取代基
催化作用
菲咯啉
钴
螯合作用
氧气
电子供体
共价键
药物化学
化学
三嗪
组合化学
结晶学
无机化学
高分子化学
有机化学
作者
Mei Lv,Cheng‐Xing Cui,Niu Huang,Mingzhu Wu,Qiao Wang,Tao Gao,Yifan Zheng,Wei Liu,Yingping Huang,Hui Li,Tianyi Ma,Liqun Ye
标识
DOI:10.1002/anie.202315802
摘要
The development of nonpyrolytic catalysts featuring precisely defined active sites represents an effective strategy for investigating the fundamental relationship between the catalytic activity of oxygen reduction reaction (ORR) catalysts and their local coordination environments. In this study, we have synthesized a series of model electrocatalysts with well‐defined CoN4 centers and nonplanar symmetric coordination structures. These catalysts were prepared by a sequential process involving the chelation of cobalt salts and 1,10‐phenanthroline‐based ligands with various substituent groups (phen(X), where X = OH, CH3, H, Br, Cl) onto covalent triazine frameworks (CTFs). By modulating the electron‐donating or electron‐withdrawing properties of the substituent groups on the phen‐based ligands, we were able to effectively control the electron density surrounding the CoN4 centers. Our results demonstrated a direct correlation between the catalytic activity of the CoN4 centers and the electron‐donating ability of the substituent group on the phenanthroline ligands. Notably, the catalyst denoted as BCTF‐Co‐phen(OH), featuring the electron‐donating OH group, exhibited the highest ORR catalytic activity. This custom‐crafted catalyst achieved a remarkable half‐wave potential of up to 0.80 V vs. RHE and an impressive turnover frequency (TOF) value of 47.4×10‐3 Hz at 0.80 V vs. RHE in an alkaline environment.
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