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Open AccessArticle

Tuning Selectivity of Maleic Anhydride Hydrogenation Reaction over Ni/Sc-Doped ZrO2 Catalysts

1
Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China
2
Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
3
Inorganic Chemistry Laboratory, Oxford University, Oxford OX1 3QR, UK
*
Authors to whom correspondence should be addressed.
Catalysts 2019, 9(4), 366; https://doi.org/10.3390/catal9040366
Received: 17 March 2019 / Revised: 10 April 2019 / Accepted: 16 April 2019 / Published: 18 April 2019
(This article belongs to the Special Issue Catalysis and Fine Chemicals)
A series of Sc-doped ZrO2 supports, with Sc2O3 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 Sc2O3 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 Sc2O3 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. View Full-Text
Keywords: Sc-doped ZrO2; selective hydrogenation; maleic anhydride; surface structure; oxygen vacancies Sc-doped ZrO2; selective hydrogenation; maleic anhydride; surface structure; oxygen vacancies
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MDPI and ACS Style

Zhao, L.; Zhang, Y.; Wu, T.; Zhao, M.; Wang, Y.; Zhao, J.; Xiao, T.; Zhao, Y. Tuning Selectivity of Maleic Anhydride Hydrogenation Reaction over Ni/Sc-Doped ZrO2 Catalysts. Catalysts 2019, 9, 366.

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