Implication of the role of oxygen anions and oxygen vacancies for methanol decomposition over zirconia supported copper catalysts

作者: Gui-Sheng Wu , Lu-Cun Wang , Yong-Mei Liu , Yong Cao , Wei-Lin Dai

DOI: 10.1016/J.APSUSC.2006.01.056

关键词: DesorptionOxygenCubic zirconiaThermal desorption spectroscopyCopperCatalysisChemistryPhotochemistryDehydrogenationMethanolInorganic chemistry

摘要: Abstract The interaction of methanol with Cu, monoclinic ZrO 2 , and Cu/m-ZrO catalysts has been investigated by temperature programmed desorption (TPD) reaction (TPRS) the aim understanding nature surface sites mechanism involved in decomposition. A synergetic effect detected since combination copper significantly facilitates decomposition facile evolution H CO species at much lower temperature. In conjunction DRIFTS -TPD measurements Cu/ZrO sample reduced elevated temperatures, over is suggested to occur primarily on aid presence oxygen anions vacancies generated species-spillover between zirconia. interface zirconia also evidenced be crucial methanol, main role metallic Cu being provide for removal efficiently recombining hydrogen atoms formed during dehydrogenation located

参考文章(36)
R.A. Koeppel, A. Baiker, Ch. Schild, A. Wokaun, Effect of Preparation Variables on Catalytic Behaviour of Copper/Zirconia Catalysts for the Synthesis of Methanol from Carbon Dioxide Studies in Surface Science and Catalysis. ,vol. 63, pp. 59- 68 ,(1991) , 10.1016/S0167-2991(08)64572-3
Yong Cao, Jun-Cheng Hu, Zhong-Shan Hong, Jing-Fa Deng, Kang-Nian Fan, Characterization of High-Surface-Area Zirconia Aerogel Synthesized from Combined Alcohothermal and Supercritical Fluid Drying Techniques Catalysis Letters. ,vol. 81, pp. 107- 112 ,(2002) , 10.1023/A:1016024509710
CP Thurgood, JC Amphlett, RF Mann, BA Peppley, Deactivation of Cu/ZnO/Al2O3 Catalyst: Evolution of Site Concentrations with Time Topics in Catalysis. ,vol. 22, pp. 253- 259 ,(2003) , 10.1023/A:1023680121028
Daniel Bianchi, T. Chafik, Mohamed Khalfallah, Stanislas Jean Teichner, Intermediate species on zirconia supported methanol aerogel catalysts. IV: Adsorption of carbon dioxide Applied Catalysis A-general. ,vol. 112, pp. 219- 235 ,(1994) , 10.1016/0926-860X(94)80221-1
Daniel Bianchi, Jean-Louis Gass, Mohamed Khalfallah, Stanislas Jean Teichner, Intermediate species on zirconia supported methanol aerogel catalysts: I. State of the catalyst surface before and after the adsorption of hydrogen Applied Catalysis A-general. ,vol. 101, pp. 297- 315 ,(1993) , 10.1016/0926-860X(93)80276-V
A Ruban, B Hammer, P Stoltze, H.L Skriver, J.K Nørskov, Surface electronic structure and reactivity of transition and noble metals1Communication presented at the First Francqui Colloquium, Brussels, 19–20 February 1996.1 Journal of Molecular Catalysis A: Chemical. ,vol. 115, pp. 421- 429 ,(1997) , 10.1016/S1381-1169(96)00348-2
Daniel Bianchi, Tarik Chafik, Mohamed Khalfallah, Stanislas Jean Teichner, Intermediate species on zirconia supported methanol aerogel catalysts. III: Adsorption of carbon monoxide on copper containing solids Applied Catalysis A-general. ,vol. 112, pp. 57- 73 ,(1994) , 10.1016/0926-860X(94)80136-3
M Bowker, RA Hadden, H Houghton, JNK Hyland, KC Waugh, The mechanism of methanol synthesis on copper/zinc oxide/alumina catalysts Journal of Catalysis. ,vol. 109, pp. 263- 273 ,(1988) , 10.1016/0021-9517(88)90209-6
T. Merle-Méjean, P. Barberis, S.Ben Othmane, F. Nardou, P.E. Quintard, Chemical forms of hydroxyls on/in Zirconia: An FT-IR study Journal of the European Ceramic Society. ,vol. 18, pp. 1579- 1586 ,(1998) , 10.1016/S0955-2219(98)00080-6
T.L Reitz, P.L Lee, K.F Czaplewski, J.C Lang, K.E Popp, H.H Kung, Time-resolved XANES investigation of CuO/ZnO in the oxidative methanol reforming reaction Journal of Catalysis. ,vol. 199, pp. 193- 201 ,(2001) , 10.1006/JCAT.2000.3141