| Rh基催化剂上氢甲酰化反应过程的原位高压NMR研究 |
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| 引用本文： | 兰喜杰,张维萍,严丽,丁云杰,韩秀文,林励吾,包信和.Rh基催化剂上氢甲酰化反应过程的原位高压NMR研究[J].波谱学杂志,2009,26(1):37-43. |
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| 作者姓名： | 兰喜杰 张维萍 严丽 丁云杰 韩秀文 林励吾 包信和 |
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| 作者单位： | 催化基础国家重点实验室(中国科学院,大连化学物理研究所),辽宁,大连,116023;中国科学院,研究生院,北京,100049;催化基础国家重点实验室(中国科学院,大连化学物理研究所),辽宁,大连,116023;应用催化研究室(中国科学院,大连化学物理研究所),辽宁,大连,116023 |
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| 摘 要： | 制备了用于丙烯氢甲酰化反应的Rh/SBA-15 和PPh3修饰的PPh3-Rh/SBA-15催化剂. 应用原位变温高压核磁共振技术，对比研究了丙烯在Rh/SBA-15 和PPh3修饰的多相催化剂PPh3 Rh/SBA-15上的氢甲酰化反应，实现了高压条件下催化反应的原位固体核磁共振表征. 13C MAS NMR研究结果表明：在1.0 MPa的反应压力下，随着反应温度升高丙烯与合成气在Rh/SBA-15催化剂上可转化生成丁醛，而PPh3配体修饰的PPh3-Rh/SBA-15催化剂上丁醛产物的正异比显著提高.
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| 关 键 词： | 核磁共振(NMR) 氢甲酰化反应 原位高压固体核磁共振 Rh/SBA-15催化剂 反应过程 |
| 收稿时间： | 2008-9-8 |
| 修稿时间： | 2008-9-18 |
The Reaction Process of Propene Hydroformalytion on PPh3-Rh/SBA-15 Catalyst Studied by In Situ High-ressure MAS NMR Spectroscopy |
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| LAN Xi-jie,ZHANG Wei-ping,YAN Li,DING Yun-jie,HAN Xiu-wen,LIN Li-wu,BAO Xin-he.The Reaction Process of Propene Hydroformalytion on PPh3-Rh/SBA-15 Catalyst Studied by In Situ High-ressure MAS NMR Spectroscopy[J].Chinese Journal of Magnetic Resonance,2009,26(1):37-43. |
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| Authors: | LAN Xi-jie ZHANG Wei-ping YAN Li DING Yun-jie HAN Xiu-wen LIN Li-wu BAO Xin-he |
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| Institution: | [1.State Key Laboratory of Catalysis (Dalian Institute of Chemical Physics, ;Chinese Academy of Sciences), Dalian 116023, China; 2.Natural Gas Utilization and Applied Catalysis Laboratory (Dalian Institute of Chemical Physics, ;Chinese Academy of Sciences), Dalian 116023, China; 3.Graduate School of Chinese Academy of Sciences, Beijing 100049, China] ; |
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| Abstract: | Rh/SBA-15 and ligand (triphenyl phosphine PPh3) modified heterogeneous PPh3-Rh/SBA-15 catalysts for the reaction of propene hydroformylation were prepared. The reaction process of propene hydroformylation on the Rh/SBA-15 and PPh3-Rh/SBA-15 catalysts was studied by in situ high-pressure（HP）MAS NMR techniques under the batch-like conditions. 13C MAS NMR spectra indicated that, with increasing temperature, propene and syngas could be converted into butyraldehyde on Rh/SBA-15 catalyst while the PPh3 modified heterogeneous PPh3-Rh/SBA-15 catalyst exhibited higher n/i ratio of butyraldehyde at 1.0 MPa. |
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| Keywords: | NMR hydroformylation in situ high-pressure MAS NMR Rh/SBA-15 catalyst reaction process |
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