期刊
NANO LETTERS
卷 12, 期 3, 页码 1253-1259出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl203677b
关键词
Single-particle catalysis; platinum nanoparticles; single-molecule imaging deacetylation and deoxygenation; structure sensitivity
类别
资金
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-FG02-10ER16199]
- U.S. Army Research Office [W911NF0910232]
- National Science Foundation [CBET-0851257]
- Alfred P. Sloan Research Fellowship
- Cornell Center for Materials Research (CCMR)
- NSF
- NSF-MRSEC [DMR-1120296]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1063059] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [0851257] Funding Source: National Science Foundation
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.
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