Ni and Fe Binary Single Atoms on Polyarylether‐Based Covalent Organic Framework for Electrocatalytic Overall Water Splitting

作者：Ying Wen, Wenyan Hu, Fangpei Ma, Qingping Tang, Chao Wu, Siyu Zhu, Xiao Xu, Xiaoling Liu, Yizhong Huang, Shibo Xi, Yu Zhou, Lili Zhang, Jun Wang · 发表于：Small Structures · 年份：2025 · DOI：10.1002/sstr.202500180 · 被引用次数：6 · 研究领域：Advanced Photocatalysis Techniques、Covalent Organic Framework Applications、Electrocatalysts for Energy Conversion

Binary single atoms (SAs) on the covalent organic frameworks (COFs) provide a powerful platform toward effective electrocatalyst for overall water splitting by facilitating the structure modulation and mechanism investigation at atomic level. Herein, the construction of Ni/Fe binary SAs with the configuration of Ni‐(OH) 2 C 2 N 2 +Fe‐(OH) 2 C 2 N 2 on one repeating N≡C–(benzene ring)–C≡N unit of a polyarylether‐based COF (named as HHPN) that was synthesized from the condensation of 2,3,6,7,10,11‐hexahydroxytriphenyl (HHTP) and 2,3,5,6‐tetrafluoro‐1,4‐dicyanobenzene (TFTPN) is demonstrated. The unique Ni/Fe binary SAs configuration on HHPN enhances the charge transfer and allows a high O 2 p band position to accelerate the oxygen evolution reaction (OER). The catalyst exhibits a small OER overpotential of 238 mV at 10 mA cm −2 and a huge mass activity of 2195 A g metal −1 at overpotential 300 mV. An anion exchange membrane water electrolyzer (AEMWE) using NiFe/HHPN as the anode catalyst demonstrates a comparatively low voltage of 1.50 V at 100 mA cm −2 and a duration of over 200 h. This work reveals the great potential of COFs immobilized binary SAs in the rationalization of electrocatalysts.