Polyimide covalent organic frameworks as efficient solid-state Li^(+) electrolytes  

作　　者：Xu Liu Shi Wang Siqi Liu Chengfang Liu Xiangchun Li Jian Wu Dazhi Li Shihao Xu Chongyang Liu Wen-Yong Lai 

机构地区：[1]State Key Laboratory of Organic Electronics and Information Displays(SKLOEID),Institute of Advanced Materials(IAM),School of Chemistry and Life Sciences,Nanjing University of Posts&Telecommunications,Nanjing 210023,China

出　　处：《Science China Chemistry》2024年第5期1647-1652,共6页中国科学（化学英文版）

基　　金：supported by National Key R&D Program of China (2023YFB3608904);the National Natural Science Foundation of China (62004106, 62274097, 21835003, 62005126);the Natural Science Foundation of Jiangsu Province (BE2019120,BK20210601);the Foundation of Key Laboratory of Flexible Electronics of Zhejiang Province (2023FE002);Program for Jiangsu Specially-Appointed Professors (RK030STP15001);the Excellent Scientific and Technological Innovative Teams of Jiangsu Higher Education Institutions (TJ217038);the Six Talent Peaks Project of Jiangsu Province (TD-XCL-009);the 333 Project of Jiangsu Province (BRA2017402);the Project of State Key Laboratory of Organic Electronics and Information Displays,NJUPT (GZR2023-010016);Natural Science Foundation of NJUPT (NY223079)。

摘　　要：Covalent organic frameworks(COFs) are attractive porous crystalline materials with extremely high stability, easy functionalization, and open channels, which are expected to be unique ion conductors/transporters in lithium ion batteries(LIBs). Despite recent advances, low ion conductivity and low transference number, resulting in low charging/discharging rate, low energy density, and short battery life, are the main issues that limit their direct application as solid electrolytes in LIBs. Here, we designed and synthesized a novel polyimide COF, namely, TAPA-PDI-COF, with abundant C=O groups, which has been successfully employed as high-performance solid electrolytes by doping TAPA-PDI-COF and succinonitrile(SN). Both the well-defined nanochannels of COFs and SN confined in the well-aligned channels restricted the free migration of anions, while C=O on COFs and CN groups of SN enhanced Li^(+) transport, thus achieving a high ion conductivity of 0.102 m S cm^(-1)at 80 °C and a high lithium-ion transference number of 0.855 at room temperature. According to density functional theory(DFT)calculations, Li-ion migration mainly adopted in-plane transport rather than the axial pathway, which may be due to the shorter hopping distances in the planar pathway. The results suggest an effective strategy for the design and development of all-solidstate ionic conductors for achieving high-performance LIBs.

关 键 词：lithium ion batteries(LIBs) covalent organic frameworks(COFs) solid-state ion conductors solid-state electrolytes ion conductivity 

分 类 号：TM912[电气工程—电力电子与电力传动] O646.1[理学—物理化学]