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首页> 外文期刊>Chemistry: A European journal >An atomic-level strategy for unraveling gold nanocatalysis from the perspective of Au_n(SR)_m nanoclusters
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An atomic-level strategy for unraveling gold nanocatalysis from the perspective of Au_n(SR)_m nanoclusters

机译：从Au_n（SR）_m纳米团簇的角度解开金纳米催化的原子级策略

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摘要

An atomic-level strategy is devised to gain insight into the origin of nanogold catalysis by using atomi- cally monodisperse Au_n(SR) _m nanoclusters as well-defined catalysts for sty- rene oxidation. The Au_n(SR)_m nanoclusters are emerging as a new class of gold nanocatalyst to overcome the polydispersity of conventional nanopar- ticle catalysts. The unique atom-packing structure and electronic properties of Au_n(SR)_m nanoclusters (< 2 nm) are rationalized to be responsible for their extraordinary catalytic activity observed in styrene oxidation. An interesting finding is that quantum size effects of Au _n(SR)_m nanoclusters, rather than the higher specific surface area, play a major role in gold-catalyzed selective oxidation of styrene. For example, Au_(25)(SR)_(18) nanoclusters (≈1 nm) are found to be particularly efficient in activating O_2, which is a key step in styrene oxidation, and hence, the ultra- small Au_(25) catalyst exhibits higher activity than do larger sizes. This atomiclevel strategy has allowed us to obtain an important insight into some fundamental aspects of nanogold catalysis in styrene oxidation. The ultrasmall yet robust Au_n(SR)_m nanoclusters are particularly promising for studying the mechanistic aspects of nanogold catalysis and for future design of better catalysts with high activity and selectivity for certain chemical processes.
机译：通过使用原子性单分散的Au_n（SR）_m纳米簇作为苯乙烯氧化的明确定义的催化剂，设计了一种原子级策略来洞悉纳米金催化的起源。 Au_n（SR）_m纳米团簇正在作为一种新型的金纳米催化剂而出现，以克服常规纳米粒子催化剂的多分散性。 Au_n（SR）_m纳米团簇（<2 nm）的独特原子堆积结构和电子性质被合理化，以归因于其在苯乙烯氧化中观察到的非凡催化活性。一个有趣的发现是Au _n（SR）_m纳米簇的量子尺寸效应，而不是更高的比表面积，在金催化的苯乙烯选择性氧化中起主要作用。例如，发现Au_（25）（SR）_（18）纳米团簇（≈1nm）在激活O_2方面特别有效，这是苯乙烯氧化的关键步骤，因此，超小Au_（25）催化剂比大尺寸催化剂具有更高的活性。这种原子级策略使我们对苯乙烯氧化中纳米金催化的一些基本方面有了重要的了解。超小而坚固的Au_n（SR）_m纳米簇在研究纳米金催化的机理方面以及未来对某些化学过程具有高活性和选择性的更好的催化剂的设计方面特别有希望。

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