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Supported bimetallic nano-alloys as highly active catalysts for the one-pot tandem synthesis of imines and secondary amines from nitrobenzene and alcohols

Meenakshisundaram, Sankar, He, Qian, Dawson, Simon, Nowicka, Ewa, Lu, Li, Bruijnincx, Pieter C. A., Beale, Andrew Michael, Kiely, Christopher and Weckhuysen, Bert 2016. Supported bimetallic nano-alloys as highly active catalysts for the one-pot tandem synthesis of imines and secondary amines from nitrobenzene and alcohols. Catalysis Science & Technology 14 (6) , pp. 5473-5482. 10.1039/C6CY00425C

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Abstract

The synthesis and functionalization of imines and amines are key steps in the preparation of many fine chemicals and for pharmaceuticals in particular. Traditionally, metal complexes are used as homogeneous catalysts for these organic transformations. Here we report gold-palladium and ruthenium-palladium nano-alloys supported on TiO2 acting as highly efficient heterogeneous catalysts for the one-pot synthesis of the imine N-benzylideneaniline and the secondary amine N-benzylaniline directly from the easily available and stable nitrobenzene and benzyl alcohol precursors using a hydrogen auto-transfer strategy. These reactions were carried out without any added external hydrogen, sacrificial hydrogen donor or a homogeneous base. The bimetallic catalysts were prepared by the recently developed modified impregnation strategy, giving efficient control of size and nano-alloy composition. Both bimetallic catalysts were found to be far more active than their monometallic analogues due to a synergistic effect. Based on the turnover numbers the catalytic activities follow the order Ru < Pd < Au << Au-Pd < Ru-Pd. Aberration corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAFS) studies of these catalysts revealed that the reason for the observed synergistic effect is the electronic modification of the metal sites in the case of the Au-Pd system and a size stabilisation effect in the case of the Ru-Pd catalyst.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Cardiff Catalysis Institute (CCI)
Chemistry
Subjects: Q Science > QD Chemistry
Additional Information: Pdf uploaded in accordance with publisher's policy at http://www.sherpa.ac.uk/romeo/issn/2044-4753/ (accessed 29/03/2016)
Publisher: Royal Society of Chemistry
ISSN: 2044-4753
Funders: European Commission Marie Curie Fellowship
Date of First Compliant Deposit: 30 March 2016
Date of Acceptance: 22 March 2016
Last Modified: 23 Apr 2019 21:30
URI: http://orca.cf.ac.uk/id/eprint/88258

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