Uncovering the solid-phase conversion mechanism via a new range of organosulfur polymer composite cathodes for lithium-sulfur batteries

作     者：Xiang Li Dezhong Liu Ziyi Cao Yaqi Liao Zexiao Cheng Jie Chen Kai Yuan Xing Lin Zhen Li Yunhui Huang Lixia Yuan Xiang Li;Dezhong Liu;Ziyi Cao;Yaqi Liao;Zexiao Cheng;Jie Chen;Kai Yuan;Xing Lin;Zhen Li;Yunhui Huang;Lixia Yuan

作者机构：State Key Laboratory of Material Processing and Die&Mold TechnologySchool of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2023年第84卷第9期

页      面：459-466页

核心收录：

学科分类：0808[工学-电气工程] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 

基　　金：supported by the National Science Foundation of China (22075091) the National Science Foundation of Hubei Province (2021CFA066) 

主　　题：Organosulfur polymer Lithium–sulfur batteries Allyl functional groups Reaction mechanism Solid–solid conversion 

摘      要：The sulfur cathodes operating via solid phase conversion of sulfur have natural advantages in suppressing polysulfide dissolution and lowering the electrolyte dosage,and thus realizing significant improvements in both cycle life and energy *** realize an ideal solid-phase conversion of sulfur,a deep understanding of the regulation path of reaction mechanism and a corresponding intentional material and/or cathode design are highly ***,via covalently fixing of sulfur onto the triallyl isocyanurate,a series of S-triallyl isocyanurate organosulfur polymer composites(STIs) are *** between the structure and the electrochemical conversion behavior of STIs is systematically *** is found that the structure of STIs varies with the synthetic temperature,and correspondingly the electrochemical redox of sulfur can be controlled from conventional solid-liquid-solid conversion to the solid-solid *** the STI series,the STI-5 composite realizes an ideal solid-phase conversion and demonstrates great potential for building a Li-S battery with high-energy density and long-cyclelife:it realizes stable cycling over 1000 cycles in carbonate electrolyte,with a degradation rate of0.053% per cycle;the corresponding pouch cell shows almost no capacity decay for 125 cycles under the conditions of high sulfur loading(4.5 mg cm^(-2)) and lean electrolyte(8 μL mg_s^(-1)).In addition,the tailoring strategy of STI can also apply to other precursors with allyl functional groups to develop new organosulfur polymers for solid-solid sulfur *** vulcanized triallyl phosphate(STP) and triallylamine(STA) both show great lithium storage *** strategy successfully develops a new family of organosulfur polymers as cathodes for Li-S batteries via solid-phase conversion of sulfur,and brings insights to the mechanism study in Li-S batteries.