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Rh基催化剂上氢甲酰化反应过程的原位高压NMR研究

The Reaction Process of Propene Hydroformalytion on PPh₃-Rh/SBA-15 Catalyst Studied by In Situ High-pressure MAS NMR Spectroscopy

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【Author】 LAN Xi-jie1,3,ZHANG Wei-ping1,YAN Li2,DING Yun-jie2,HAN Xiu-wen1,LIN Li-wu1,BAO Xin-he1 [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]

【机构】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)；中国科学院研究生院；应用催化研究室(中国科学院大连化学物理研究所)；

【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.13CMASNMR研究结果表明:在1.0MPa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.更多还原

【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.更多还原