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

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

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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.The π-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 hydro-gen bonds(N-H...O)between phenolic hydroxyl groups and the-NH groups of imidazole rings further enhance the structural planarity,resulting in higher π-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 capac-ity(～308 mA h g-1at 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 com-pounds than those without hydroxyl groups attributed to intramolecular hydrogen bond-induced conju-gation enhancement will inspire the structure design of organic electrodes for better energy storage.

BipolarP-phenylenediimidazoleIntramolecular hydrogen bondsPlanarity and conjugation degreeHigh capacity

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

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Institute for Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China

Beijing Institute of Nanoenergy and Nanosystems,Chinese Academy of Sciences,Beijing 101400,China

College of Chemistry,Nankai University,Tianjin 300071,China

School of Materials Science and Engineering,Beihang University,Beijing 100191,China

ShenSi Lab,Shenzhen Institute for Advanced Study,University of Electronic Science and Technology of China,Shenzhen 518110,Guangdong,China

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of Chinathe"Hundred Talents Program"of the Chinese Academy of SciencesFundamental Research Funds for the Central UniversitiesShenzhen Science and Technology ProgramShenzhen Science and Technology ProgramShenzhen Science and Technology ProgramShenzhen Science and Technology ProgramGuangdong Basic and Applied Basic Research Foundation

223710102177101751702009JCYJ20210324115412035JCYJ2021-0324123202008JCYJ20210324122803009ZDSYS202108130955340012021A1515110880

2024

10.1016/j.jechem.2024.05.009

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.96(9)