Unraveling the cation and anion effects and kinetics for ionic liquid catalyzed direct synthesis of methyl acrylate under mild conditions
文献类型:期刊论文
作者 | Wang, Gang1,3; Li, Zengxi1,3; Li, Chunshan2,4; Zhang, Suojiang2,4 |
刊名 | GREEN CHEMISTRY
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出版日期 | 2020-11-21 |
卷号 | 22期号:22页码:7913-7923 |
ISSN号 | 1463-9262 |
DOI | 10.1039/d0gc03133j |
英文摘要 | The direct synthesis of methyl acrylate (MA) from methyl acetate and trioxane at 350-380 degrees C is regarded as a supplementary route for the industrial propylene oxidation process; however, it suffers from rapid catalyst deactivation. Herein, a novel ionic liquid catalyzed mild liquid-phase system was developed for the direct synthesis of MA from methyl acetate and trioxane, where N,O-bis(trimethylsilyl)acetamide (BSA) was used as a probase for alpha-deprotonation and enol silyl etherification of methyl acetate. The trioxane decomposition to formaldehyde and methyl acetate enolization to 1-methoxy-1-trimethylsilyloxyethene proceeded with the catalysis of [Cation]Cl/MClx (M = Cu+, Fe3+, Zn2+ and Al3+) and [Cation]F, respectively. The cations and anions were observed to have significant effects on the yield and selectivity of MA, owing to the steric hindrance, acid site category and strength confirmed by pyridine probing FT-IR characterization. As a result, up to 60.2% yield with 94.6% selectivity of MA could be achieved when [N3,3,3,3]F and [N3,3,3,3]Cl/AlCl3 with 67 mol% AlCl3 were used in the presence of BSA at 25 degrees C. Kinetic studies indicated that the trioxane decomposition with the activation barrier of 41.2 +/- 0.3 kJ mol(-1) was the rate-determining step. |
WOS关键词 | PHASE ALDOL CONDENSATION ; ONE-STEP SYNTHESIS ; SELECTIVE OXIDATION ; ACETIC-ACID ; ACETATE ; FORMALDEHYDE ; OXIDE ; TRIOXANE ; TRIFLUOROMETHANE ; PERFORMANCE |
资助项目 | Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH022] ; National Natural Science Foundation of China[21878293] ; National Natural Science Foundation of China[21676270] ; Innovation Academy for Green Manufacture ; Chinese Academy of Sciences[IAGM-2019-A14] ; K. C. Wong Education Foundation[GJTD-2018-04] |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics |
语种 | 英语 |
WOS记录号 | WOS:000589891500020 |
出版者 | ROYAL SOC CHEMISTRY |
资助机构 | Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; Innovation Academy for Green Manufacture ; Chinese Academy of Sciences ; K. C. Wong Education Foundation |
源URL | [http://ir.ipe.ac.cn/handle/122111/42642] ![]() |
专题 | 中国科学院过程工程研究所 |
通讯作者 | Li, Zengxi; Li, Chunshan |
作者单位 | 1.Chinese Acad Sci, CAS Key Lab Green Proc & Engn, Inst Proc Engn, Beijing 100190, Peoples R China 2.Chinese Acad Sci, Innovat Acad Green Manufacture, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 101408, Peoples R China 4.Chinese Acad Sci, Inst Proc Engn, Beijing Key Lab Ion Liquids Clean Proc, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China |
推荐引用方式 GB/T 7714 | Wang, Gang,Li, Zengxi,Li, Chunshan,et al. Unraveling the cation and anion effects and kinetics for ionic liquid catalyzed direct synthesis of methyl acrylate under mild conditions[J]. GREEN CHEMISTRY,2020,22(22):7913-7923. |
APA | Wang, Gang,Li, Zengxi,Li, Chunshan,&Zhang, Suojiang.(2020).Unraveling the cation and anion effects and kinetics for ionic liquid catalyzed direct synthesis of methyl acrylate under mild conditions.GREEN CHEMISTRY,22(22),7913-7923. |
MLA | Wang, Gang,et al."Unraveling the cation and anion effects and kinetics for ionic liquid catalyzed direct synthesis of methyl acrylate under mild conditions".GREEN CHEMISTRY 22.22(2020):7913-7923. |
入库方式: OAI收割
来源:过程工程研究所
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