Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C3N4 to dramatically enhance photocatalytic hydrogen evolution
Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C3N4 to dramatically enhance photocatalytic hydrogen evolution
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DOI：
10.1016/s1872-2067(22)64109-3
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发表时间：
2022-08-01
影响因子：
16.5
通讯作者：
Liu, Jun-Min
中科院分区：
文献类型：
--
作者：
Lei, Yang;Huang, Jian-Feng;Liu, Jun-Min
The rational design of photochemical molecular device (PMD) and its hybrid system has great po-tential in improving the activity of photocatalytic hydrogen production. A series of Pd6L3type met-al-organic cages, denoted as MOC-Py-M (M = H, Cu, and Zn), are designed for PMDs by combining metalloporphyrin-based ligands with catalytically active Pd2+ centers. These metal-organic cages (MOCs) are first successfully hybridized with graphitic carbon nitride (g-C3N4) to form direct Z-scheme heterogeneous MOC-Py-M/g-C3N4 (M = H, Cu, and Zn) photocatalysts via pi-pi interactions. Benefiting from its better light absorption ability, the MOC-Py-Zn/g-C3N4 catalyst exhibits high H-2 production activity under visible light (10348 mu mol g(-1) h(-1)), far superior to MOC-Py-H/g-C3N4 and MOC-Py-Cu/g-C3N4. Moreover, the MOC-Py-Zn/g-C3N4 system obtains an enhanced turn over num-ber (TON) value of 32616 within 100 h, outperforming the homogenous MOC-Py-Zn (TON of 507 within 100 h), which is one of the highest photochemical hybrid systems based on MOC for visi-ble-light-driven hydrogen generation. This confirms the direct Z-scheme heterostructure can pro-mote effective charge transfer, expand the visible light absorption region, and protect the cages from decomposition in MOC-Py-Zn/g-C3N4. This work presents a creative example that direct Z-scheme PMD-based systems for effective and persistent hydrogen generation from water under visible light are obtained by heterogenization approach using homogeneous porphyrin-based MOCs and g-C3N4 semiconductors. (C) 2022, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
