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首页> 外文期刊>Chemistry: A European journal >In situ formation of Au-Pd bimetallic active sites promoting the physically mixed monometallic catalysts in the liquid-phase oxidation of alcohols
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In situ formation of Au-Pd bimetallic active sites promoting the physically mixed monometallic catalysts in the liquid-phase oxidation of alcohols

机译：原位形成Au-Pd双金属活性位，促进醇液相氧化中物理混合的单金属催化剂

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The catalytic oxidation of alcohols with molecular oxygen on supported nanometallic catalysts represents one of the green methods in a crucial process for the synthesis of fine chemicals. We have designed an experiment using physically mixed Au/AC and Pd/AC (AC=activated carbon) as the catalyst in the liquid-phase oxidation of benzyl alcohol by aerobic oxygen. The evolution of the physically mixed catalyst structures at different stages in the catalytic reaction was investigated by aberration-corrected high-resolution transmission electron microscopy and spatially resolved element mapping techniques at the nanometre scale, and they were also compared with the structure of the bimetallic alloy. For the first time we show the formation of surface Au-Pd bimetallic sites by reprecipitation of Pd onto Au nanoparticles. Negligible Au leaching was observed. The in situ structural evolution can be directly correlated to the great enhancement of the catalyst activity. Moreover, we distinguish the different behaviours of Au and Pd, thus suggesting an oxygen differentiating mechanism for Au and Pd sites. The findings are of great importance to both the understanding of the structure-activity correlation and the design of highly active catalysts in green chemistry.
机译：在载体化的纳米金属催化剂上用分子氧催化醇的氧化代表了精细化学品合成的关键过程中的绿色方法之一。我们设计了一个实验，使用物理混合的Au / AC和Pd / AC（AC =活性炭）作为催化剂，通过好氧将苯甲醇液相氧化。通过像差校正高分辨率透射电子显微镜和空间分辨元素图谱技术研究了纳米混合催化剂结构在催化反应不同阶段的演变，并将其与双金属合金的结构进行了比较。 。我们首次展示了通过将Pd再沉淀到Au纳米颗粒上而形成的表面Au-Pd双金属位点。观察到可忽略的金浸出。原位结构演变可以直接与催化剂活性的大大提高相关。此外，我们区分了Au和Pd的不同行为，从而提出了Au和Pd位置的氧区分机制。这些发现对绿色化学中结构活性相关性的理解和高活性催化剂的设计均具有重要意义。

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