| Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite | |
| Department | ERC国家工程研究中心 |
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
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| 2013 | |
| Source Publication | Journal of the American Chemical Society
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| ISSN | 0002-7863 |
| Volume | 135Issue:36Pages:13567-13573 |
| Abstract | 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. |
| Subject Area | 物理化学与绿色催化 |
| DOI | 10.1021/ja406978q |
| Funding Organization | the National Natural Science Foundation of China (No. 20933009);the 111 Project |
| Indexed By | SCI |
| If | 11.444 |
| Language | 英语 |
| Funding Project | C4利用及多产丙烯催化剂研究组 |
| compositor | 第二作者单位 |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.licp.cn/handle/362003/13435 |
| Collection | 精细石油化工中间体国家工程研究中心（ERC） |
| Affiliation | 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 |
| Recommended Citation 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. |
| Files in This Item: | ||||||
| File Name/Size | DocType | Version | Access | License | ||
| LZ01027497.pdf（399KB） | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Application Full Text | |
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