卟啉
光催化
超分子化学
材料科学
光降解
光化学
催化作用
氧化剂
轨道能级差
析氧
超分子组装
可见光谱
分子
物理化学
光电子学
化学
电化学
有机化学
电极
作者
Zijian Zhang,Yongfa Zhu,Xianjie Chen,Hanjie Zhang,Jun Wang
标识
DOI:10.1002/adma.201806626
摘要
A full-spectrum (300-700 nm) responsive porphyrin supramolecular photocatalyst with a theoretical solar spectrum efficiency of 44.4% is successfully constructed. For the first time, hydrogen and oxygen evolution (40.8 and 36.1 µmol g-1 h-1 ) is demonstrated by a porphyrin photocatalyst without the addition of any cocatalysts. The strong oxidizing performance also presents an efficient photodegradation activity that is more than ten times higher than that of g-C3 N4 for the photodegradation of phenol. The high photocatalytic reduction and oxidation activity arises from a strong built-in electric field due to molecular dipoles of electron-trapping groups and the nanocrystalline structure of the supramolecular photocatalyst. The appropriate band structure of the supramolecular photocatalyst adjusted via the highest occupied molecular orbital and lowest unoccupied molecular orbital energy levels of the porphyrin gives rise to thermodynamic driving potential for H2 and O2 evolution under visible light irradiation. Controlling the energy band structure of photocatalysts via the ordered assembly of structure-designed organic molecules could provide a novel approach for the design of organic photocatalysts in energy and environmental applications.
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