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钯催化剂上甲烷的氧化:载体的影响。

Oxidation of methane over palladium catalysts: effect of the support.

作者信息

Escandón Lara S, Ordóñez Salvador, Vega Aurelio, Díez Fernando V

机构信息

Department of Chemical and Environmental Engineering, University of Oviedo c/Julián Clavería s/n, 33006 Oviedo, Spain.

出版信息

Chemosphere. 2005 Jan;58(1):9-17. doi: 10.1016/j.chemosphere.2004.09.012.

Abstract

This work is focused on the deep catalytic oxidation of methane over supported palladium catalysts. The influences of the metal loading, oxidation state of palladium, nature of supports, presence of promoters in the supports (for zirconia-based supports), and thermal stability have been studied experimentally. Catalysts were prepared by incipient wetness of commercially available supports with aqueous solutions of palladium nitrate. For gamma-alumina support, it was observed that the optimal amount of palladium is between 0.5% and 2%, with higher amounts leading to a loss in specific activity. Concerning the oxidation state of the catalyst, it is concluded that for all the supports tested in the present work, a reduction of the catalyst is not needed, yielding the same conversion at steady state catalysts reduced and oxidised. The thermal stability of various supported catalysts were also studied, zirconia supports being the most active. These supports, specially Y-modified zirconia support, do not suffer appreciable deactivation below 500 degrees C.

摘要

本工作聚焦于负载型钯催化剂上甲烷的深度催化氧化。实验研究了金属负载量、钯的氧化态、载体性质、载体中促进剂的存在(对于基于氧化锆的载体)以及热稳定性的影响。通过用硝酸钯水溶液对市售载体进行初湿浸渍来制备催化剂。对于γ-氧化铝载体,观察到钯的最佳用量在0.5%至2%之间,用量更高会导致比活性降低。关于催化剂的氧化态,得出的结论是,对于本工作中测试的所有载体,不需要对催化剂进行还原,还原态和氧化态的稳态催化剂具有相同的转化率。还研究了各种负载型催化剂的热稳定性,氧化锆载体活性最高。这些载体,特别是钇改性的氧化锆载体,在500℃以下不会出现明显失活。

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