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用于高效可见光驱动光催化产氢的金属有机框架衍生的ZnO/ZnS异质纳米结构

Metal-Organic Framework-Derived ZnO/ZnS Heteronanostructures for Efficient Visible-Light-Driven Photocatalytic Hydrogen Production.

作者信息

Zhao Xiuxia, Feng Jianrui, Liu Jingwei, Lu Jia, Shi Wei, Yang Guangming, Wang Guichang, Feng Pingyun, Cheng Peng

机构信息

College of Chemistry and Key Laboratory of Advanced Energy Materials Chemistry (MOE) Nankai University Tianjin 300071 China.

Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin 300071 China.

出版信息

Adv Sci (Weinh). 2018 Jan 3;5(4):1700590. doi: 10.1002/advs.201700590. eCollection 2018 Apr.

Abstract

Developing highly active, recyclable, and inexpensive photocatalysts for hydrogen evolution reaction (HER) under visible light is significant for the direct conversion of solar energy into chemical fuels for various green energy applications. For such applications, it is very challenging but vitally important for a photocatalyst to simultaneously enhance the visible-light absorption and suppress photogenerated electron-hole recombination, while also to maintain high stability and recyclability. Herein, a metal-organic framework (MOF)-templated strategy has been developed to prepare heterostructured nanocatalysts with superior photocatalytic HER activity. Very uniquely, the synthesized photocatalytic materials can be recycled easily after use to restore the initial photocatalytic activity. It is shown that by controlling the calcination temperature and time with MOF-5 as a host and guest thioacetamide as a sulfur source, the chemical compositions of the formed heterojunctions of ZnO/ZnS can be tuned to further enhance the visible-light absorption and photocatalytic activity. The nanoscale heterojunction ZnO/ZnS structural feature serves to reduce the average free path of charge carriers and improve the charge separation efficiency, thus leading to significantly enhanced HER activity under visible-light irradiation (λ > 420 nm) with high stability and recyclability without any cocatalyst.

摘要

开发用于可见光下析氢反应(HER)的高活性、可回收且廉价的光催化剂,对于将太阳能直接转化为化学燃料以用于各种绿色能源应用具有重要意义。对于此类应用而言,光催化剂要同时增强可见光吸收并抑制光生电子 - 空穴复合,同时还要保持高稳定性和可回收性,这极具挑战性但至关重要。在此,已开发出一种金属有机框架(MOF)模板策略来制备具有优异光催化HER活性的异质结构纳米催化剂。非常独特的是,合成的光催化材料在使用后可轻松回收以恢复其初始光催化活性。结果表明,以MOF - 5为主体、客体硫代乙酰胺为硫源,通过控制煅烧温度和时间,可以调节形成的ZnO/ZnS异质结的化学组成,以进一步增强可见光吸收和光催化活性。纳米级异质结ZnO/ZnS结构特征有助于降低电荷载流子的平均自由程并提高电荷分离效率,从而在可见光照射(λ > 420 nm)下显著增强HER活性,且具有高稳定性和可回收性,无需任何助催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b7fb/5908348/247bfb7bbd29/ADVS-5-1700590-g001.jpg

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