Autor: |
Li, Xin-Ao, Tan, Li-Lin, Wang, Xiao-Lin, Liu, Yang, Liang, Zi-Zhan, Huang, Jian-Feng, Xiao, Li-Min, Liu, Jun-Min |
Zdroj: |
Journal of Materials Chemistry A; 12/14/2024, Vol. 12 Issue 46, p32307-32317, 11p |
Abstrakt: |
The construction of Z-scheme heterojunction composite catalysts for overall water splitting is promising. Herein, a triangle-shaped prismatic metal–organic cage MOC-Q3 consisting of two photosensitive ligands and three catalytic Pd2+ centers is synthesized as an intramolecular photocatalytic molecular device (IPMD) to conduct a photocatalytic light-to-fuel reaction. MOC-Q3 is then coupled with graphitic phase carbon nitride (g-C3N4) to form a composite catalyst by intermolecular π–π stacking through quasi-2D/2D contact. And the charge transfers at the MOC-Q3/g-C3N4 interface are proven to follow a Z-scheme pathway by radical trapping experiments and theoretical calculations. The optimized 11 wt% MOC-Q3/g-C3N4 catalyst exhibits a remarkable photocatalytic H2 evolution activity of 50.1 mmol h−1 g−1, one of the highest values reported among g-C3N4-based Z-scheme systems in recent years. And a high turnover number (TON) of 363 740 based on the MOC moles is achieved in a prolonged photocatalytic experiment lasting 32 h. Furthermore, the overall water splitting reaction was successfully conducted using MOC-Q3/g-C3N4 in combination with a classical water oxidation catalyst (WOC) IrO2, without the addition of any sacrificial agent, yielding H2 and O2 amounts of 400.7 and 200.5 μmol g−1 within 5 h, respectively. This study presents an inspiring approach of combining IPMDs and g-C3N4 to prepare highly efficient composite catalysts for visible light-driven H2 evolution and overall water splitting. [ABSTRACT FROM AUTHOR] |
Databáze: |
Complementary Index |
Externí odkaz: |
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