| 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,(3):186-192 |
| 单斜及四方晶相ZrO2催化CO加氢反应性能的比较 |
| Comparison of CO Hydrogenation on Monoclinicand Tetragonal ZrO2 Catalysts |
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| DOI： |
| 中文关键词: 二氧化锆 CO加氢 催化剂晶相 异丁烯 |
| 英文关键词: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. |
| 基金项目: |
| 李文 殷元骐 |
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)
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| 中文摘要: |
| 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 |
| 英文摘要: |
| 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 |
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