Construction of triazine-based COF/Zr-based MOF S-scheme heterojunctions for efficient photocatalytic H2O2 production under simulated sunlight irradiation
摘要
The anthraquinone method for commercial hydrogen peroxide (H2O2) synthesis is plagued by organic pollution and elevated prices, necessitating the advancement of eco-friendly photocatalytic alternatives. Covalent organic frameworks (COFs) and metal–organic frameworks (MOFs) exhibit potential; yet, they are constrained by inferior charge separation and limited light absorption. Considering triazine-based TFPT-Pa(CH3)2-COF has a distinctive Schiff structure and amino-containing Zr-based MOF (e.g., NH2-UiO-66) has superior visible light absorption and stability, TFPT-Pa(CH3)2/NH2-UiO-66 (COF/MOF) heterojunctions were synthesized by solvothermal methods, and photocatalytic H2O2 production experiments were conducted. The results show that optimum TNU-2 (mass ratio 1:0.5) exhibits a significant H2O2 generation rate of 0.19 mmol g−1 h−1, which is 3.8-fold and 2.4-fold higher than that of pure TFPT-Pa(CH3)2 and NH2-UiO-66, respectively. Furthermore, TNU-2 demonstrates its remarkable cycle stability after five cycles. The radical trapping controlled experiments reveal that the oxygen reduction reaction (ORR) and the water oxidation reaction (WOR) pathways occur simultaneously for the TFPT-Pa(CH3)2/NH2-UiO-66 heterojunction during the H2O2 production process. The constructed COF/MOF S-scheme heterojunction, which creates an internal electric field to promote charge separation, prevent recombination, and preserve strong redox capabilities, is responsible for the enhanced performance. This work offers a novel method for building efficient COF/MOF-based photocatalysts for the production of H2O2.