Issue 32, 2010

Osmium(0) nanoclusters stabilized by zeolite framework; highly active catalyst in the aerobic oxidation of alcohols under mild conditions

Abstract

Osmium(0) nanoclusters stabilized by zeolite-Y framework were reproducibly prepared by a simple two step procedure involving the incorporation of osmium(III) cations into the zeolite matrix by ion-exchange, followed by their reduction within the cavities of zeolite with sodium borohydride in aqueous solution all at room temperature. The composition and morphology of osmium(0) nanoclusters stabilized by zeolite framework, as well as the integrity and crystallinity of the host material were investigated by using ICP-OES, XRD, XPS, SEM, TEM, HRTEM, TEM/EDX, mid-IR, far-IR spectroscopies, and N2-adsorption/desorption technique. The results of the multiprong analysis reveal the formation of osmium(0) nanoclusters within the cavities of zeolite-Y without causing alteration in the framework lattice, formation of mesopores, or loss in the crystallinity of the host material. More importantly, far-IR studies showed that after the reduction of Os3+ cations by sodium borohydride the Na+ cations reoccupy their authentic cation sites restoring the integrity of zeolite-Y. The catalytic activity of osmium(0) nanoclusters stabilized by zeolite framework was tested in the aerobic oxidation of activated, unactivated and heteroatom containing alcohols to carbonyl compounds and was found to provide high activity and selectivity even under mild conditions (80 °C and 1 atm O2 or air). Moreover, they were found to be stable enough to be isolated and bottled as solid material, which can be reused as active catalyst under the identical conditions of the first run.

Graphical abstract: Osmium(0) nanoclusters stabilized by zeolite framework; highly active catalyst in the aerobic oxidation of alcohols under mild conditions

Article information

Article type
Paper
Submitted
15 Feb 2010
Accepted
28 May 2010
First published
07 Jul 2010

Dalton Trans., 2010,39, 7521-7527

Osmium(0) nanoclusters stabilized by zeolite framework; highly active catalyst in the aerobic oxidation of alcohols under mild conditions

M. Zahmakıran, S. Akbayrak, T. Kodaira and S. Özkar, Dalton Trans., 2010, 39, 7521 DOI: 10.1039/C003200J

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