Insight into the Mechanism of Glycerol Dehydration and Subsequent Pyridine Synthesis
文献类型：期刊论文
| 作者 | Jiang, Ding2; Wang, Shuang2; Li, Hongping5; Xu, Lujiang3; Hu, Xun4; Barati, Bahram2; Zheng, Anqing1
|
| 刊名 | ACS SUSTAINABLE CHEMISTRY & ENGINEERING
 |
| 出版日期 | 2021-03-01 |
| 卷号 | 9期号:8页码:3095-3103 |
| 关键词 | thermal decomposition glycerol pyrolysis pyridine pyridine synthesis |
| ISSN号 | 2168-0485 |
| DOI | 10.1021/acssuschemeng.0c07460 |
| 通讯作者 | Wang, Shuang(alexjuven@ujs.edu.cn) ; Li, Hongping(hongpingli@ujs.edu.cn) |
| 英文摘要 | In the present study, glycerol was exploited as the feedstock to synthesize pyridine with ammonia gas as a carrier and reactant through thermal conversion. A density functional theory (DFT) at the M06-2X method was applied to understand the mechanism of glycerol dehydration, the ammonization of oxygenated compounds, and the condensation of imines. The results confirmed that glycerol could be directly converted into pyridine in ammonia atmosphere at 550 degrees C. The overall view of the thermal conversion mechanism of glycerol was compared with the previous experimental data and the proposed mechanisms, which indicated that the neutral glycerol dehydration process should mainly produce acrolein, acetaldehyde, formaldehyde, and acetol. The produced oxygenated compounds (acrolein and acetaldehyde) can react with ammonia to form imine, which would further undergo Michael addition, a Diels-Alder reaction, deammonization, and dehydrogenation to form pyridine. In a catalytic condition, ZSM-5 not only plays a shape-selective effect on the conversion of glycerol to pyridine but also changes the path of the reaction. The structure of ZSM-5 limits the formation of multisubstituted pyridine products, which is beneficial to the formation of pyridine and monosubstituted pyridine. Protonated vinylamine intermediates may be a critical step limiting pyridine yield and selectivity. The kinetic analysis that is based on transition state theory was consistent with product contribution in experiments. The present study confirmed the selectivity and the conversion route of glycerol to pyridine. |
| 资助项目 | Jiangsu Province 333 Project[BRA2019277] ; CAS Key Laboratory of Renewable Energy[Y907k41001] ; Six Talent Peaks Project in Jiangsu Province[XNY-007] ; Foundation of State Key Laboratory of Coal Combustion[FSKLCCA1904] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:000625460400009 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | Jiangsu Province 333 Project ; CAS Key Laboratory of Renewable Energy ; Six Talent Peaks Project in Jiangsu Province ; Foundation of State Key Laboratory of Coal Combustion |
| 源URL | [http://ir.giec.ac.cn/handle/344007/32885]  |
| 专题 | 中国科学院广州能源研究所 |
| 通讯作者 | Wang, Shuang; Li, Hongping |
| 作者单位 | 1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Guangdong, Peoples R China 2.Jiangsu Univ, Sch Energy & Power Engn, Zhenjiang 212013, Jiangsu, Peoples R China 3.Nanjing Agr Univ, Coll Engn, Nanjing 210031, Jiangsu, Peoples R China 4.Univ Jinan, Sch Mat Sci & Engn, Jinan 250024, Shandong, Peoples R China 5.Jiangsu Univ, Inst Energy Res, Zhenjiang 212013, Jiangsu, Peoples R China |
| 推荐引用方式 GB/T 7714 | Jiang, Ding,Wang, Shuang,Li, Hongping,et al. Insight into the Mechanism of Glycerol Dehydration and Subsequent Pyridine Synthesis[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2021,9(8):3095-3103. |
| APA | Jiang, Ding.,Wang, Shuang.,Li, Hongping.,Xu, Lujiang.,Hu, Xun.,...&Zheng, Anqing.(2021).Insight into the Mechanism of Glycerol Dehydration and Subsequent Pyridine Synthesis.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,9(8),3095-3103. |
| MLA | Jiang, Ding,et al."Insight into the Mechanism of Glycerol Dehydration and Subsequent Pyridine Synthesis".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9.8(2021):3095-3103. |
入库方式： OAI收割
来源：广州能源研究所
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