Experimental and computational analysis of the structure-activity relationship of ionic gel electrolytes based on bistrifluoromethanesulfonimide salts for supercapacitors  

作　　者：Wei Chen Ying Wei Xiuling Dong Zhong-Xia Wang Zheng Xing Qingguo Zhang Xiang Liu 

机构地区：[1]College of Chemistry and Materials Engineering,Bohai University,Jinzhou,121013,Liaoning,China [2]College of Chemistry and Chemical Engineering,Gannan Normal University,Ganzhou,341000,Jiangxi,China [3]Institute of Medicine&Chemical Engineering,Zhenjiang College,Zhenjiang,212028,Jiangsu,China

出　　处：《Journal of Materiomics》2024年第6期1222-1233,共12页无机材料学学报（英文）

基　　金：This study was supported by the National Natural Science Foundation of China(22222502);The authors would like to thank the Key Project of the Education Department of Liaoning Province of China(No.LJKZ1010);the Zhenjiang“Jinshan Talents”Project 2021,the Doctoral Foundation of Bohai University(0521bs005);the Innovation Fund Project for Graduate Students of Bohai University(YJC2023-016).

摘　　要：Ionic gel(IG)electrolytes are emerging as promising components for the development of next-generation supercapacitors(SCs),offering benefits in terms of safety,cost-effectiveness,and flexibility.The ionic conductivity,stability,and mechanical properties of the gel electrolyte are relevant factors to be considered and the key to improving the performance of the SC.However,the structure–activity relationship between the internal structure of IGs and their SC properties is not fully understood.In the current study,the intuitive and regular structure–activity relationship between the structure and properties of IGs was revealed via combining computational simulation and experiment.In terms of conductivity,the ionic liquid(IL)([EMIM][TFSI])in the IG has a high self-diffusion coefficient calculated by molecular dynamics simulation(MDS),which is conductive to transfer and then improves the conductivity.The radial distribution function of the MDS shows that the larger the g(r)between the particles in the polymer network,the stronger the interaction.For stability,IGs based on[EMIM][TFSI]and[EOMIM][TFSI]ILs have higher density functional theory calculated binding energy,which is reflected in the excellent thermal stability and excellent capacitor cycle stability.Based on the internal pore size distribution and stress-strain characterization of the gel network([ME3MePy][TFSI]and[BMIM][TFSI]as additives),the highly crosslinked aggregate network significantly reduces the internal mesoporous distribution and plays a leading role in improving the mechanical properties of the network.By using this strategy,it will be possible to design the ideal structure of the IG and achieve excellent performance.

关 键 词：Ionic gel electrolytes Density functional theory Molecular dynamics simulation Self-diffusion coefficient Mean square displacement 

分 类 号：U46[机械工程—车辆工程]