Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, USA.
Nano Lett. 2012 Mar 14;12(3):1253-9. doi: 10.1021/nl203677b. Epub 2012 Jan 30.
Using single-molecule microscopy of fluorogenic reactions we studied Pt nanoparticle catalysis at single-particle, single-turnover resolution for two reactions: one an oxidative N-deacetylation and the other a reductive N-deoxygenation. These Pt nanoparticles show distinct catalytic kinetics in these two reactions: one following noncompetitive reactant adsorption and the other following competitive reactant adsorption. In both reactions, single nanoparticles exhibit temporal activity fluctuations attributable to dominantly spontaneous surface restructuring. Depending on the reaction sequence, single Pt nanoparticles may or may not show activity correlations in catalyzing both reactions, reflecting the structure insensitivity of the N-deacetylation reaction and the structure sensitivity of the N-deoxygenation reaction.
我们使用荧光反应的单分子显微镜，在单粒子、单转换分辨率下研究了铂纳米粒子催化的两种反应：一种是氧化 N-去乙酰化反应，另一种是还原 N-脱氧反应。这些铂纳米粒子在这两种反应中表现出明显不同的催化动力学：一种遵循非竞争性反应物吸附，另一种遵循竞争性反应物吸附。在这两种反应中，单个纳米粒子表现出归因于主要自发表面重构的时间活性波动。根据反应顺序，单个 Pt 纳米粒子在催化这两种反应时可能表现出或不表现出活性相关性，这反映了 N-去乙酰化反应的结构不敏感性和 N-脱氧反应的结构敏感性。
