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A highly active and selective mesostructured Cu/AlCeO catalyst for CO2 hydrogenation to methanol

Journal 2018 · IF 4.521 · 发表于 2018 年 12 月 11 日
作者: Shaozhong Li,Yu Wang,Bin Yang,Limin Guo
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摘要

Mesostructured catalysts with optimized microstructure and surface properties endowed them attractive catalytic performance. Herein, the mesostructured AlCeO supports with different weight ratio of Al 2 O 3 and CeO 2 have been prepared on the basis of a self-assembly sol-gel process, then 15 wt.% Cu was loaded onto the mesostructured AlCeO supports by incipient wetness impregnation method. The mesostructured AlCeO supports with varied ratio of Al 2 O 3 to CeO 2 resulted in the very different Cu particle size, and for the optimized catalyst Cu/AlCeO-7 (the amount of Al 2 O 3 in AlCeO support was 70 wt.%), the Cu crystal size was around 7 nm based on the characterization of XRD and TEM. The Cu/AlCeO-7 catalyst had strong metal-support interactions (SMSI) and more Cu-ceria interface, which was confirmed by the XPS. Furthermore, the Cu/AlCeO-7 catalyst showed the highest exposed Cu surface area ( S Cu ) (25.5 m 2 /g cat ) from the analysis results of H 2 -TPR and dissociative chemisorption of nitrous oxide. The CO 2 -TPD results demonstrated the Cu/AlCeO-7 had strong surface basicity. Hence, Cu/AlCeO-7 catalyst showed the highest space time yield of methanol (STY MeOH ). The CO 2 conversion (Cu/AlCeO-7, V(H 2 )/V(CO 2 ) = 3/1, GHSV = 6000 mL h −1 g −1 and P = 4 MPa) was up to 22.5% at 553 K, the methanol selectivity can reach 94% at 473 K, and the STY MeOH was up to 7.2 mmol g cat. -1 h -1 at 493 K. The as-prepared mesostructured Cu/AlCeO-7 exhibited a promising catalyst candidate for CO 2 hydrogenation to methanol.

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