Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite

CORC > 兰州化学物理研究所 > 中国科学院兰州化学物理研究所 > ERC国家工程研究中心

	Mechanistic Insight into the Formation of Acetic Acid from the Direct Conversion of Methane and Carbon Dioxide on Zinc-Modified H-ZSM-5 Zeolite
	Wu, Jian-Feng 1; Yu, Si-Min 1; Wang, Wei David 1; Fan, Yan-Xin 1; Bai, Shi 1; Zhang CW(张传卫)2 ; Gao Q(高强)2 ; Huang, Jun 3; Wang, Wei 1
刊名	Journal of the American Chemical Society
	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
内容类型	期刊论文
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.