Intrazeolite anchoring of ruthenium carbonyl clusters: Synthesis, characterization, and their catalytic performances

This paper focuses attention on the intrazeolite anchoring of ruthenium carbonyl clusters and their catalytic performances. The synthesis involves the adsorption of metal carbonyl species or metal ion exchange into zeolite cages followed by reductive carbonylation under a mixed CO and H2 atmosphere. The characterization of the structure and properties of these samples was based on a multianalytical approach, including FT-IR, UV−vis, EXAFS spectroscopies, CO/H2 gas chemisorption, and 13CO isotopic exchange. Methane homologation was carried out on the zeolitic ruthenium clusters using a two-step process. The research encompassed several key points as follows. (i) [Ru3(CO)12] guests in Na56Y zeolite were thermally activated in a hydrogen atmosphere, generating intrazeolitic [H4Ru4(CO)12]. (ii) Hexammineruthenium(III) complexes in Na56X zeolite were thermally activated progressively in a mixed CO and H2 atmosphere. The generation process was considered to occur through conversion of the intermediate [Ru(NH3)5...