Breaking interfacial Lithium-Ion conduction barriers by a Small-Molecule blocker of interfacial reactions for All-Solid-State Lithium-Sulfur batteries

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2025-04-01 DOI:10.1016/j.cej.2025.162077

Congying Song, Jian Gao, Han Shen, Zhongqiang Wang, Fang Li, Guoxing Li

{"title":"Breaking interfacial Lithium-Ion conduction barriers by a Small-Molecule blocker of interfacial reactions for All-Solid-State Lithium-Sulfur batteries","authors":"Congying Song, Jian Gao, Han Shen, Zhongqiang Wang, Fang Li, Guoxing Li","doi":"10.1016/j.cej.2025.162077","DOIUrl":null,"url":null,"abstract":"The decomposition of Li6PS5Cl at polyethylene oxide-Li6PS5Cl (PEO-Li6PS5Cl) interface is the intrinsic factor restricting the lithium-ion (Li+) transport in PEO-Li6PS5Cl-based composite solid polymer electrolyte (PL-CSE). Here, a small molecule-induced interface-reaction blocking strategy is proposed to suppress the decomposition of Li6PS5Cl and significantly improve the Li+ conductivity of PL-CSE. C-propylpyrogallol[4]arene (PgC3) with unique structure is designed to serve as a small-molecule blocker of interfacial reactions to active the interfacial Li+ transport. The abundant hydrogen bonds between PgC3 and PEO not only accelerate the Li+ transport in PEO phase but also weaken the nucleophilic attack of PEO to Li6PS5Cl, thus inhibiting the decomposition of Li6PS5Cl and breaking the Li+ transport barriers at the PEO-Li6PS5Cl interface. The unique electrostatic potential and bowl-shaped configuration of PgC3 also induce an attraction to the anions, which promotes the dissociation of Li salts. Benefiting from these features, the PL-CSE containing PgC3 (PPL-CSE) exhibits a high Li+ conductivity of 1.93 × 10-4 S cm−1 (35 ℃). The PPL-CSE-based Li‖Li symmetric cell shows an outstanding stability with a lifespan over 14000 h. The assembled all-solid-state lithium-sulfur battery also delivers a high specific capacity of 1012mAh g−1 and stable cycling performance at 0.1C.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"75 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.162077","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}

引用次数: 0

Abstract

The decomposition of Li₆PS₅Cl at polyethylene oxide-Li₆PS₅Cl (PEO-Li₆PS₅Cl) interface is the intrinsic factor restricting the lithium-ion (Li⁺) transport in PEO-Li₆PS₅Cl-based composite solid polymer electrolyte (PL-CSE). Here, a small molecule-induced interface-reaction blocking strategy is proposed to suppress the decomposition of Li₆PS₅Cl and significantly improve the Li⁺ conductivity of PL-CSE. C-propylpyrogallol[4]arene (PgC₃) with unique structure is designed to serve as a small-molecule blocker of interfacial reactions to active the interfacial Li⁺ transport. The abundant hydrogen bonds between PgC₃ and PEO not only accelerate the Li⁺ transport in PEO phase but also weaken the nucleophilic attack of PEO to Li₆PS₅Cl, thus inhibiting the decomposition of Li₆PS₅Cl and breaking the Li⁺ transport barriers at the PEO-Li₆PS₅Cl interface. The unique electrostatic potential and bowl-shaped configuration of PgC₃ also induce an attraction to the anions, which promotes the dissociation of Li salts. Benefiting from these features, the PL-CSE containing PgC₃ (PPL-CSE) exhibits a high Li⁺ conductivity of 1.93 × 10^-4 S cm⁻¹ (35 ℃). The PPL-CSE-based Li‖Li symmetric cell shows an outstanding stability with a lifespan over 14000 h. The assembled all-solid-state lithium-sulfur battery also delivers a high specific capacity of 1012mAh g⁻¹ and stable cycling performance at 0.1C.

Abstract Image

查看原文本刊更多论文

求助全文

约1分钟内获得全文求助全文

来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.