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Achieving overall water splitting on plasmon-based solid Z-scheme photocatalysts free of redox mediators
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-09-14 , DOI: 10.1016/j.jcat.2017.08.018
Shengyang Wang , Yuying Gao , Yu Qi , Ailong Li , Fengtao Fan , Can Li

Plasmonic photocatalysis is one of the potential approaches for solar hydrogen production, but successful construction of plasmonic photocatalysts for overall water splitting (OWS) is still a challenge. In this work, we achieved OWS by developing a plasmon-based solid Z-scheme photocatalytic system. Firstly, visible-light responsive plasmonic photocatalysts (Au/TiO2) was demonstrated as a stable and efficient photocatalyst for water oxidation half reaction. When Au/TiO2 was combined with a H2-evolution photocatalyst, i.e. Rh doped SrTiO3 (SrTiO3:Rh), hydrogen and oxygen evolution in a stoichiometric ratio (2:1) were achieved under visible light irradiation without using any redox mediator. In addition, the charge separation process in the plasmonic Z-scheme system is studied through employing photoassisted Kelvin probe force microscopy (KPFM) technology and we demonstrated that the plasmon-induced hot electrons can be transferred to SrTiO3:Rh through a solid interface. At last, the mechanism of plasmon induced solid Z-scheme system was proposed, in which Au nanoparticles play both as visible light absorber and electron conductor. These results give us an alternative way to efficiently utilize both the hot electrons and holes from plasmon effects in an integrated plasmonic solid photocatalyst.



中文翻译:

在不含氧化还原介体的基于等离激元的固态Z方案光催化剂上实现总水分解

等离子体光催化是产生太阳能氢的潜在方法之一,但是成功构建用于整体水分解(OWS)的等离子体光催化剂仍然是一个挑战。在这项工作中,我们通过开发基于等离激元的固态Z方案光催化系统实现了OWS。首先,可见光响应型等离激元光催化剂(Au / TiO 2)被证明是一种稳定有效的水氧化半反应光催化剂。当Au / TiO 2与H 2演化型光催化剂结合时,即Rh掺杂的SrTiO 3(SrTiO 3:Rh),在可见光辐照下不使用任何氧化还原介体,以化学计量比(2:1)释放出氢气和氧气。此外,通过使用光辅助开尔文探针力显微镜(KPFM)技术研究了等离子体Z方案系统中的电荷分离过程,并且我们证明了等离子体诱导的热电子可以通过固体界面转移到SrTiO 3:Rh中。最后,提出了等离激元诱导的固体Z-方案体系的机理,其中金纳米颗粒同时起着可见光吸收剂和电子导体的作用。这些结果为我们提供了一种替代方法,可以在集成的等离激元固体光催化剂中有效利用等离激元效应产生的热电子和空穴。

更新日期:2017-09-14
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