Cu 10 μm foil anode, and a thick high-nickel cathode dry electrode, exhibit high discharge areal and specific capacities (5 mAh cm−2 and 200 mAh g−1, respectively) and pouch battery device energy density exceeding 440 Wh kg−1. Impressively, even in the presence of Cu or Fe powder contamination on the CuSn foil anode or cathode, this separator can still achieve uniform electric field distribution and lithium deposition, demonstrating good cycle stability.
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spelling doaj-art-4b187bd627ae4462bd5d58e7030f5acf2025-02-03T04:17:01ZengElsevierChemical Engineering Journal Advances2666-82112025-03-0121100694Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteriesHaitao Zhou0Lianlu Wan1Jiacheng Han2Jian-Chun Wu3Yihong Deng4Jie Gu5Huanggang Wang6Hongquan Gao7Zilong Su8School of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR China; Corresponding authors.School of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaSchool of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaSchool of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR China; Corresponding authors.School of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaSchool of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaSchool of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaSchool of Materials Science and Engineering, Jiangsu University, No 301, Xuefu Road, Zhenjiang, Jiangsu Province, 212013, PR ChinaChina Automotive Battery Research Institute Co., Ltd., No.11 Xingke Dong Street, Huairou District, Beijing, 101407, PR China; Corresponding authors.Dry electrode film fabrication technology, known for its environmental friendliness and low energy consumption, is recognized as an effective industrial approach for producing highly dense solid-state electrolytes and pore-free separators. It holds promise for applying thin lithium metal and Li metal-free anodes in ultra-high energy density Li-ions batteries. However, the films produced by this method suffer from issues such as poor toughness, low strength, uneven thickness, and difficulties in rewinding, which limit its widespread adoption in the large-scale manufacturing of lithium batteries. In this study, we propose a hydrothermal process to introduce a chlorocatechol-based cross-linker onto the surface of highly crystalline polyphenylene sulfide (PPS) powder. By employing the dry electrode process, a PPS-based solid-state separator (PPS-SSS) is fabricated, featuring a thin profile (18±2 μm), a smoother surface, and a denser structure, significantly enhancing its mechanical properties. Moreover, the dense integration structure and chlorocatechol groups contribute to a higher Li+ transference number and more effectively inhibit the growth of Li dendrites. Li metal-free batteries, constructed with this separator, a Sn-plated Cu 10 μm foil anode, and a thick high-nickel cathode dry electrode, exhibit high discharge areal and specific capacities (5 mAh cm−2 and 200 mAh g−1, respectively) and pouch battery device energy density exceeding 440 Wh kg−1. Impressively, even in the presence of Cu or Fe powder contamination on the CuSn foil anode or cathode, this separator can still achieve uniform electric field distribution and lithium deposition, demonstrating good cycle stability.http://www.sciencedirect.com/science/article/pii/S266682112400111XSolvent-free dry electrodePolyphenylene sulfideChlorocatecholLi metal-free batterySolid-state separator
spellingShingle Haitao Zhou
Lianlu Wan
Jiacheng Han
Jian-Chun Wu
Yihong Deng
Jie Gu
Huanggang Wang
Hongquan Gao
Zilong Su
Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
Chemical Engineering Journal Advances
Solvent-free dry electrode
Polyphenylene sulfide
Chlorocatechol
Li metal-free battery
Solid-state separator
title Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
title_full Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
title_fullStr Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
title_full_unstemmed Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
title_short Dense integration of chlorocatechols crosslinked polyphenylene sulfide solid-state separator for Li metal-free batteries
title_sort dense integration of chlorocatechols crosslinked polyphenylene sulfide solid state separator for li metal free batteries
topic Solvent-free dry electrode
Polyphenylene sulfide
Chlorocatechol
Li metal-free battery
Solid-state separator
url http://www.sciencedirect.com/science/article/pii/S266682112400111X
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