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首页> 美国卫生研究院文献>Nanomaterials >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
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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

机译：氧空位和Ni物种对Ni / ZrO2催化剂的选择性选择性的影响该催化剂用于将马来酸酐氢化为琥珀酸酐和γ-丁氧基丙酮

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摘要

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.
机译：制备了具有不同四方相含量的ZrO2纳米粒子ZrO2（P）和ZrO2（H）。 ZrO2（P）具有比ZrO2（H）高的四方相含量。使用ZrO2（P）和ZrO2（H）作为载体的Ni / ZrO2催化剂（10％（w / w））使用浸渍方法制备，并使用XRD，拉曼，H2-TPR，XPS和H2进行表征-TPD技术。测试了它们在马来酸酐加氢中的催化性能。 Ni / ZrO2（P）催化剂比Ni / ZrO2（H）催化剂表现出更强的金属-载体相互作用，因为它的氧空位数量更高且表面的配位氧离子低。因此，在Ni / ZrO2（P）催化剂上，获得了较小的Ni微晶和较高的马来酸酐为琥珀酸酐的C = C氢化活性。但是，Ni / ZrO2（P）催化剂的C = O氢化活性远低于Ni / ZrO2（H）催化剂。在210°C和5 MPa的H 2 压力下，在Ni / ZrO2（H）催化剂上，γ-丁内酯的收率仅为4.8％，而收率仅为4.8％。 Ni / ZrO 2 （P）催化剂在相同的反应条件下FT-IR原位表征表明Ni / ZrO 2 （H）催化剂的高C = O加氢活性可归因于活性金属镍物种与电子相对缺乏的氧之间的表面协同作用空缺。

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