Detecting the Genesis of a High-Performance Carbon-Supported Pd Sulfide Nanophase and Its Evolution in the Hydrogenation of Butadiene

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• 作者：Bel茅n Bachiller-Baeza ; Ana Iglesias-Juez ; Eva Castillejos-L贸pez ; Antonio Guerrero-Ruiz ; Marco Di Michiel ; Marcos Fern谩ndez-Garc铆a ; Inmaculada Rodr铆guez-Ramos
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：September 4, 2015
• 年：2015
• 卷：5
• 期：9
• 页码：5235-5241
• 全文大小：429K
• ISSN：2155-5435

文摘

A new procedure for preparation of palladium sulfide nanoparticles, which are deposited and anchored over highly graphitized carbon nanofibers, is presented. The preparation method is based on the use of PdSO₄ as metal precursor or alternatively in the previous functionalization of the carbon surfaces with sulfonic groups by treatment with fuming sulfuric acid. Using an in situ high-energy X-ray diffraction technique, in both cases it is demonstrated that during the reduction treatment, the initially present palladium hydride is transformed into a palladium sulfide (Pd₄S). The catalytic properties of these materials have been tested in the gas-phase butadiene partial reduction to butenes. Although metallic palladium nanoparticles supported in the same carbon fibers produce butane as the principal product, the supported Pd₄S nanocrystals mainly yield different isomers of butenes independently of the conversion level. Furthermore, applying the same X-ray diffraction method reveals that this catalytic phase is stable during reaction.