1. Tuning Selectivity of Maleic Anhydride Hydrogenation Reaction over Ni/Sc-Doped ZrO2 Catalysts.
- Author
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Zhao, Lili, Zhang, Yin, Wu, Tianjie, Zhao, Min, Wang, Yongzhao, Zhao, Jianghong, Xiao, Tiancun, and Zhao, Yongxiang
- Subjects
MALEIC anhydride ,HYDROGENATION ,METHANATION ,NICKEL catalysts ,SUCCINIC anhydride ,METAL catalysts ,STRUCTURE-activity relationships - Abstract
A series of Sc-doped ZrO
2 supports, with Sc2 O3 content in the range of 0 to 7.5% (mol/mol), were prepared using the hydrothermal method. Ni/Sc-doped ZrO2 catalysts with nickel loading of 10% (w/w) were prepared using impregnation method, and characterized with the use of XRD, Raman, H2 temperature-programmed reduction (H2 -TPR), H2 temperature-programmed desorption (H2 -TPD), XPS, and in situ FT-IR techniques. The catalytic performances of Ni/Sc-doped ZrO2 catalysts in maleic anhydride hydrogenation were tested. The results showed that the introduction of Sc3+ into ZrO2 support could effectively manipulate the distribution of maleic anhydride hydrogenation products. γ-butyrolactone was the major hydrogenation product over Sc-free Ni/ZrO2 catalyst with selectivity as high as 65.8% at 210 °C and 5 MPa of H2 pressure. The Ni/Sc-doped ZrO2 catalyst, with 7.5 mol% of Sc2 O3 content, selectively catalyzed maleic anhydride hydrogenation to succinic anhydride, the selectivity towards succinic anhydride was up to 97.6% under the same reaction condition. The results of the catalysts' structure–activity relationships revealed that there was an interdependence between the surface structure of ZrO2 -based support and the C=O hydrogenation performance of the ZrO2 -based supported nickel catalysts. By controlling the Sc2 O3 content, the surface structure of ZrO2 -based support could be regulated effectively. The different surface structure of ZrO2 -based supports, resulted in the different degree of interaction between the nickel species and ZrO2 -based supports; furthermore, the different interaction led to the different surface oxygen vacancies electron properties of ZrO2 -based supported nickel catalysts and the C=O hydrogenation activity of the catalyst. This result provides new insight into the effect of ZrO2 support on the selective hydrogenation activity of ZrO2 -supported metal catalysts and contributes to the design of selective hydrogenation catalysts for other unsaturated carbonyl compounds. [ABSTRACT FROM AUTHOR]- Published
- 2019
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