不同结晶度的WO3负载Pt低温催化萘加氢合成十氢萘

Hydrogenation of naphthalene to decalin catalyzed by Pt supported on WO3 of different crystallinity at low temperature

  • 摘要: 不同温度下直接煅烧偏钨酸铵制备了晶化程度不同的两种氧化钨(WO3-500和WO3-900),通过XRD、SEM、TEM、XPS、H2-TPR和NH3-TPD手段对WO3载体负载Pt前后的物化性质进行了系统的表征,低温反应条件下研究了不同氧化钨负载Pt对萘加氢的催化性能。与WO3-900载体相比,低温煅烧得到具有较低的结晶程度,载体中大量的W5+物种和负载的Pt具有强的相互作用,并显示出较强的酸性。在低的反应温度下(70 ℃),Pt/WO3-500催化剂对萘加氢合成十氢萘具有优异的催化性能,萘的转化率和十氢萘的选择性均达到100%;在Pt/WO3-900催化下萘的转化率和十氢萘的选择性仅为26.7%和1.7%。结合催化剂的表征和催化反应结果,揭示了氧化钨中的氧缺陷位是提升Pt/WO3催化性能的关键因素,对设计高效的WO3负载 Pt催化剂催化萘合成十氢萘提供了一定的理论指导。

     

    Abstract: Two tungsten oxides (WO3-500 and WO3-900) were prepared at different calcination temperatures by using ammonium mettungstate as tungsten source. The physicochemical properties of WO3 before and after Pt loading were systematically characterized by XRD, SEM, TEM, XPS, H2-TPR, and NH3-TPD. The influence of the crystallization degree of WO3 on the hydrogenation of naphthalene was studied under low-temperature reaction conditions. Compared with the WO3-900 support, WO3-500 obtained by calcination at lower temperature exhibited a lower crystallization degree with a large amount of W5+ species, which resulted in strong interactions with Pt. The strong interaction between W species and Pt contributed to the high acidic strength. The Pt/WO3-500 catalyst demonstrated excellent catalytic performance for naphthalene hydrogenation to decalin at low reaction temperature (70 ℃) with full conversion and 100% decalin selectivity. Under identical conditions, conversion and decalin selectivity were only 26.7% and 1.7% over the Pt/WO3-900 catalyst. Combining the characteristics of the catalysts and their catalytic results, we revealed the promoting role of oxygen defects in WO3-supported Pt catalysts in the hydrogenation of naphthalene to decalin, which will provide theoretical guidance for designing efficient WO3-supported Pt catalysts for hydrogenation reactions.

     

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