Issue 10, 2017

MOFs-Derived Co@CN bi-functional catalysts for selective transfer hydrogenation of α,β-unsaturated aldehydes without use of base additives

Abstract

Transfer hydrogenation protocols involve versatile and environmentally benign methods capable of providing alternatives to traditional hydrogenation processes. However, most of the non-noble metal catalysts used for transfer hydrogenation processes proceed with the aid of base additives or phosphorus-containing ligands to obtain good yields. We report a green and sustainable catalytic system by fabrication of a Co@CN bi-functional nanocatalyst with a new N-containing [Co(TPA)(ted)0.5] as a sacrificial template. This catalytic system was employed effectively for selective transfer hydrogenation of an α,β-unsaturated aldehyde (cinnamaldehyde, CAL) to obtain a high yield of an α,β-unsaturated alcohol (cinnamyl alcohol, COL) under a mild reaction condition without use of additives. During thermolysis, the retained N atoms were distributed uniformly in catalysts and endowed the catalysts with abundant basic sites, and Co2+ in [Co(TPA)(ted)0.5] were converted in situ into Co nanoparticles. Experimental results indicated obvious coordination interactions between Co nanoparticles and N atoms in these bi-functional catalysts. By optimizing the reaction conditions, a catalytic system with Co@CN-900 as a catalyst and n-hexanol as the proton donor exhibited the optimal activity for this transformation, achieving 99% selectivity for COL with full conversion. In addition, a reasonable reaction mechanism for the transfer hydrogenation of CAL to COL was proposed. Furthermore, this catalytic system also demonstrated good recyclability as well as wide substrates compatibility.

Graphical abstract: MOFs-Derived Co@CN bi-functional catalysts for selective transfer hydrogenation of α,β-unsaturated aldehydes without use of base additives

Supplementary files

Article information

Article type
Research Article
Submitted
06 شعبان 1438
Accepted
07 رمضان 1438
First published
10 رمضان 1438

Mater. Chem. Front., 2017,1, 2005-2012

MOFs-Derived Co@CN bi-functional catalysts for selective transfer hydrogenation of α,β-unsaturated aldehydes without use of base additives

X. Liu, S. Cheng, J. Long, W. Zhang, X. Liu and D. Wei, Mater. Chem. Front., 2017, 1, 2005 DOI: 10.1039/C7QM00189D

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