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1135725495铁杆木虫 (著名写手)
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The previous studies on the interactions of acetaldehyde with TiO2(001) surfaces,however, indicated that aldol condensation occurs on both{011} - and{114}-faceted TiO2(001) surfaces and that aldol condensation, although a bimolecular reaction, is relatively insensitive to the surface structures based on the comparison of the results obtained from the {011}- and{114}-facetedsurfaces. The{011}-faceted surface, in their studies, was thought to be a fully oxidized surface exposing only five-coordinated cations. The STM study, however, showed a certain number of mixed coordination sites on the same surface. Comparing the results obtained in this study with the interpretations of the previous studies, and assuming that the STM results revealed the correct structural information on the{011}-faceted surface, we suggest that the nonuniform cation sites on the fully oxidized surfaces are responsible for the initiation of aldol condensation.The{011}- and{114}-faceted surfaces containing four-, five-,and six-coordinated cations are capable of initiating aldol condensation, whereas the fully oxidized SrTiO3(100) surface lacks unsaturated cation sites and is, therefore, inert to aldol condensation. Thus, the enhanced reactivity of CH3CHO on theTiO2(100) surfaces can be related to the unique structures of the faceted TiO2 (001) surfaces that possess a variety of surface sites, many of which are very active toward the reactions of organic molecules adsorbed on these surfaces. |
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baoshanqiu
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1135725495: 金币+20, 翻译EPI+1, ★有帮助 2015-07-09 08:05:27
1135725495: 金币+20, 翻译EPI+1, ★有帮助 2015-07-09 08:05:27
| 然而先前对乙醛与二氧化钛（001）表面相互作用的研究表明醛醇缩合反应发生在二氧化钛（001）表面的{011}-和{114}晶面上。虽然这是一个双分子反应，但从比较研究{011}- 和114}-晶面的结果来看，该反应对表面结构相对不敏感。在他们的研究中，{011}晶面仅暴露五-配位阳离子，是一个完全氧化的表面。但扫描隧道显微镜（STM）研究发现在同一个表面有一定数量的复合配位点存在。比较本研究与先前研究结果的解释，如果STM结果揭示的是{011}晶面正确的结构信息，那么我们认为在完全氧化的表面上的非均匀阳离子位点就是启动醛醇缩合反应的所在。{011}- 和{114}-晶面具有四-、五-和六-配位阳离子，能够启动醛醇缩合反应，而完全氧化的三氧化锶钛（SrTiO3(100)）表面缺乏不饱和的阳离子位点，因而不能启动醛醇缩合反应。因此在二氧化钛(100)表面上乙醛的反应活性增强可能与二氧化钛（001）表面独特的晶面结构有关。该表面上拥有各种表面位点，其中的许多位点对于吸附在表面的有机分子反应有很强的活性。 |
2楼2015-07-09 00:25:30