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《化学科学与工程前沿(英文)》 >> 2016年 第10卷 第2期 doi: 10.1007/s11705-016-1568-0

Stability of Ni/SiO

. Institute of Chemical Technology, Universität Leipzig, Linnéstr. 3, 04103 Leipzig, Germany.. hte GmbH, Kurpfalzring 104, 69123 Heidelberg, Germany.. BASF SE, Carl-Bosch-Straße 38, 67056 Ludwigshafen, Germany

录用日期: 2016-04-27 发布日期: 2016-05-19

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摘要

Ni/SiO -ZrO catalysts with Ni loadings of 1 to 13 wt-% were prepared, characterized by elemental analysis, X-ray diffraction, N sorption, temperature programmed oxidation, temperature programmed reduction, and tested for their activity and stability in the dry reforming of methane with carbon dioxide at 850 °C, gas hourly space velocity of 6000 and 1800 h and atmospheric pressure. The SiO -ZrO support as obtained through a simple and efficient sol-gel synthesis is highly porous ( = 90 m ·g , = 4.4 nm) with a homogeneously distributed Si-content of 3 wt-%. No loss of Si or formation of monoclinic ZrO , even after steaming at 850 °C for 160 h, was detectable. The catalyst with 5 wt-% Ni loading in its fully reduced state is stable over 15?h on-stream in the dry reforming reaction. If the catalyst was not fully reduced, a reduction during the early stages of dry reforming is accompanied by the deposition of up to 44 mg·g carbon as shown by experiments in a magnetic suspension balance. Rapid coking occurs for increased residence times and times-on-stream starting at 50 h. The Ni loading of 5 wt-% on SiO -ZrO was shown to provide an optimal balance between activity and coking tendency.

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