摘要
基于双氧化还原活性有机配体的二维导电金属-有机框架(2D c-MOFs)是极具潜力的锂离子电池(LIBs)电极材料.然而,双配体竞争配位导致该类材料合成具有极大挑战性.本文以乙二胺为调节剂,发展了一步法合成双配体基2D c-MOF Cu_(3)(HHTP)(THQ)(HHTP=2,3,6,7,10,11-六羟基三亚苯,THQ=四羟基-1,4-苯醌).所得Cu_(3)(HHTP)(THQ)具有良好的导电性、丰富的活性位点和优异的化学稳定性,其作为LIBs负极材料展现出高比容量、良好的倍率性能和长循环稳定性.实验结果和理论计算表明,Cu_(3)(HHTP)(THQ)中CuO_(4)活性位点和苯环单元均参与了锂存储,从而优化了储锂性能.该工作为构筑双配体基2D c-MOFs和高性能LIBs电极材料提供了新的途径.
Two-dimensional conductive metal-organic frameworks(2D c-MOFs)are emerging as promising electrode materials for lithium-ion batteries(LIBs).However,2D c-MOFs with binary redox-active organic ligands are rare and suffer from complicated synthesis procedures.Herein,a facile one-step method is developed for the synthesis of a dual-ligand-based 2D c-MOF Cu_(3)(HHTP)(THQ)(HHTP=2,3,6,7,10,11-hexahydroxytriphenylene,THQ=tetrahydroxy-1,4-benzoquinone)by using the ethylenediamine regulator.The resulting Cu_(3)(HHTP)(THQ)possesses good conductivity,abundant active sites,and excellent chemical stability.As an anode material for LIBs,Cu3(HHTP)(THQ)exhibits high specific capacity,good rate performance,and long-term cycling stability.Comprehensive experimental studies and theoretical calculations reveal that CuO_(4)units and aromatic benzene rings in Cu_(3)(HHTP)(THQ)are involved in lithium storage,thereby optimizing the lithium storage performance.This work provides a new way for the construction of dualligand 2D c-MOFs and high-performance LIB electrode materials.
作者
尹佳成
张印强
李志刚
程明仁
刘明
李伟
李娜
卜显和
Jia-Cheng Yin;Yin-Qiang Zhang;Zhi-Gang Li;Mingren Cheng;Ming Liu;Wei Li;Na Li;Xian-He Bu(School of Materials Science and Engineering,National Institute for Advanced Materials,Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry,Nankai University,Tianjin 300350,China;State Key Laboratory of Elemento-Organic Chemistry,College of Chemistry,Nankai University,Tianjin 300071,China)
基金
supported by the National Natural Science Foundation of China(22035003 and 21905142)
the Programme of Introducing Talents of Discipline to Universities(B18030).
