Nanostructured supported palladium catalysts-Non-oxidative methane coupling

被引:15
|
作者
Moya, Silvia F. [1 ]
Martins, Ruth L. [1 ]
Ota, Antje [2 ]
Kunkes, Edward L. [2 ]
Behrens, Malte [2 ]
Schmal, Martin [1 ]
机构
[1] Univ Fed Rio de Janeiro, Programa Engn Quim, COPPE, NUCAT, BR-21941972 Rio De Janeiro, RJ, Brazil
[2] Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
关键词
Palladium; Nanostructure; Sonochemistry; Colloidal method; Methane activation; Non-oxidative process; 2-STEP REACTION SEQUENCE; OXYGEN-FREE CONVERSION; HIGHER HYDROCARBONS; CARBON-MONOXIDE; LOW-TEMPERATURE; SONOCHEMICAL PREPARATION; HIGHER ALKANES; PLATINUM; RUTHENIUM; HYDROGEN;
D O I
10.1016/j.apcata.2011.10.025
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The Pd on alpha-Al2O3 catalysts with Pd particles in the low nanometer range have been prepared by a sonochemical reduction and a colloidal method, respectively. The two catalysts differ in their particle size, the widths of their particle size distributions and the amount of carbon incorporation in the Pd lattice. The adsorptive properties of the Pd/Al2O3 samples are different as a result of the different preparation methods. The methane adsorption capacity of that sample with smaller particles is lower than that of the catalyst with larger particles and the energy of activation is nearly doubled. DRIFTS and TPD results of CO adsorption supported by transmission electron microscopy data indicate that the PdSON catalyst with smaller and more homogeneous particles than PdCOL is highly dispersed which influences the coupling-hydrogenolysis process. The catalytic activity evidenced the formation of different adspecies during methane coupling and chemisorption on both catalysts. During the hydrogenation the carbon adspecies formed mainly methane at low adsorption temperatures. The significant amount of adsorbed methane at 773 K is governed by the highly active coordination unsaturated sites at the surface. (C) 2011 Elsevier BM. All rights reserved.
引用
收藏
页码:105 / 113
页数:9
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