Mo2N/Zr-MCM-41新型催化剂的制备、表征及其麻疯树油加氢脱氧的催化性能

Preparation and characterization of Mo2N/Zr-MCM-41 catalyst and its performance in hydrodeoxygenation of Jatropha curcas oil

  • 摘要: 采用水热法合成载体MCM-41与不同初始n(Si)/n(Zr)的Zr-MCM-41,由(NH46Mo7O24与载体经过共浸渍、高温焙烧、氨气程序升温氮化制备了Mo2N/Zr-MCM-41新型加氢脱氧催化剂。采用XRD、BET、XPS、TEM以及吡啶红外等手段对催化剂进行了表征,并采用高压反应釜评价了不同n(Si)/n(Zr)的Mo2N/Zr-MCM-41催化麻疯树油加氢脱氧反应的性能。结果表明,Zr改性后的载体与纯硅MCM-41同样具有良好的孔道结构,且L酸、B酸酸值提高。Mo2N作为活性组分体现出了优异的加氢脱氧性能,在反应温度350℃、氢气分压3.0 MPa条件下催化的产品油组成主要为直链烷烃与芳香族化合物,占产品组分的90%(质量分数)以上;不同n(Si)/n(Zr)的新型催化剂脱氧率可高达100%;芳香族化合物含量高于直链烷烃,最高可占组成的72.09%(质量分数),主要以单环、双环芳香烃为主,碳链长度分布在C8-16;直链烷烃碳链长度分布在C8-17。通过Mo2N/Zr-MCM-41催化后的麻疯树油经分馏处理后可制备生物燃料。

     

    Abstract: MCM-41 and Zr-MCM-41 with different initial n(Si)/n(Zr) ratios were synthesized by hydrothermal method. Mo2N/Zr-MCM-41 hydrodeoxygenation catalysts were prepared by (NH4)6Mo7O24 carrier co-impregnation, calaination, temperature programing and nitridation, and characterized by XRD, XPS, TEM and Py-FTIR methods. The catalytic performance of Mo2N/Zr-MCM-41 in hydrodeoxygenation of Jatropha curcas oil was evaluated in a high pressure reactor. The results indicate that Zr modified carrier has the same pore structure as pure silicon MCM-41, and the value of L acid and B acid increases. As the active component, the Mo2N has an excellent HDO performance. Under the reaction temperature of 350℃ and the hydrogen pressure of 3.0 MPa, the catalyzed product oil is mainly composed of straight chain alkanes and aromatic compounds, accounting for more than 90% of the product components. The deoxygenation rates of the new catalysts with different n(Si)/n(Zr) ratios are all above 98%, and the content of aromatic compounds is higher than that of straight chain alkanes, which accounts for 72.09% of the total composition. The aromatic compounds are mainly single ring and bicyclic aromatic hydrocarbons with the length of carbon chain of C8-16. After the leprosy oils catalyzed by Mo2N/Zr-MCM-41 are fractionated, it can be prepared to be biofuels.

     

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