Regulating intramolecular hydrogen bonds of p-phenylenediimidazole-based small-molecule compounds towards the enhanced lithium storage capacity  

作　　者：Liping Zheng Bei Wang Jianze Zhang Wenjie Zhou Jiayi Ren Huige Ma Rui Li Chengming Li Mingjun Hu Jun Yang 

机构地区：[1]Institute for Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China [2]Beijing Institute of Nanoenergy and Nanosystems,Chinese Academy of Sciences,Beijing 101400,China [3]College of Chemistry,Nankai University,Tianjin 300071,China [4]School of Materials Science and Engineering,Beihang University,Beijing 100191,China [5]ShenSi Lab,Shenzhen Institute for Advanced Study,University of Electronic Science and Technology of China,Shenzhen 518110,Guangdong,China

出　　处：《Journal of Energy Chemistry》2024年第9期406-413,共8页能源化学（英文版）

基　　金：the financial support by the National Natural Science Foundation of China (22371010, 21771017, and 51702009);the "Hundred Talents Program" of the Chinese Academy of Sciences, the Fundamental Research Funds for the Central Universities;the Shenzhen Science and Technology Program (JCYJ20210324115412035, JCYJ2021-0324123202008, JCYJ20210 324122803009 and ZDSYS20210813095534001);the Guangdong Basic and Applied Basic Research Foundation (2021A1515110880)

摘　　要：The use of redox-active organic electrode materials in energy storage is restricted due to their inferior solvent resistance,abysmal conductivity,and the resultant low practical capacity.To address these issues,a class of bipolar p-phenylenediimidazole-based small-molecule compounds are designed and fabricated.Theπ-conjugated backbone of these small molecules allows for electron delocalization on a big conjugation plane,endowing them with good conductivity and reaction reversibility.Furthermore,when the para-positions of phenylene are occupied by hydroxyl groups,as-formed intramolecular hydrogen bonds(N-H...O)between phenolic hydroxyl groups and the–NH groups of imidazole rings further enhance the structural planarity,resulting in higherπ-conjugation degree and better conductivity,and thus higher utilization of active sites and electrode capacity,proved by both experimental results and theoretical calculations.The optimized composite electrode DBNQ@rGO-45 shows a high specific capacity(∼308 mA h g^(−1)at 100 mA g^(−1))and a long cycling stability(112.9 mA h g^(−1)after 6000 cycles at 2000 mA g^(−1)).The significantly better electrochemical properties for hydroxyl group-containing compounds than those without hydroxyl groups attributed to intramolecular hydrogen bond-induced conjugation enhancement will inspire the structure design of organic electrodes for better energy storage.

关 键 词：Bipolar P-phenylenedimidazole Intramolecular hydrogenbonds Planarity and conjugationd egree High capacity 

分 类 号：TM912[电气工程—电力电子与电力传动] O641.3[理学—物理化学]