Comparative Study on the Catalytic Performance of Single-Phase Mo−V−O-Based Metal Oxide Catalysts in Propane Ammoxidation to Acrylonitrile
Comparative Study on the Catalytic Performance of Single-Phase Mo−V−O-Based Metal Oxide Catalysts in Propane Ammoxidation to Acrylonitrile
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DOI：
10.1021/ie0509286
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发表时间：
2006
影响因子：
4.2
通讯作者：
N. Watanabe;W. Ueda
中科院分区：
文献类型：
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作者：
N. Watanabe;W. Ueda
采用水热法制备了五种单相Mo-V-O基混合金属氧化物：Mo-V-O、Mo-V-Te-O、Mo-V-Sb-O、Mo-V-Te-Nb-O和Mo-V-Sb-Nb-O，它们都具有相同的斜方晶系结构，并以这些混合氧化物为催化剂进行丙烷氨氧化制丙烯腈（AN）反应，以阐明组成元素的作用。所有的催化剂被发现是活性的丙烷氨氧化。通过将Te或Sb引入到Mo-V-O氧化物催化剂中，AN选择性提高了约2倍，并且通过将Nb引入到Mo-V-Te-O和Mo-V-Sb-O催化剂中，AN选择性进一步提高。同时，Te、Sb和Nb的引入也抑制了氨氧化分解为氮的反应。对每种催化剂的反应网络分析表明，框架结构中的Mo和V负责丙烷到丙烯的氧化活化，这是速率决定步骤，并且Te或Sb明显促进所形成的催化剂的转化。
Five single-phase Mo−V−O-based mixed metal oxides, Mo−V−O, Mo−V−Te−O, Mo−V−Sb−O, Mo−V−Te−Nb−O, and Mo−V−Sb−Nb−O, all of which assume the same orthorhombic structure, were prepared by hydrothermal method, and propane ammoxidation to acrylonitrile (AN) using these mixed oxides as catalysts was performed in order to clarify roles of the constituent elements. All of the catalysts were found to be active for propane ammoxidation. The AN selectivity was increased by approximately a factor of 2 by the introduction of Te or Sb to the Mo−V−O oxide catalyst and further increased by the introduction of Nb to the Mo−V−Te−O and Mo−V−Sb−O catalyst. At the same time, the oxidative decomposition of ammonia to nitrogen was retarded by the introduction of Te, Sb, and Nb. Reaction network analyses for each catalyst revealed that Mo and V in a framework structure are responsible for oxidative activation of propane to propene, which is the rate-determining step, and that Te or Sb clearly promotes the conversion of the formed ...