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单斜及四方晶相ZrO2催化CO加氢反应性能的比较
引用本文:李文,殷元骐.单斜及四方晶相ZrO2催化CO加氢反应性能的比较[J].分子催化,1999,13(3):186-192.
作者姓名:李文  殷元骐
作者单位:中国科学院兰州化学物理研究所(李文,殷元骐),中科院感光化学研究所(高润雄,侯瑞玲)
摘    要:研究了以纯单斜(m)和四方(t)晶相ZrO2为催化剂的CO加氢反应.尽管两种晶相催化剂均有较高的低碳烯烃的选择性,但是也发现了两者催化性能的显著差别.m-ZrO2催化剂对异丁烯有突出的选择性,而t-ZrO2催化剂,则只有乙烯和丙烯,几乎没有C4烯烃的选择性.室温下CO吸附的原位IR谱测试可见,只有在t-ZrO2催化剂上观测到不可逆含氧吸附物种.吡啶吸附的Raman谱显示出它们之间表面性质的差别,m-ZrO2催化剂表面存在等强度的Lewis和Bronsted酸中心,而在t-ZrO2催化剂表面几乎只有Bronsted酸中心.催化过程的一些模型分子电子结构计算也表明了ZrO2催化剂对低碳烯烃选择性内在的电子结构条件.我们推测CO在m-ZrO2催化剂表面的孪式吸附物种可能是导致异丁烯产物的根源

关 键 词:二氧化锆  CO加氢  催化剂晶相  异丁烯

Comparison of CO Hydrogenation on Monoclinicand Tetragonal ZrO2 Catalysts
LI Wen,YIN Yuan\|qi,GAO Rong\|xiong,HOU Rui\|ling.Comparison of CO Hydrogenation on Monoclinicand Tetragonal ZrO2 Catalysts[J].Journal of Molecular Catalysis (China),1999,13(3):186-192.
Authors:LI Wen  YIN Yuan\|qi  GAO Rong\|xiong  HOU Rui\|ling
Institution:LI Wen,YIN Yuan\|qi1),GAO Rong\|xiong,HOU Rui\|ling
Abstract:CO hydrogenation was studied over pure monoclinic and tetragonal ZrO2 catalysts. Although there were high selectivities to olefins for both m \|ZrO2 and t \|ZrO2 catalysts the significant difference between them is found that only monoclinic ZrO2 has high selectivity to isobutene . IR spectra of CO adsorption on them at room temperature show that the irreversible adsorption of the oxygen containing species could be observed only for tetragonal catalyst. Raman spectra after pyridine adsorption reveal the difference of surface properties between them. There are Lewis and Br nsted acid sites with equal strength on the surface of monoclinic zirconia, but there was almost only Br nsted acid site on the surface of tetragonal zirconia. Quantum calculations of some model molecules for the surface structures of catalysts and the intermediate species during the catalytic process also show the structural feature of ZrO2 catalysts inducing to the selectivities to olefins. Finally, we conjecture t
Keywords:Zirconia  CO hydrogenation  Crystal phase of catalyst  Isobutenehat the adsorption species (CO)2 Zr3  should be  the original species producing isobutene during the catalytic reaction  
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