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Effect of initial nickel particle size on stability of nickel catalysts for aqueous phase reforming

Journal of Energy Chemistry 2016年第2期25卷 287-294页

作者： tomas van haasterecht Marten Swart Krijn P.de Jong Johannes Hendrik Bitter Inorganic Chemistry and Catalysis Utrecht University 3508 TB Utrecht The Netherlands Biobased Chemistry and Technology Wageningen University 6708 WG Wageningen The Netherlands

The deactivation behavior by crystallite growth of nickel nanoparticles on various supports（carbon nanofibers, zirconia, Si C, α-Al2O3 and γ-Al2O3） was investigated in the aqueous phase reforming of ethylene glycol. Supported Ni catalysts of ~10 wt% were prepared by impregnation of carbon nanofibers（CNF）,Zr O2, SiC, γ-Al2O3 and α-Al2O3. The extent of the Ni nanoparticle growth on various support materials follows the order CNF ~ ZrO2〉 SiC 〉 γ-Al2O3〉〉 α-Al2O3 which sequence, however, was determined by the initial Ni particle size. Based on the observed nickel leaching and the specific growth characteristics; the particle size distribution and the effect of loading on the growth rate, Ostwald ripening is suggested to be the main mechanism contributing to nickel particle growth. Remarkably, initially smaller Ni particles（~12 nm） supported on α-Al2O3 were found to outgrow Ni particles with initially larger size（~20 nm）. It is put forward that the higher susceptibility with respect to oxidation of the smaller Ni nanoparticles and differences in initial particle size distribution are responsible for this behavior.

关键词： Aqueous phase reforming Particle growth Catalyst stability Ostwald ripening Leaching Nickel catalysts Particle size effect Support effect

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Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

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Journal of Energy Chemistry 2013年第2期22卷 257-269页

作者： T. van haasterecht C. C. I. Ludding K. P. de Jong J. H. Bitter Inorganic Chemistry and Catalysis Utrecht University

Nickel, cobalt, copper and platinum nanoparticles supported on carbon nano-fibers were evaluated with respect to their stability, catalytic activity and selectivity in the aqueous phase reforming of ethylene glycol （230 ℃, autogenous pressure, batch reactor）. The initial surface-specific activities for ethylene glycol reforming were in a similar range but decreased in the order of Pt （15.5 h-1 ）〉Co（13.0 h 1 ）〉Ni（5.2 h-1） while the Cu catalyst only showed low dehydrogenation activity. The hydrogen molar selectivity decreased in the order of Pt （53%）〉Co（21%）〉Ni （15%） as a result of the production of methane over the latter two catalysts. Over the Co catalyst acids were formed in the liquid phase while alcohols were formed over Ni and Pt. Due to the low pH of the reaction mixture, especially in the case of Co （as a result of the formed acids）, significant cobalt leaching occurs which resulted in a rapid deactivation of this catalyst. Investigations of the spent catalysts with various techniques showed that metal particle growth is responsible for the deactivation of the Pt and Ni catalysts. In addition, coking might also contribute to the deactivation of the Ni catalyst.

关键词： carbon nano-fiber catalyst deactivation aqueous phase reforming non-noble metal catalyst

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