Single-Molecule Kinetics of Nanoparticle Catalysis

被引:41
|
作者
Xu, Weilin [1 ]
Shen, Hao [1 ]
Liu, Guokun [1 ]
Chen, Peng [1 ]
机构
[1] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA
基金
美国国家科学基金会;
关键词
Single-nanoparticle catalysis; single-molecule fluorescence detection; Langmuir Hinshelwood mechanism; reactivity heterogeneity; parallel reaction pathways; differential selectivity; DYNAMIC DISORDER; ENZYME MOLECULES; DIHYDROFOLATE-REDUCTASE; FLUCTUATING ENZYMES; SHAPE CONTROL; NANOCRYSTALS; ELECTROCHEMISTRY; HYDROLYSIS; ENZYMOLOGY; REACTIVITY;
D O I
10.1007/s12274-009-9100-1
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Owing to their structural dispersion, the catalytic properties of nanoparticles are challenging to characterize in ensemble-averaged measurements. The single-molecule approach enables studying the catalysis of nanoparticles at the single-particle level with real-time single-turnover resolution. This article reviews our single-molecule fluorescence studies of single Au-nanoparticle catalysis, focusing on the theoretical formulations for extracting quantitative reaction kinetics from the single-turnover resolution catalysis trajectories. We discuss the single-molecule kinetic formulism of the Langmuir-Hinshelwood mechanism for heterogeneous catalysis, as well as of the two-pathway model for product dissociation reactions. This formulism enables the quantitative evaluation of the heterogeneous reactivity and the differential selectivity of individual nanoparticles that are usually hidden in ensemble measurements. Extension of this formulism to single-molecule catalytic kinetics of oligomeric enzymes is also discussed.
引用
收藏
页码:911 / 922
页数:12
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