期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202310847
关键词
Conductive Metal-Organic Framework; H2O2 Production; O-2 Reduction; Photocatalysis; Single-Atom Catalysis
In this study, a strongly coupled hybrid photocatalyst consisting of polymeric carbon nitride (CN) and a two-dimensional conductive Zn-containing metal-organic framework (Zn-MOF) was reported. The catalytic capability of Zn-MOF for H2O2 production was unlocked by annealing-induced effects. The annealing treatment not only activated the Zn sites in Zn-MOF to a relatively electron-rich state but also facilitated photoelectron migration from the CN photocatalyst to the Zn-MOF catalytic unit, resulting in significantly enhanced H2O2 production activity and excellent stability.
Developing highly efficient catalytic sites for O-2 reduction to H2O2, while ensuring the fast injection of energetic electrons into these sites, is crucial for artificial H2O2 photosynthesis but remains challenging. Herein, we report a strongly coupled hybrid photocatalyst comprising polymeric carbon nitride (CN) and a two-dimensional conductive Zn-containing metal-organic framework (Zn-MOF) (denoted as CN/Zn-MOF(lc)/400; lc, low crystallinity; 400, annealing temperature in ?), in which the catalytic capability of Zn-MOF(lc) for H2O2 production is unlocked by the annealing-induced effects. As revealed by experimental and theoretical calculation results, the Zn sites coordinated to four O (Zn-O4) in Zn-MOF(lc) are thermally activated to a relatively electron-rich state due to the annealing-induced local structure shrinkage, which favors the formation of a key *OOH intermediate of 2e(-) O-2 reduction on these sites. Moreover, the annealing treatment facilitates the photoelectron migration from the CN photocatalyst to the Zn-MOF(lc) catalytic unit. As a result, the optimized catalyst exhibits dramatically enhanced H2O2 production activity and excellent stability under visible light irradiation.
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