How Does a Single Pt Nanocatalyst Behave in Two Different Reactions? A Single-Molecule Study

被引：101

作者：

Han, Kyu Sung ^{[1
]}

Liu, Guokun ^{[1
]}

Zhou, Xiaochun ^{[1
]}

Medina, Rita E. ^{[1
]}

Chen, Peng ^{[1
]}

机构：

[1] Cornell Univ, Dept Chem & Biol Chem, Ithaca, NY 14853 USA

来源：

NANO LETTERS | 2012年 / 12卷 / 03期

基金：

美国国家科学基金会;

关键词：

Single-particle catalysis; platinum nanoparticles; single-molecule imaging deacetylation and deoxygenation; structure sensitivity; HETEROGENEOUS CATALYSIS; NANOPARTICLE CATALYSIS; METAL NANOPARTICLES; GOLD NANOPARTICLES; CHEMICAL-REACTIONS; SHAPE CONTROL; NANOCRYSTALS; ELECTROCATALYSIS; CHEMISTRY; SIZE;

D O I：

10.1021/nl203677b

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：1253 / 1259

页数：7

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