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Interrogating reactions of gold nanoclusters: insights into catalysis and the Brust-Schiffrin synthesis




Dreier, Timothy Andrew, author
Ackerson, Christopher J., advisor
Kennan, Alan J., committee member
Henry, Charles, committee member
Peebles, Christie, committee member

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Over the past several decades, interest in the synthesis and behavior of atomically precise gold nanoclusters has gained substantial momentum. Herein, both catalytic behavior and synthetic mechanisms are explored using techniques more typically applied to organic chemistry. In the case of catalysis, Au25(SR)18 has emerged as a well-studied model system. In an effort to investigate their potential as intact, homogeneous, unsupported catalysts, we have discovered that Au25(SR)18 clusters are not stable in oxidizing conditions reported for catalytic styrene oxidation. Further investigation suggests that the active catalytic species is an Au(I) species resulting from oxidative decomposition of the starting gold cluster. Equally important to chemical behavior is an understanding of the reaction dynamics during the synthesis of atomically precise clusters. Because the Brust-Schiffrin method is the standard procedure by which gold nanoclusters are synthesized, the role of oxygen in it has been investigated for both organic and aqueous systems. In either case, it is clear obtaining the desired product depends on a radically mediated etching step. These results give new insight into how the Brust-Schiffrin method might be modified to further synthesis of uniquely interesting nanocluster systems.


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