@article{Qin2025, 
author = {Na Qin and Yaxiong Huo and Linqiang Li and Diandian Han and Mengyuan Chen and Yanjie Wang and Lipeng Zhai},
title = {N-heterocycle regulation in robust imidazolate covalent organic frameworks for efficient photocatalytic hydrogen peroxide production},
year = {2025},
journal = {Nano Research},
volume = {18},
number = {9},
pages = {94907630},
keywords = {hydrogen peroxide production, photocatalysis, covalent organic frameworks, imidazole linkage, N-heterocycle},
url = {https://www.sciopen.com/article/10.26599/NR.2025.94907630},
doi = {10.26599/NR.2025.94907630},
abstract = {The development of covalent organic frameworks (COFs) with robust linkages is fundamentally important for the photocatalytic production of H2O2. In this work, a series of isostructural COFs with robust imidazole linkage were synthesized as photocatalysts for H2O2 production via the precise N-substituted microenvironment regulation (benzene, pyridine, pyrimidine, and triazine). The corresponding frameworks enable water and dissolved oxygen to reach the catalytic sites easily via planar skeletons and regulation of nitrogen-atom numbers. Additionally, the N-adjustment of heterocycle units in these COFs could significantly regulate the electronic band structures, light-harvesting capacity, and hydrophilic properties. The experimental investigation demonstrated that the photocatalytic process of COFs was composed of a dominant and indirect two-electron (2e−) oxygen reduction reaction (ORR). Notably, compared to H-COF (benzene), P-COF (pyridine), and M-COF (pyrimidine), T-COF with triazine unit exhibited the highest H2O2 production rate of 42,180 μmol·g−1·h−1 due to its wider visible light absorption and higher separation efficiency of photogenerated electron-hole pairs. Theoretical investigations confirmed that N-heterocycle units in COFs could precisely modulate the energy barrier related to the formation of *OOH and *O2. This study is expected to provide a new way for rationally designing imidazole-linked COFs as promising photocatalysts for efficiently photocatalytic H2O2 generation.}
}