On the study of the catalytic transfer hydrogenation reaction: The hydrogenation of 3-buten-1-ol on a Pd-black film

• Published in: Journal of molecular catalysis. A, Chemical Chemical, 2007-07, Vol.272 (1), p.225-232
• Main Author: Oliveira, Maria Cristina F.
• Format: Article
• Language: English
• Subjects: Catalysis; Catalytic transfer hydrogenation; Chemistry; Electrocatalysis; Electrocatalytic hydrogenation; Electrochemistry; Exact sciences and technology; General and physical chemistry; Heterogeneous catalysis; Hydrogen donor; Hydrogenation; Hypophosphite; Kinetics and mechanism of reactions; Pd-black; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
• ISSN: 1381-1169; 1873-314X
• DOI: 10.1016/j.molcata.2007.03.039

The spontaneous catalytic transfer hydrogenation (CTH) was investigated using the H 2PO 2 − ion as the H-donor, 3-buten-1-ol as the model organic molecule and a Pd-black film as the catalyst. A pre-evaluation of the competitive ability of the unsaturated alcohol and H-donor to co-adsorb on the surface was performed by cyclic voltammetric experiments. The performance of the CTH was characterized in terms of the reaction selectivity, H-donor efficiency, material yield, reactant conversion, reaction rate and catalyst stability in successive hydrogenation reactions. The effect of the H-donor concentration on these parameters was also analysed. Evidence was given for the modification of the surface catalyst during the course of the hydrogenation but no effect on the catalytic activity was observed. The prospective ability of this catalyst material to be pre-charged in a hypophosphite solution and to operate as a source of hydrogen for the catalytic hydrogenation was demonstrated. For comparison, the electrocatalytic hydrogenation was also studied using the same organic compound and catalytic material as in the CTH. The catalytic transfer hydrogenation relies on the in situ formation of atomic hydrogen from a hydrogen donor, and its transfer to an organic or inorganic acceptor, through the use of an appropriate catalyst. A comprehensive investigation on the catalytic transfer hydrogenation using the hypophosphite ion as the hydrogen donor was carried out on a Pd-black film. ▪