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Total oxidation of propane on Pt/WO_x/Al_2O_3 catalysts by formation of metastable Pt~(δ+) species interacted with WO_x clusters

机译:丙烷在Pt / WO_x / Al_2O_3催化剂上通过与WO_x团簇相互作用形成亚稳Pt〜(δ+)物种而完全氧化

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摘要

A series of Pt/Al_2O_3 catalysts with various tungsten oxide loadings were prepared by a stepwise wet impregnation method. The catalysts were characterized by X-ray diffraction, nitrogen physisorption, Raman, UV-vis diffuse reflectance, transmission electron microscopy and infrared spectroscopy of adsorbed probe molecules (CO, NH_3 or C_3H_8). The propane oxidation activity of Pt/Al_2O_3 catalyst is significantly improved by the addition of tungsten oxide. The tungsten oxide overlayer is presented as monomeric/polymeric WO_x clusters and WO_3 crystals depending on the loading amount. The most active catalyst occurs at an intermediate surface tungsten density corresponding to the maximum of polytungstate species. The electronic interactions between Pt and WO_x clusters lead to the generation of more reducible Pt~(δ+) species which are suggested to be active sites for propane oxidation. Basically, a simple model is proposed involving the initial C-H bond activation at the platinum-tungsten oxide interface.
机译:采用逐步湿法浸渍法制备了一系列负载不同氧化钨的Pt / Al_2O_3催化剂。通过X射线衍射,氮物理吸附,拉曼,紫外可见漫反射,透射电子显微镜和吸附的探针分子(CO,NH_3或C_3H_8)的红外光谱对催化剂进行表征。通过添加氧化钨,Pt / Al_2O_3催化剂的丙烷氧化活性显着提高。取决于负载量,氧化钨覆盖层呈现为单体/聚合物WO_x团簇和WO_3晶体。活性最高的催化剂出现在对应于多钨酸盐种类最大值的中间表面钨密度处。 Pt和WO_x簇之间的电子相互作用导致生成更多可还原的Pt〜(δ+)物种,这些物种被认为是丙烷氧化的活性位点。基本上,提出了一个简单的模型,涉及在铂-钨氧化物界面上的初始C-H键活化。

著录项

  • 来源
    《Journal of Hazardous Materials》 |2012年第30期|p.146-154|共9页
  • 作者单位

    Laboratory of Advanced Materials. Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;

    Laboratory of Advanced Materials. Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;

    Laboratory of Advanced Materials. Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;

    Laboratory of Advanced Materials. Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;

    Advanced Materials Institute, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, China;

    The Administrative Centre for China's Agenda 21, Beijing 100038, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    platinum; tungsten oxide; acidic support; metastable active sites; propane oxidation;

    机译:铂;氧化钨酸性支持物亚稳态活性位点;丙烷氧化;

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