Article Title

Theoretical investigations of the catalytic role of water in propene epoxidation on gold nanoclusters: A hydroperoxyl-mediated pathway

Authors

Chun-Ran Chang, Department of Chemistry and Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Tsinghua University, Beijing 100084, China
Yang-Gang Wang, Department of Chemistry and Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Tsinghua University, Beijing 100084, China
Jun Li, Department of Chemistry and Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Tsinghua University, Beijing 100084, China

Keywords

Gold nanocluster, propene epoxidation, hydroperoxyl radical, density functional theory

Abstract

We report a comprehensive theoretical investigation of the catalytic reaction mechanisms of propene epoxidation on gold nanoclusters using density functional theory (DFT). We have shown that water acts as a catalytic promoter for propene epoxidation on gold catalysts. Even without reducible supports, hydroperoxyl (OOH) and hydroxyl (OH) radicals are readily formed on small-size gold clusters from co-adsorbed H2O and O2, with energy barriers as low as 4–6 kcal/mol (1 cal = 4.186 J). Propene epoxidation occurs easily through reactions between C3H6 and the weakened O–O bond of the OOH radicals on the surfaces of gold clusters.

Graphical Abstract

DOI

https://doi.org/10.1007/s12274-010-0083-8

Publisher

Tsinghua University Press

Recommended Citation

Chun-Ran Chang,Yang-Gang Wang,Jun Li, Theoretical investigations of the catalytic role of water in propene epoxidation on gold nanoclusters: A hydroperoxyl-mediated pathway. NanoRes.2011, 4(1): 131–142