Towards high performance polyimide cathode materials for lithium–organic batteries by regulating active-site density, accessibility, and reactivity
Jun Wang,
Haichao Liu,
Chunya Du,
Bing Liu,
Haoran Guan,
Yu Liu,
Shaowei Guan,
Zhenhua Sun,
Hongyan Yao
Affiliations
Jun Wang
National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, Key Laboratory of High Performance Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun 130012, China
Haichao Liu
State Key Lab of Supramolecular Structure and Materials, Jilin University, Changchun 130012, China
Chunya Du
State Key Lab of Supramolecular Structure and Materials, Jilin University, Changchun 130012, China
Bing Liu
National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, Key Laboratory of High Performance Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun 130012, China
Haoran Guan
National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, Key Laboratory of High Performance Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun 130012, China
Yu Liu
College of Sciences, Shenyang University of Chemical Technology, Shenyang 110142, China
Shaowei Guan
National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, Key Laboratory of High Performance Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun 130012, China
Zhenhua Sun
Shenyang National Laboratory for Materials Science Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China; Corresponding authors.
Hongyan Yao
National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, Key Laboratory of High Performance Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun 130012, China; Corresponding authors.
Organic carbonyl electrode materials offer promising prospects for future energy storage systems due to their high theoretical capacity, resource sustainability, and structural diversity. Although much progress has been made in the research of high-performance carbonyl electrode materials, systematic and in-depth studies on the underlying factors affecting their electrochemical properties are rather limited. Herein, five polyimides containing different types of diamine linkers are designed and synthesized as cathode materials for Li-ion batteries. First, the incorporation of carbonyl groups increases the active-site density in both conjugated and non-conjugated systems. Second, increased molecular rigidity can improve the accessibility of the active sites. Third, the introduction of the conjugated structure between two carbonyl groups can increase the reactivity of the active sites. Consequently, the incorporation of carbonyl structures and conjugated structures increases the capacity of polyimides. PTN, PAN, PMN, PSN, and PBN exhibit 212, 198, 199, 151, and 115 mAh g−1 at 50 mA g−1, respectively. In addition, the introduction of a carbonyl structure and a conjugated structure is also beneficial for improving cycling stability and rate performance. This work can deepen the understanding of the structure–function relationship for the rational design of polyimide electrode materials and can be extended to the molecular design of other organic cathode materials.
