Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite
文献类型：期刊论文
| 作者 | Wu, Jian-Feng1; Yu, Si-Min1; Wang, Wei David1; Fan, Yan-Xin1; Bai, Shi1; Zhang CW(张传卫)2 ; Gao Q(高强)2; Huang, Jun3; Wang, Wei1
|
| 刊名 | Journal of the American Chemical Society
 |
| 出版日期 | 2013 |
| 卷号 | 135期号:36页码:13567-13573 |
| ISSN号 | 0002-7863 |
| 英文摘要 | Methane and carbon dioxide are known greenhouse gases, and the conversion of these two C-1-building blocks into useful fuels and chemicals is a subject of great importance. By solid-state NMR spectroscopy, we found that methane and carbon dioxide can be co-converted on a zinc-modified H-ZSM-5 zeolite (denoted as Zn/H-ZSM-5) to form acetic acid at a low temperature range of 523-773 K. Solid-state C-13 and H-1 MAS NMR investigation indicates that the unique nature of the bifunctional Zn/H-ZSM-5 catalyst is responsible for this highly selective transformation. The zinc sites efficiently activate CH4 to form zinc methyl species (-Zn-CH3), the Zn-C bond of which is further subject to the CO2 insertion to produce surface acetate species (-Zn-OOCCH3). Moreover, the Bronsted acid sites play an important role for the final formation of acetic acid by the proton transfer to the surface acetate species. The results disclosed herein may offer the new possibility for the efficient activation and selective transformation of methane at low temperatures through the co-conversion strategy. Also, the mechanistic understanding of this process will help to the rational design of robust catalytic systems for the practical conversion of greenhouse gases into useful chemicals. |
| 学科主题 | 物理化学与绿色催化 |
| 收录类别 | SCI |
| 资助信息 | the National Natural Science Foundation of China (No. 20933009);the 111 Project |
| 语种 | 英语 |
| WOS记录号 | WOS:000330163200055 |
| 源URL | [http://210.77.64.217/handle/362003/13435]  |
| 专题 | 兰州化学物理研究所_ERC国家工程研究中心 |
| 作者单位 | 1.Lanzhou Univ, State Key Lab Appl Organ Chem, Coll Chem & Chem Engn, Lanzhou 730000, Gansu, Peoples R China 2.Chinese Acad Sci, Natl Engn Res Ctr Fine Petrochem Intermediates, Lanzhou Inst Chem Phys, Lanzhou 730000, Gansu, Peoples R China 3.Univ Sydney, Lab Catalysis Engn, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia |
| 推荐引用方式 GB/T 7714 | Wu, Jian-Feng,Yu, Si-Min,Wang, Wei David,et al. Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite[J]. Journal of the American Chemical Society,2013,135(36):13567-13573. |
| APA | Wu, Jian-Feng.,Yu, Si-Min.,Wang, Wei David.,Fan, Yan-Xin.,Bai, Shi.,...&Wang, Wei.(2013).Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite.Journal of the American Chemical Society,135(36),13567-13573. |
| MLA | Wu, Jian-Feng,et al."Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite".Journal of the American Chemical Society 135.36(2013):13567-13573. |
入库方式： OAI收割
来源：兰州化学物理研究所
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。