Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone
ZrO2 nanoparticles, ZrO2 (P) and ZrO2 (H), with different tetragonal phase contents, were prepared. ZrO2 (P) possessed higher tetragonal phase content than ZrO2 (H). Ni/ZrO2 catalysts (10% (w/w)), using ZrO2 (P) and ZrO2 (H) as supports, were prepared using an impregnation method, and were character...
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2019-03-01
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author | Lili Zhao Jianghong Zhao Tianjie Wu Min Zhao Wenjun Yan Yin Zhang Haitao Li Yongzhao Wang Tiancun Xiao Yongxiang Zhao |
author_facet | Lili Zhao Jianghong Zhao Tianjie Wu Min Zhao Wenjun Yan Yin Zhang Haitao Li Yongzhao Wang Tiancun Xiao Yongxiang Zhao |
author_sort | Lili Zhao |
collection | DOAJ |
description | ZrO2 nanoparticles, ZrO2 (P) and ZrO2 (H), with different tetragonal phase contents, were prepared. ZrO2 (P) possessed higher tetragonal phase content than ZrO2 (H). Ni/ZrO2 catalysts (10% (w/w)), using ZrO2 (P) and ZrO2 (H) as supports, were prepared using an impregnation method, and were characterized using XRD, Raman, H2-TPR, XPS, and H2-TPD techniques. Their catalytic performance in maleic anhydride hydrogenation was tested. The Ni/ZrO2 (P) catalyst exhibited stronger metal-support interactions than the Ni/ZrO2 (H) catalyst because of its higher number of oxygen vacancies and the low-coordinated oxygen ions on its surface. Consequently, smaller Ni crystallites and a higher C=C hydrogenation activity for maleic anhydride to succinic anhydride were obtained over a Ni/ZrO2 (P) catalyst. However, the C=O hydrogenation activity of Ni/ZrO2 (P) catalyst was much lower than that of the Ni/ZrO2 (H) catalyst. A 43.5% yield of γ-butyrolacetone was obtained over the Ni/ZrO2 (H) catalyst at 210 °C and 5 MPa of H2 pressure, while the yield of γ-butyrolactone was only 2.8% over the Ni/ZrO2 (P) catalyst under the same reaction conditions. In situ FT-IR characterization demonstrated that the high C=O hydrogenation activity for the Ni/ZrO2 (H) catalyst could be attributed to the surface synergy between active metallic nickel species and relatively electron-deficient oxygen vacancies. |
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spelling | doaj.art-1a6fc8a3d4b64d9ab6bd2eb67d7947862022-12-21T23:07:11ZengMDPI AGNanomaterials2079-49912019-03-019340610.3390/nano9030406nano9030406Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-ButyrolacetoneLili Zhao0Jianghong Zhao1Tianjie Wu2Min Zhao3Wenjun Yan4Yin Zhang5Haitao Li6Yongzhao Wang7Tiancun Xiao8Yongxiang Zhao9Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaInstitute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaInstitute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaInorganic Chemistry Laboratory, Oxford University, Oxford, OX1 3QR, UKEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaZrO2 nanoparticles, ZrO2 (P) and ZrO2 (H), with different tetragonal phase contents, were prepared. ZrO2 (P) possessed higher tetragonal phase content than ZrO2 (H). Ni/ZrO2 catalysts (10% (w/w)), using ZrO2 (P) and ZrO2 (H) as supports, were prepared using an impregnation method, and were characterized using XRD, Raman, H2-TPR, XPS, and H2-TPD techniques. Their catalytic performance in maleic anhydride hydrogenation was tested. The Ni/ZrO2 (P) catalyst exhibited stronger metal-support interactions than the Ni/ZrO2 (H) catalyst because of its higher number of oxygen vacancies and the low-coordinated oxygen ions on its surface. Consequently, smaller Ni crystallites and a higher C=C hydrogenation activity for maleic anhydride to succinic anhydride were obtained over a Ni/ZrO2 (P) catalyst. However, the C=O hydrogenation activity of Ni/ZrO2 (P) catalyst was much lower than that of the Ni/ZrO2 (H) catalyst. A 43.5% yield of γ-butyrolacetone was obtained over the Ni/ZrO2 (H) catalyst at 210 °C and 5 MPa of H2 pressure, while the yield of γ-butyrolactone was only 2.8% over the Ni/ZrO2 (P) catalyst under the same reaction conditions. In situ FT-IR characterization demonstrated that the high C=O hydrogenation activity for the Ni/ZrO2 (H) catalyst could be attributed to the surface synergy between active metallic nickel species and relatively electron-deficient oxygen vacancies.http://www.mdpi.com/2079-4991/9/3/406maleic anhydrideoxygen vacanciesselective hydrogenationNi/ZrO2 |
spellingShingle | Lili Zhao Jianghong Zhao Tianjie Wu Min Zhao Wenjun Yan Yin Zhang Haitao Li Yongzhao Wang Tiancun Xiao Yongxiang Zhao Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone Nanomaterials maleic anhydride oxygen vacancies selective hydrogenation Ni/ZrO2 |
title | Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone |
title_full | Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone |
title_fullStr | Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone |
title_full_unstemmed | Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone |
title_short | Synergistic Effect of Oxygen Vacancies and Ni Species on Tuning Selectivity of Ni/ZrO2 Catalyst for Hydrogenation of Maleic Anhydride into Succinic Anhydride and γ-Butyrolacetone |
title_sort | synergistic effect of oxygen vacancies and ni species on tuning selectivity of ni zro2 catalyst for hydrogenation of maleic anhydride into succinic anhydride and γ butyrolacetone |
topic | maleic anhydride oxygen vacancies selective hydrogenation Ni/ZrO2 |
url | http://www.mdpi.com/2079-4991/9/3/406 |
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