Nat Mater. 2011 Oct 23;11(1):49-52. doi: 10.1038/nmat3143.
Catalysis using gold is emerging as an important field of research in connection with 'green' chemistry. Several hypotheses have been presented to explain the markedly high activities of Au catalysts. So far, the origin of the catalytic activities of supported Au catalysts can be assigned to the perimeter interfaces between Au nanoclusters and the support. However, the genesis of the catalytic activities of colloidal Au-based bimetallic nanoclusters is unclear. Moreover, it is still a challenge to synthesize Au-based colloidal catalysts with high activity. Here we now present the 'crown-jewel' concept (Supplementary Fig. S1) for preparation of catalytically highly Au-based colloidal catalysts. Au-Pd colloidal catalysts containing an abundance of top (vertex or corner) Au atoms were synthesized according to the strategy on a large scale. Our results indicate that the genesis of the high activity of the catalysts could be ascribed to the presence of negatively charged top Au atoms.
使用金进行催化作为与“绿色”化学有关的一个重要研究领域正在兴起。已经提出了几个假设来解释 Au 催化剂的显著高活性。到目前为止,负载 Au 催化剂的催化活性的起源可以归因于 Au 纳米簇与载体之间的边界界面。然而,胶体 Au 基双金属纳米簇的催化活性的起源尚不清楚。此外,合成具有高活性的基于 Au 的胶体催化剂仍然是一个挑战。在这里,我们现在提出了用于制备催化活性高的基于 Au 的胶体催化剂的“皇冠上的宝石”概念(补充图 S1)。根据该策略,在大规模上合成了含有丰富的顶(顶点或角)Au 原子的 Au-Pd 胶体催化剂。我们的结果表明,催化剂的高活性的起源可以归因于带负电荷的顶 Au 原子的存在。