Partial oxidation of propylene catalyzed by VO3 clusters: A density functional theory study
文献类型：期刊论文
| 作者 | Wang, Zhe-Chen1,2; Xue, Wei1,2; Ma, Yan-Ping1; Ding, Xun-Lei1; He, Sheng-Gui1; Dong, Feng4; Heinbuch, Scott3; Rocca, Jorge J.3; Bernstein, Elliot R.4 |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY A
 |
| 出版日期 | 2008-07-03 |
| 卷号 | 112期号:26页码:5984-5993 |
| ISSN号 | 1089-5639 |
| DOI | 10.1021/jp7115774 |
| 英文摘要 | Density functional theory (DFT) calculations are carried out to investigate partial oxidation of propylene over neutral VO3 clusters. C=C bond cleavage products CH3CHO + VO2CH2 and HCHO + VO2CHCH3 can be formed overall barrierlessly from the reaction of propylene with VO3 at room temperature. Formation of hydrogen transfer products H2O + VO2C3H4, CH2=CHCHO + VO2H2, CH3CHCHO + VO2, and (CH3)(2)CO + VO2 is subject to tiny (0.01 eV) or small (0.06 eV, 0.19 eV) overall free energy barriers, although their formation is thermodynamically more favorable than the formation of C=C bond cleavage products. These DFT results are in agreement with recent experimental observations. VO3 regeneration processes at room temperature are also investigated through reaction Of 02 with the C=C bond cleavage products VO2CH2 and VO2CHCH3. The following barrierless reaction channels are identified: VO2CH2 + O-2 -> VO3 + CH2O; VO2CH2 + O-2 - VO3C + H2O, VO3C + O-2 -> VO3 + CO2; VO2CHCH3 + O-2 -> VO3 + CH3CHO; and VO2CHCH3 + O-2 -> VO3C + CH3OH, VO3C + O-2 -> VO3 + CO2. The kinetically most favorable reaction products are CH3CHO, H2O, and CO2 in the gas phase model catalytic cycles. The results parallel similar behavior in the selective oxidation of propylene over condensed phase V2O5/SiO2 catalysts. |
| 语种 | 英语 |
| WOS记录号 | WOS:000257155700030 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/64565]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | He, Sheng-Gui |
| 作者单位 | 1.Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Beijing 100080, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100039, Peoples R China 3.Colorado State Univ, Dept Elect & Comp Engn, Ft Collins, CO 80523 USA 4.Colorado State Univ, Dept Chem, Ft Collins, CO 80523 USA |
| 推荐引用方式 GB/T 7714 | Wang, Zhe-Chen,Xue, Wei,Ma, Yan-Ping,et al. Partial oxidation of propylene catalyzed by VO3 clusters: A density functional theory study[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2008,112(26):5984-5993. |
| APA | Wang, Zhe-Chen.,Xue, Wei.,Ma, Yan-Ping.,Ding, Xun-Lei.,He, Sheng-Gui.,...&Bernstein, Elliot R..(2008).Partial oxidation of propylene catalyzed by VO3 clusters: A density functional theory study.JOURNAL OF PHYSICAL CHEMISTRY A,112(26),5984-5993. |
| MLA | Wang, Zhe-Chen,et al."Partial oxidation of propylene catalyzed by VO3 clusters: A density functional theory study".JOURNAL OF PHYSICAL CHEMISTRY A 112.26(2008):5984-5993. |
入库方式： OAI收割
来源：化学研究所
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。