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Hydrodechlorination of chlorobenzene over silica-supported nickel phosphide catalysts / Xuguang Liu in Industrial & engineering chemistry research, Vol. 47 n°15 (Août 2008) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 47 n°15 (Août 2008) . - p. 5362–5368 Titre : Hydrodechlorination of chlorobenzene over silica-supported nickel phosphide catalysts Type de document : texte imprimé Auteurs : Xuguang Liu, Auteur ; Jixiang Chen, Auteur ; Jiyan Zhang, Auteur Année de publication : 2008 Article en page(s) : p. 5362–5368 Note générale : Bibliogr. p. 5367-5368 Langues : Anglais (eng) Mots-clés : Chlorobenzene  --  hydrodechlorination;  Nickel  phosphate  catalysts Résumé : Silica-supported Ni3P, Ni12P5, and Ni2P catalysts were prepared by the temperature-programmed reduction method from nickel phosphate precursors. A Ni/SiO2 catalyst was also prepared as a reference. The effect of the initial Ni/P molar ratio in the precursor on the catalyst structure and hydrodechlorination performance was investigated. The physicochemical properties of the catalysts were characterized by means of N2 adsorption, hydrogen temperature-programmed reduction, X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet and visible spectroscopy, hydrogen temperature-programmed desorption, and inductively coupled plasma spectroscopy. The catalyst activities in the hydrodechlorination of chlorobenzene were evaluated in a fixed-bed reactor at atmospheric pressure. The silica-supported nickel phosphides exhibited superior hydrodechlorination activities to that of supported nickel. This can be attributed to the special physicochemical properties of nickel phosphides and a great amount of spillover hydrogen species. In nickel phosphides, there is a small amount of electron transfer from Ni to P, leading to a small positive charge on Ni. This favors a weakening of the interaction between chlorine and nickel sites, as well as between adsorbed hydrogen species and nickel phosphides. The “ensemble effect” of P is also beneficial in decreasing the coverage of chlorine on nickel sites. Because of the reduced interaction between adsorbed hydrogen species and nickel phosphides, the energy barrier of the hydrogen spillover on the silica-supported nickel phosphide catalysts decreases, which accounts for the increased amount of spillover hydrogen species on the catalyst surface. Spillover hydrogen species not only promote the hydrogenolysis of the C−Cl bond, but also favor the removal of chlorine ions from the surface of the catalysts. Hydrodechlorination over the nickel phosphide catalysts is characterized by a reaction induction period that becomes longer with increasing phosphorus content in the catalyst precursor. This is related to the blocking of active sites by excess phosphorus. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie7017542 [article] Hydrodechlorination of chlorobenzene over silica-supported nickel phosphide catalysts [texte imprimé] / Xuguang Liu, Auteur ; Jixiang Chen, Auteur ; Jiyan Zhang, Auteur . - 2008 . - p. 5362–5368. Bibliogr. p. 5367-5368 Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 47 n°15 (Août 2008) . - p. 5362–5368 Mots-clés : Chlorobenzene  --  hydrodechlorination;  Nickel  phosphate  catalysts Résumé : Silica-supported Ni3P, Ni12P5, and Ni2P catalysts were prepared by the temperature-programmed reduction method from nickel phosphate precursors. A Ni/SiO2 catalyst was also prepared as a reference. The effect of the initial Ni/P molar ratio in the precursor on the catalyst structure and hydrodechlorination performance was investigated. The physicochemical properties of the catalysts were characterized by means of N2 adsorption, hydrogen temperature-programmed reduction, X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet and visible spectroscopy, hydrogen temperature-programmed desorption, and inductively coupled plasma spectroscopy. The catalyst activities in the hydrodechlorination of chlorobenzene were evaluated in a fixed-bed reactor at atmospheric pressure. The silica-supported nickel phosphides exhibited superior hydrodechlorination activities to that of supported nickel. This can be attributed to the special physicochemical properties of nickel phosphides and a great amount of spillover hydrogen species. In nickel phosphides, there is a small amount of electron transfer from Ni to P, leading to a small positive charge on Ni. This favors a weakening of the interaction between chlorine and nickel sites, as well as between adsorbed hydrogen species and nickel phosphides. The “ensemble effect” of P is also beneficial in decreasing the coverage of chlorine on nickel sites. Because of the reduced interaction between adsorbed hydrogen species and nickel phosphides, the energy barrier of the hydrogen spillover on the silica-supported nickel phosphide catalysts decreases, which accounts for the increased amount of spillover hydrogen species on the catalyst surface. Spillover hydrogen species not only promote the hydrogenolysis of the C−Cl bond, but also favor the removal of chlorine ions from the surface of the catalysts. Hydrodechlorination over the nickel phosphide catalysts is characterized by a reaction induction period that becomes longer with increasing phosphorus content in the catalyst precursor. This is related to the blocking of active sites by excess phosphorus. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie7017542