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Direct methylation of N-methylaniline with CO2/H-2 catalyzed by gold nanoparticles supported on alumina | |
Tang, G; Bao, HL; Jin, C; Zhong, XH; Du, XL; Zhong, XH (reprint author), E China Univ Sci & Technol, Inst Appl Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China. | |
2015 | |
Source Publication | RSC ADVANCES
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ISSN | 2046-2069 |
Volume | 5Issue:121Pages:99678—99687 |
Subtype | 期刊文献 |
Abstract | Small gold nanoparticles (similar to 3 nm) loaded onto various supports have been prepared by a deposition-precipitation method and studied for direct methylation of N-methylaniline with CO2/H-2. Among the catalysts examined, an acid-base bifunctional support gamma-alumina supported gold catalyst (Au/g-Al2O3) exhibits the best catalytic performance. Au/gamma-Al2O3 catalysts with controlled mean Au particle sizes (1.8-8.3 nm) have also been successfully prepared by regulating the concentration of HAuCl4 in solution, aging time, aging temperature and mole ratio of urea to gold in the process of deposition-precipitation with urea. The turnover frequency (TOF) values for direct methylation of N-methylaniline with CO2/H-2 increase on decreasing the mean size of Au nanoparticles (from 8.3 to 1.8 nm), showing that methylation of N-methylaniline with CO2/H-2 is a structure-sensitive reaction. A fast increase in TOF occurs when the mean Au particle size becomes smaller than 3 nm. Through TEM (transmission electron microscope), gold L-3-edge XAFS (X-ray absorption fine structure) and CO2- and NH3-TPD (temperature programmed desorption) analysis, we can conclude the Au particle sizes, oxidation state of the gold species and acid-base properties of the supports are responsible for the high catalytic activity of direct methylation of N-methylaniline with CO2/H-2. |
Keyword | Mild Reaction Conditions Carbon-dioxide Molecular-hydrogen Nitro-compounds Co Oxidation Formic-acid Secondary-amines Aromatic-amines Au Catalysts Size |
Indexed By | SCI |
Language | 英语 |
WOS ID | WOS:000365406800013 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.sinap.ac.cn/handle/331007/24904 |
Collection | 中科院上海应用物理研究所2011-2020年 |
Corresponding Author | Zhong, XH (reprint author), E China Univ Sci & Technol, Inst Appl Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China. |
Recommended Citation GB/T 7714 | Tang, G,Bao, HL,Jin, C,et al. Direct methylation of N-methylaniline with CO2/H-2 catalyzed by gold nanoparticles supported on alumina[J]. RSC ADVANCES,2015,5(121):99678—99687. |
APA | Tang, G,Bao, HL,Jin, C,Zhong, XH,Du, XL,&Zhong, XH .(2015).Direct methylation of N-methylaniline with CO2/H-2 catalyzed by gold nanoparticles supported on alumina.RSC ADVANCES,5(121),99678—99687. |
MLA | Tang, G,et al."Direct methylation of N-methylaniline with CO2/H-2 catalyzed by gold nanoparticles supported on alumina".RSC ADVANCES 5.121(2015):99678—99687. |
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Direct methylation o(790KB) | 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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