文献类型：期刊文献

英文题名：Hydrogen bonding network induced by ambipolar small molecules facilitates high-performance all-solid-state Li batteries

作者：Li, Jing[1];Chai, Ruiqi[2];Sun, Yaping[2];Wang, Hengyi[1];Lian, Cheng[1,2];Su, Haiping[2];Li, Jingkun[2];Liu, Honglai[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：530

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20260519987021);WOS:【SCI-EXPANDED(收录号:WOS:001682455700001)】；

基金：This work was financially supported by the National Key Research and Development Program of China (2022YFA1503501) , the National Natural Science Foundation of China (No. 22278127, 52321002, 22078088, 22102114) , the Fundamental Research Funds for the Central Universities (No. 2022ZFJH004) .

语种：英文

外文关键词：All-solid-state lithium batteries; solid-state polymer electrolytes; polyethylene oxide; short-straight-chain primary amide; hydrogen bonding network

摘要：The flexible and easy-to-process qualities of polyethylene oxide (PEO) make it one of the most promising candidates for next generation all-solid-state lithium batteries (ASSLBs). However, the insufficient Li+ transport kinetics and electrochemical stability of PEO limit its rate and cycling performances. In this work, we introduce short-straight-chain primary amide (SSPA) with ambipolar properties into PEO-based solid-state polymer electrolytes (SPEs) to construct hydrogen bonding network. The hydrogen bonding network not only loosens the PEO matrix, but also modulates the Li+ coordination microenvironment to promote Li salt dissociation, weaken Li+- EO interaction, and shorten Li+ transport pathway, thereby tailoring Li+ transport kinetics and electrode/electrolyte interface. Additionally, the hydrogen bonding strength is optimized by regulating the alkyl chain length of SSPA, achieving superior performance in LiFePO4-based ASSLB with a high initial specific capacity of 166.0 mAh (g-)1 and a long cycle-life of over 500 cycles with a capacity retention of 85.2% at 0.5C. This work highlights the critical role of hydrogen bonding network induced by ambipolar small molecules on regulating Li+ transport properties and electrode/electrolyte interfacial stability, providing a promising strategy for high-safety/energydensity ASSLBs.