ChemSusChem | 2021
Atomically dispersed Co clusters anchored on N-doped carbon nanotubes for efficient dehydrogenation of alcohols and subsequent conversion to carboxylic acids.
Abstract
The catalytic dehydrogenation of readily available alcohols to high value-added carbonyl compounds is a research hotspot with scientific significance. While most of the current research about this reaction performed with noble metal-based homogeneous catalysts of high price and poor reusability. Herein, highly dispersed Co-cluster decorated N-doped carbon nanotubes (Co/N-CNTs) were fabricated via a facile strategy and used for the dehydrogenation of alcohols with high efficiency. AC-HAADF STEM and EXAFS characterizations confirmed the presence of metallic Co clusters with almost atomic dispersion. And the N-doped carbon supports also enhance the catalytic activity of Co clusters in the dehydrogenation reaction. The dehydrogenation products aldehydes were further transformed in situ to carboxylic acids through a Cannizzaro-type pathway under alkaline conditions. The reaction pathway of the dehydrogenation of alcohols is clearly confirmed by the theoretical calculations. This work should provide an effective and simple approach for the accurate design and synthesis of small Co-clusters catalysts for the efficient dehydrogenation-based transformation of alcohols to carboxylic acids under mild reaction conditions.