Chemistry in confined space: a strategy for selective oxidation of hydrocarbons with high catalytic efficiencies and conversion yields under ambient conditions

Selective catalytic oxidation of hydrocarbons is challenging. Here, we show how this chemistry could be accomplished for cyclohexane (C 6 H 12 ) at room temperature with good turnover numbers, excellent catalytic efficiencies, high conversion yields and product selectivity, when the catalysis is med...

Ausführliche Beschreibung

Gespeichert in:
Bibliographische Detailangaben
Veröffentlicht in:Catalysis science & technology 2016-01, Vol.6 (2), p.7623-763
Hauptverfasser: Liu, Chih-Cheng, Ramu, Ravirala, Chan, Sunney I, Mou, Chung-Yuan, Yu, Steve S.-F
Format: Artikel
Sprache:eng
Schlagworte:
Online-Zugang:Volltext
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
Beschreibung
Zusammenfassung:Selective catalytic oxidation of hydrocarbons is challenging. Here, we show how this chemistry could be accomplished for cyclohexane (C 6 H 12 ) at room temperature with good turnover numbers, excellent catalytic efficiencies, high conversion yields and product selectivity, when the catalysis is mediated by a tricopper cluster complex immobilized in the nanochannels of mesoporous silica nanoparticles. The Cu I Cu I Cu I tricopper cluster is activated by dioxygen (O 2 ) to mediate the hydrocarbon oxidation to cyclohexanol (C 6 H 12 O) and cyclohexanone (C 6 H 10 O) by a direct O-atom transfer mechanism and the turnover of the catalyst is driven by hydrogen peroxide (H 2 O 2 ). The desired product is obtained by simply varying the experimental conditions. In the case of limiting H 2 O 2 , the catalytic efficiency can reach 96%. When H 2 O 2 is in large excess, the conversion of C 6 H 12 and selectivity to C 6 H 10 O can reach close to 100%. The nano-confined catalytic system leads to higher solubility of O 2 and thus to higher activity. The heterogeneous catalyst is robust and reusable after many cycles. Selective catalytic oxidation of hydrocarbons by a tricopper complex is demonstrated.
ISSN:2044-4753
2044-4761
DOI:10.1039/c6cy01501h