Artificial Photosynthetic Z-scheme Photocatalyst for Hydrogen Evolution with High Quantum Efficiency

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• 作者：Hong-Li Guo ; Hong Du ; Yi-Fan Jiang ; Nan Jiang ; Cong-Cong Shen ; Xiao Zhou ; Ya-Nan Liu ; An-Wu Xu
• 刊名：Journal of Physical Chemistry C
• 出版年：2017
• 出版时间：January 12, 2017
• 年：2017
• 卷：121
• 期：1
• 页码：107-114
• 全文大小：510K
• ISSN：1932-7455

文摘

As global energy consumption continues to rise, it is imperative to develop clean and renewable sources of energy as alternatives to the fossil fuel energy sources. Photocatalytic hydrogen generation or photochemical water splitting is a promising carbon-free technology producing H₂ and O₂ from water. Here, we report an exciting advance in the photocatalytic hydrogen evolution from water under visible light, using newly developed direct Z-scheme heterostructures constructed by oxygen deficient ZnO_1–x nanorods and Zn_0.2Cd_0.8S nanoparticles by calcination. The highest rate for hydrogen production reaches 2518 μmol h^–1 over optimal ZnO_1–x (10 wt %)/Zn_0.2Cd_0.8S Z-scheme photocatalyst with a high apparent quantum efficiency (AQY) of 49.5% at 420 nm, which is 20 times higher than bare Zn_0.2Cd_0.8S and 25 times higher than ZnO_1–x sample. From the results of photocurrent response, electrochemical impedance spectroscopy and time-resolved PL spectra, we demonstrate that the high increase in the photocatalytic hydrogen generation arises from the formation of artificial photosynthetic Z-scheme system and oxygen vacancy abundant ZnO_1–x in the heterojunction. Direct Z-scheme ZnO_1–x/Zn_0.2Cd_0.8S nanoheterostructures result in an efficient charge carrier separation and strong reduction ability for enhanced H₂ production; additionally, the presence of oxygen vacancies in the sample significantly enhances visible light absorption, these synergistic effects lead to highly efficient photocatalytic hydrogen production with an exceptional high quantum efficiency under visible light irradiation. Our findings provide possibilities for creating other high-efficiency photocatalysts mimicking natural photosynthetic Z-scheme system.