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Synthesis and Characterization of Massive Molybdenum Carbides and Supported Carbide-Containing Catalysts Mo_2C/C Prepared through Mechanical Activation

机译:机械活化法制备大体积碳化钼及负载型负载钼催化剂Mo_2C / C的合成与表征

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Procedures for the synthesis of massive molybdenum carbide by the mechanical activation of a mixture of MoO_3, commercial carbon, and Zn in air and the synthesis of the supported carbide-containing catalyst Mo_2C/C by the mechanical activation of commercial carbon impregnated with a 16% aqueous solu- tion of ammonium paramolybdate in an inert atmosphere were developed for the first time. With the use of a set of physicochemical methods, the metal contents, particle sizes, specific surface areas, and phase compo- sitions of the mechanically activated composites were determined. The structure of the carbide-containing supported catalyst was studied by electron microscopy, and its acidic properties were studied by the temper- ature-programmed desorption of ammonia; catalytic tests in the model reactions of dibenzothiophene (DBT) and alkane aromatization were performed. It was found that the Mo_2C/C catalyst exhibited high activity in these reactions: the conversion of DBT at a contact time of 3–6 h was 80–85%. The conversion of n-heptane at a contact time of 2 h was 31.2%, and 100% toluene was the reaction product. An increase in the contact time to 6 h led to a decrease in the conversion of n-heptane to 1.3%, and to 47% C_6–C_7 cycloalkanes were present in the reaction products. The results of this work are indicative of the high catalytic activity of the Mo_2C/C catalyst obtained by mechanical activation.
机译:通过在空气中机械活化MoO_3,商品碳和Zn的混合物合成块状碳化钼的程序,以及通过机械活化16%浸渍的商品碳来合成负载型含碳化物的催化剂Mo_2C / C的步骤首次在惰性气氛中开发了仲钼酸铵的水溶液。使用一组物理化学方法,确定了机械活化复合材料的金属含量,粒径,比表面积和相组成。用电子显微镜研究了含碳化物的负载型催化剂的结构,并通过温度程序控制的氨解吸研究了其酸性。在二苯并噻吩(DBT)和烷烃芳构化模型反应中进行了催化测试。已发现Mo_2C / C催化剂在这些反应中表现出高活性:在3–6 h的接触时间DBT的转化率为80–85%。接触时间为2 h时,正庚烷的转化率为31.2%,反应产物为100%甲苯。接触时间增加至6 h导致正庚烷转化率降低至1.3%,反应产物中存在C_6-C_7环烷烃降低至47%。这项工作的结果表明通过机械活化获得的Mo_2C / C催化剂具有很高的催化活性。

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