Cao Dong, Wang Jiayi, Xu Haoxiang, Cheng Daojian
State Key Laboratory of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Small. 2021 Aug;17(31):e2101163. doi: 10.1002/smll.202101163. Epub 2021 Jul 2.
Rationally integrating multi-active sites into one ideal catalyst is an effective approach to accelerate multistep reactions by synergic catalysis. Herein, a universal and facile room temperature impregnation strategy is developed to construct Ru atomically dispersed catalyst (Ru ADC) with Ru-C single atoms and Ru oxide nanoclusters (≈1.5 nm), which can also be extended to prepare Ir, Rh, Pt, Au, and Mo atomically dispersed catalysts (ADCs). It is found that the obtained Ru ADC largely boosts alkali hydrogen evolution by concerted catalysis between single atoms and sub-nanoclusters, which only needs an overpotential of 18 mV at 10 mA cm . Further mechanistic studies reveal that Ru-C single atoms and Ru oxide nanoclusters with Ru-O configuration in one catalyst can synergically boost water molecule capture, water dissociation, and hydrogen release. This study opens up a simple method to synthesize dual-site metal ADCs for synergic catalysis of typical multistep reactions.
将多个活性位点合理整合到一个理想的催化剂中是通过协同催化加速多步反应的有效方法。在此，开发了一种通用且简便的室温浸渍策略来构建具有Ru-C单原子和Ru氧化物纳米团簇（≈1.5 nm）的Ru原子分散催化剂（Ru ADC），该策略也可扩展用于制备Ir、Rh、Pt、Au和Mo原子分散催化剂（ADC）。研究发现，所制备的Ru ADC通过单原子与亚纳米团簇之间的协同催化极大地促进了碱性析氢反应，在10 mA cm 时仅需18 mV的过电位。进一步的机理研究表明，一种催化剂中具有Ru-O构型的Ru-C单原子和Ru氧化物纳米团簇可以协同促进水分子捕获、水分解和氢气释放。该研究开辟了一种合成双位点金属ADC的简单方法，用于典型多步反应的协同催化。
