Regulating Intramolecular Electron Transfer of Nickel‐Based Coordinations through Ligand Engineering for Aqueous Batteries

作者：Yichun Su, Jinliang Hu, Guoqiang Yuan, Guangxun Zhang, Wenxian Wei, Yangyang Sun, Xiaoxing Zhang, Zheng Liu, Nian‐Tzu Suen, Hsiao‐Chien Chen, Huan Pang · 发表于：Advanced Materials · 年份：2023 · DOI：10.1002/adma.202307003 · 被引用次数：100 · 研究领域：Advanced battery technologies research、Electrocatalysts for Energy Conversion、Advancements in Battery Materials

Abstract The integration of electronic effects into complexes for the construction of novel materials has not yet attracted significant attention in the field of energy storage. In the current study, eight one‐dimensional (1D) nickel‐based salicylic acid complexes (Ni‐XSAs, X = p H, p Me, p MeO, m Me, p Br, p Cl, p F, and p CF 3 ), are prepared by ligand engineering. The coordination environments in the Ni–XSAs are explored using X‐ray absorption fine structure spectroscopy. The charge transfer of the complexes is modulated according to the difference in the electron‐donating ability of the substituents, in combination with frontier orbital theory. Furthermore, density functional theory is used to investigate the effect of the substituent position on the electronic properties of the complexes. Ni‐ m MeSA exhibits better electrical conductivity than Ni‐ p MeSA. The electrochemical performance of Ni‐ m MeSA as an aqueous battery cathode is remarkably improved with a maximum energy density of 0.30 mWh cm −2 (125 Wh kg −1 ) and a peak power density of 33.72 mW cm −2 (14.03 kW kg −1 ). This study provides ideas for the application of new coordination chemistry in the field of energy materials science.