Role of Palladium in Iron Based Fischer鈭扵ropsch Catalysts Prepared by Flame Spray Pyrolysis

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• 作者：Melanie Minnermann ; Suman Pokhrel ; Karsten Thiel ; Robert Henkel ; Johannes Birkenstock ; Torsten Laurus ; Ardalan Zargham ; Jan-Ingo Flege ; Volkmar Zielasek ; Edyta Piskorska-Hommel ; Jens Falta ; Lutz Ma虉dler ; Marcus Ba虉umer
• 刊名：Journal of Physical Chemistry C
• 出版年：2011
• 出版时间：February 3, 2011
• 年：2011
• 卷：115
• 期：4
• 页码：1302-1310
• 全文大小：451K
• 年卷期：v.115,no.4(February 3, 2011)
• ISSN：1932-7455

文摘

Flame spray pyrolysis (FSP) is a novel technique for the fabrication of nanostructured catalysts with far-reaching options to control structure and composition even in cases where complex composites need to be prepared. In this study, we took advantage of this technique to synthesize highly dispersed pure and Pd-doped iron oxide nanoparticles and investigated them as Fischer鈭扵ropsch (FT) catalysts. By systematically varying the Pd content over a large range from 0.1 to 10 wt %, we were able to directly analyze the influence of the Pd content on activity and selectivity. In addition to catalytic measurements, the structure and composition of the particles were characterized before and after these measurements, using transmission electron microscopy, adsorption measurements, X-ray diffraction, and EXAFS. The comparison revealed on the one hand that small Pd clusters (diameter: 1鈭? nm) evolve from initially homogeneously distributed Pd and on the other hand that the iron oxide transforms into iron carbides depending on the Pd content. The presence of Pd influences the particle size in the pristine samples (8鈭?1 nm) resulting in specific surface areas that increase as the Pd content increases. However, after activation and reaction the specific surface areas become similar due to partial agglomeration and sintering. In a fixed bed FT reaction test, enhanced FT activity was observed with increasing Pd content while the selectivity shifts to longer chain hydrocarbons, mainly paraffins. Mechanistic implications regarding the role of Pd for the performance of the catalysts are discussed.