화학공학소재연구정보센터
Applied Catalysis A: General, Vol.529, 108-117, 2017
Synthesis, characterization and catalytic activity of a cobalt catalyst: Silica-supported, bis(1,5-diphenyl-1,3,5-pentanetrionato)dicobalt(II) [Co-2(dba)(2)]
Models of silica supported cobalt catalysts were formed by decorating the surface of Cab-O-Sil with the dinuclear cobalt complex, bis(1,5-dipheny1-1,3,5-pentanetrionato) dicobalt(II), [Co-2(dba)(2)]. To confirm the formation of a monolayer and multilayer of the complex on Cab-O-Sil, various loadings of [Co-2(dba)(2)] were combined with Cab-O-Sil by batch impregnation. The supported samples were characterized by elemental analysis, DRIFTS, and TGA to show that the Co-2(dba)(2) complex was adsorbed, on the silica surface intact and DRIFTS confirmed the loading of the Co-2(dba)(2) as a monolayer on the Cab-O-Sil up to a loading <2.09 wt% Co. This experimental monolayer loading confirmed the predicted loading (2.06 wt% Co metal) based on the surface area of the support, 200 m(2)/g, and the footprint area of the complex (1.866 nm(2)). When this precatalyst was decomposed in air and reduced in hydrogen, the morphology of the resulting particles depended upon the initial disposition of the metal complex on the support. Monolayer films of the metal complex decomposed into metal or metal oxide particles which are too small to give XRD reflections (2.09 wt% Co); whereas, catalyst derived from a multilayer film (4.1 wt% Co) showed large metal particles developing a very sharp XRD reflection from the Co(111) index. Both catalysts were active for the Fischer-Tropsch reaction at 350 degrees C with the catalyst derived from the multilayers of complex showing an activity, as characterized by first order rate constants, about 33 times that of the catalyst derived from a monolayer of the complex:71.4 vs 2.16 (mol Co-hour)(-1). The selectivity to liquid hydrocarbons showed a remarkably narrow distribution of molecular weights, comprised of mainly iso- and cycloalkanes having 6-8 carbons. (C) 2016 Elsevier B.V. All rights reserved.