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Size-Dependent Activity and Selectivity of Fe/MCF-17 in the Catalytic Hydrogenation of Carbon Monoxide Using Fe(0) Nanoparticles as Precursors

par Iablokov, Viacheslav ;Xiang, Yi-Zhi ;Meffre, Anca;Fazzini, Pier Francesco;Chaudret, Bruno;Kruse, Norbert
Référence ACS Catalysis, 6, 4, page (2496-2500)
Publication Publié, 2016-04

Article révisé par les pairs

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Résumé :

Monodisperse Fe(0) nanoparticles with diameters between 1.8 and 9.0 nm were prepared from organometallic {Fe[N(SiMe3)2]2}2 and intercalated into mesoporous MCF-17 silica. We observed high turnover frequencies of the catalytic CO hydrogenation; they increased with Fe particle size. Methane and short-chain olefin selectivities were highest for small particles, while the opposite trend applied to long-chain terminal olefins and oxygenates. The Anderson-Schulz-Flory chain lengthening probabilities were found to increase with Fe particle size for both paraffins and terminal olefins. Reaction-induced sintering of the metal particles was limited and could be explained by the transformation of Fe(0) precursors into (mainly) Fe-carbides. The results cast new light on the structure sensitivity of the catalytic CO hydrogenation.