Bipyridine-integrated bisoxazole-based donor-acceptor covalent organic framework for enhanced photocatalytic H2O2 synthesis

doi:10.1016/S1872-2067(25)64864-9

Abstract

Abstract:

The deliberate integration and precise arrangement of electron donor (D) and acceptor (A) moieties within the crystalline lattices of covalent organic frameworks (COFs) represent a sophisticated strategy to optimize charge separation and electron transfer processes, thereby enhancing photocatalytic efficiency. Herein, we report the rational design and synthesis of two novel bisoxazole-based D-A type COFs, designated as Bpy-COF and Bph-COF. These frameworks incorporate identical acceptor units but are distinguished by their unique donor motifs, enabling a comparative evaluation of their structural and functional properties. The results reveal that Bpy-COF, which incorporates bipyridyl (Bpy) donor moieties, exhibits superior photocatalytic H₂O₂ production performance compared to Bph-COF, potentially related to its broader light response range and increased availability of reactive sites. Furthermore, the coplanar and conjugated nature of the Bpy groups facilitates efficient charge separation and migration, thereby accelerating the two-electron oxygen reduction reaction critical to H₂O₂synthesis. This study affirms the effectiveness of manipulating the structural components of COF photocatalysts, propelling new insights for the design and synthesis of high-performance catalysts.

Key words: Covalent organic frameworks, Donor-acceptor, Photocatalysis, H₂O₂ production, Oxygen reduction reaction

Jiaping Lu, Chao Lin, Chao Li, Hongjie Shi, Nengyi Liu, Wandong Xing, Sibo Wang, Guigang Zhang, Teng-Teng Chen, Xiong Chen. Bipyridine-integrated bisoxazole-based donor-acceptor covalent organic framework for enhanced photocatalytic H₂O₂ synthesis[J]. Chinese Journal of Catalysis, 2026, 81: 185-194.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64864-9

https://www.cjcatal.com/EN/Y2026/V81/I2/185

Figures/Tables 4

Fig. 1. (a) Synthetic routes for Bpy-COF and Bph-COF. The PXRD profiles of Bpy-COF (b) and Bph-COF (c): experimental (red), Pawley refined (dotted green), the difference (black), the simulated curves for eclipsed AA stacking mode (orange) (Insets are the top view (left) and side view (right) of the AA packing mode of Bpy-COF (b) and Bph-COF (c), Grey: C atoms; blue: N atoms; red: O atoms; white: H atoms).

Fig. 2. (a) UV-vis DRS of COFs in the solid state (insets are the optical images of Bph-COF and Bpy-COF). (b) Band alignments of COFs. (c) The reaction photocatalytic activities of COFs within 1 h. (d) The wavelength-dependent of the AQYs of Bpy-COF. (e) Long-term photocatalytic activities of COFs within a 16-h period. (f) Recycling photocatalytic activity of COFs for four 4-h cycles times (total 16 h).

Fig. 3. Estimated exciton binding energy value (a)s and steady-state photoluminescence spectra (b) of COFs (λex = 475 nm). The complete transient absorption (TA) surface and the corresponding TA spectra at selected pump-probe time delays of Bpy-COF (c) and Bph-COF (d) following 435 nm excitation. The break in the region of 700?900 nm is due to the data being recorded in two separate experiments (450?700 nm and > 900 nm). In-situ DRIFTS acquired over different illumination times for the Bpy-COF (e) and Bph-COF (f) photocatalytic systems (1283?933 cm?1), respectively.

Fig. 4. DFT-calculated Gibbs free energy (ΔG, eV) profiles using implicit solvation models for photocatalytic H2O2 production by two-step single-electron reduction route (a) and one-step two-electron reduction route (b). Proposed mechanism for the photocatalytic H2O2 production by two-step single-electron reduction route (c) and one-step two-electron reduction route (d).

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Bipyridine-integrated bisoxazole-based donor-acceptor covalent organic framework for enhanced photocatalytic H₂O₂ synthesis

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