Engineering cyano groups into hydrogen-bonded organic supramolecules with multi redox centers for high-performance Li-ion battery cathode

作者：Wu, Yong; Wang, Yifan; Wei, Facai; Zhang, Tingting; Li, Wenda; Huang, Lingyan; Qi, Ruijuan; Fu, Jianwei; Jing, Chengbin; Cheng, Jiangong; Liu, Shaohua^*

来源：Energy Storage Materials, 2023, 63: 102993.

DOI：10.1016/j.ensm.2023.102993

• Hydrogen -bond
• Supramolecules
• Organic cathode
• Lithium -ion batteries

Bottom-up molecular engineering by rational design has emerged as a promising strategy for exploring advanced organic cathodes. However, directly programming organic moieties into high-performance electro-active materials remains a great challenge. Herein, we design and synthesize a hydrogen-bonded supramolecule (hexaazatrinaphthalene hexacarbonitrile, HATN-6CN) anchored with abundant cyano groups, which ensures structural stability, extended pi-conjugated system, and multiple redox active centers. As a result, the HATN-6CN cathode delivers a high specific capacity (297.6 mAh g-1 at 0.5 A g-1, 225.2 mAh g-1 at 5 A g-1) and outstanding long-term cycling performance (191.9 mAh g-1 over 1000 cycles at 5 A g-1 with a capacity retention of 85.2 %). Moreover, the charge storage mechanisms, structural evolution, and reversibility during the redox process of HATN-6CN were systematically investigated. This work offers a feasible and promising avenue for bottom-up molecular engineering of organic electrodes by rational design.

• 单位
  中国科学院; 浙江大学; 郑州大学