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yingxingwang

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3.5. Effect of the redox properties on the activity
To further explore the relationship between the redox property and activity, XPS and H2-TPR techniques were conducted. The O 1s spectra of the M-OMS-2 catalysts are shown in Fig. 6, and the results of O 1s peak fittting are in Table 1. For all the catalysts, the O1s peak is composed of three subpeaks at around 530, 531.5 and 533 eV, which can be attributed to the lattice oxygen (Oa),the defect oxide or a hydroxyl-like group (Ob), and the adsorbed molecular water (Oc), respectively [20,37,38]. The amount of the Oa and Ob species were calculated from the relative area of the subpeaks. For each catalyst, the most abundant species is lattice oxygen (Oa), suggesting that lattice oxygen is important for the catalytic activity. The Ob species has higher mobility than the Oa species, and allow the diffusion of lattice oxygen [39,40]. To confirm the contribution of Ob species in the reaction, the area ratios of AOb/AO(b+a) were calculated (Table 1). The AOb/AO(b+a)
values  follow  the  order:  Ni-OMS-2≈ Cu-OMS-2 > Co-OMS-2 >Cr-OMS-2 > Fe-OMS-2, which is very similar to the orders of the Rs and AOS values. Kim et al. [39] reported that a defect-oxide or Rs and AOS values. Kim et al. [39] reported that a defect-oxide or a hydroxyl-like group could positively participate in the catalytic activity of VOCs combustion over K, Ca and Mg promoted Mn3O4 catalysts. Wang et al. [41] found that the accessibility was more important than the concentration of catalyst lattice oxygen for ethanol and acetaldehyde oxidation. Therefore, the defect-oxide species in M-OMS-2 catalyst could contribute to the catalytic activities of DME combustion.
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yingxingwang: 金币+50, 翻译EPI+1, 有帮助, 嗯,那也谢谢了 2013-04-06 13:27:25
3.5氧化还原性对活性的作用
为了进一步探究氧化还原性和活性之间的关系,采用了XPS和H2-TPR技术。M-OMS-2催化剂的O-1s谱如图6,各峰在表1中列出。对于所有的催化剂,O1s峰都是有三个亚峰,530、531.5和533eV构成,分别对归于晶格氧(Oa),缺陷氧化物或氢氧根类似基团(Ob)和吸附了的分子水(Oc)。Oa和Ob类的含量是通过计算亚峰的相对面积求得的。对于每个一催化剂,最多的是Oa,表明Oa对于催化活性是很重要的。Ob比Oa具有更高的移动性,有助于Oa的扩散。为了确定反应中Ob的作用,计算了面积比AOb/AO(b+a)(表一)。AOb/AO(b+a)顺序是:Ni-OMS-2≈ Cu-OMS-2 > Co-OMS-2 >Cr-OMS-2 > Fe-OMS-2,这种关系和Rs和AOS的顺序非常像。Kim等报道过缺陷氧或氢氧根类似基团能对于VOCs的氧化反应具有更好的催化能力相比于K,Ca和Mg催化MN3O4反应。Wang等发现在乙醇和乙醛的氧化反应中,Oa的可接近性比浓度具有更大的重要性。所以,M-OMS-2催化剂中的缺陷氧对于DME的氧化是有作用的。

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2楼2013-04-05 23:34:18
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