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首页> 外文期刊>ACS catalysis >Highly Dispersed RuO2 Hydrates Prepared via Simple Adsorption as Efficient Cocatalysts for Visible-Light-Driven Z-Scheme Water Splitting with an IO3-/I- Redox Mediator
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Highly Dispersed RuO2 Hydrates Prepared via Simple Adsorption as Efficient Cocatalysts for Visible-Light-Driven Z-Scheme Water Splitting with an IO3-/I- Redox Mediator

机译：通过简单的吸附制备的高度分散的RuO2水合物，作为高效助催化剂，用于与IO3- / I-氧化还原介体用IO3- / I-氧化还原介体进行可见光Z样品水分

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摘要

Loading a cocatalyst onto a photocatalyst is a well-known effective way to improve the efficiency of both one-step water splitting and Z-scheme water splitting with a redox mediator. In Z-scheme water splitting systems with an IO3-/I- redox couple, the reduction of IO3- on O-2-evolving photocatalysts via a six-electron process often represents the rate-determining step of the overall process and therefore necessitates effective cocatalysts such as PtOx and RuO2. However, these cocatalysts cannot be loaded onto thermally unstable materials via conventional impregnation processes involving calcination. In the present study, we introduce a Ru-based cocatalyst that can be loaded without calcination and effectively promotes the reduction of IO3- on various photocatalysts, including nonoxide materials. The results reveal that the Ru species adsorbed via simple stirring of photocatalyst particles such as WO3 in an aqueous RuCl3 solution effectively trigger O-2 generation in the presence of IO3- as electron acceptor; moreover, the O-2 evolution rate on the present Ru-loaded WO3 sample was much higher than that on WO3 loaded with conventional RuO2. The structural analysis indicates that the Ru species adsorbed on WO3 are highly dispersed and characterized by octahedral RuO6 environments similar to those found in RuO2 center dot nH(2)O. It was confirmed that the loaded Ru species (most likely analogous to RuO2-nH(2)O) exhibit higher activity in the reduction of IO3- than anhydrous RuO2, whereas RuO2 exhibits much higher activity for the oxidation of water than RuO2 center dot nH(2)O. The developed Ru-based cocatalyst was also applicable to thermally unstable materials such as H2WO4 and Ta3N5, thus enabling them to generate O-2 in the presence of IO3-.
机译：将助催化剂加载到光催化剂上是一种有效的方法，可以通过氧化还原介体提高一步水分裂和Z方案水分裂的效率。在Z样品用IO3 / I-氧化还原耦合的水分裂系统中，通过六电子过程的IO3 - 在O-2演化光催化剂上的还原通常代表整个过程的速率确定步骤，因此需要有效Ptox和Ruo2等助催化剂。然而，这些助催化剂不能通过涉及煅烧的常规浸渍方法加载到热不稳定材料上。在本研究中，我们介绍了可以在没有煅烧的情况下装载的Ru基助催化剂，并有效地促进在各种光催化剂上的IO3减少，包括非氧化物。结果表明，通过简单地搅拌的Ru物种在水性RuCl 3溶液中的简单搅拌如WO3，有效地触发IO3-作为电子受体的存在;此外，目前Ru加载的WO3样品上的O-2演化率远高于常规RuO2的WO3上的o-2进化率。结构分析表明，在WO3上吸附的Ru物种高度分散，其特征在于八面体Ru6环境，其类似于Ruo2中心点NH（2）O中的那些。被证实已加载的Ru物种（最有可能类似于RuO 2-NH（2））的物质表现出更高的活性在减少IO3-比无水RuO 2的减少，而Ruo2表现出比Ruo2中心点NH的水氧化更高的活性（2）o。研制的Ru基助催化剂也适用于热不稳定的材料，例如H 2 O 4和Ta3N5，因此使它们能够在IO3-存在下产生O-2。

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