Constructing Heterogeneous Direct Z-Scheme Photocatalysts Based on Metal-Organic Cages and Graphitic-C3N4 for High-Efficiency Photocatalytic Water Splitting.
Constructing Heterogeneous Direct Z-Scheme Photocatalysts Based on Metal-Organic Cages and Graphitic-C3N4 for High-Efficiency Photocatalytic Water Splitting.
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DOI：
10.1021/acsami.1c03617
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发表时间：
2021-05
影响因子：
9.5
通讯作者：
Su Qin;Yang Lei;Jing Guo;Jian-feng Huang;Chao-Ping Hou;Jun‐Min Liu
中科院分区：
文献类型：
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作者：
Su Qin;Yang Lei;Jing Guo;Jian-feng Huang;Chao-Ping Hou;Jun‐Min Liu
模拟自然界中高效而巧妙的光系统的人工装置的发展值得深入研究。设计了一个金属-有机笼（MOC） Pd2(M-4)4(BF4)4，记为MOC- q1，将四个有机光敏配体M-4和两个Pd2+催化中心整合在一起，用于光化学分子器件（PMD）。通过氢键成功地将MOC-Q1固定在石墨氮化碳（g-C3N4）上，得到了一种坚固的非均相直接z型g-C3N4/MOC-Q1光催化剂，用于可见光下的H2生成。优化后的g-C3N4/MOC-Q1 （2 wt %）体系具有较高的析氢活性（基于催化剂质量为4495 μmol g-1 h-1），且在25 h内表现稳定（基于MOC-Q1的周转次数为19,268），显著优于纯MOC-Q1、g-C3N4和比较材料Pd/g-C3N4/M-4，是目前报道的多相moc基光催化剂中最高的。这种增强可以归因于g-C3N4/MOC-Q1高效的直接z型异质结构带来的高效电子转移、扩大的可见光响应区域和良好的MOC-Q1保护环境的协同效应。合理设计合成的MOC/g- c3n4基非均相PMD在光催化水裂解方面具有很大的潜力。
The development of artificial devices that mimic the highly efficient and ingenious photosystems in nature is worthy of in-depth study. A metal-organic cage (MOC) Pd2(M-4)4(BF4)4, denoted as MOC-Q1, integrating four organic photosensitized ligands M-4 and two Pd2+ catalytic centers is designed for a photochemical molecular device (PMD). MOC-Q1 is successfully immobilized on graphitic carbon nitride (g-C3N4) by hydrogen bonds to obtain a robust heterogeneous direct Z-scheme g-C3N4/MOC-Q1 photocatalyst for H2 generation under visible light. The optimized g-C3N4/MOC-Q1 (2 wt %) system shows high hydrogen evolution activity (4495 μmol g-1 h-1 based on the catalyst mass) and exhibits stable performances for 25 h (a turnover number of 19,268 based on MOC-Q1), significantly outperforming pure MOC-Q1, g-C3N4, and comparsion materials Pd/g-C3N4/M-4, which is the highest one of all reported heterogeneous MOC-based photocatalysts under visible irradiation. This enhancement can be ascribed to the synergistic effects of high-efficient electron transfer, extended visible-light response region, and good protective environment for MOC-Q1 arising from an efficient direct Z-scheme heterostructure of g-C3N4/MOC-Q1. This rationally designed and synthesized MOC/g-C3N4-based heterogeneous PMD is expected to have great potential in photocatalytic water splitting.