Selective oxidation of alcohols in a continuous multifunctional reactor: Ruthenium oxide catalysed oxidation of benzyl alcohol
Selective oxidation of alcohols in a continuous multifunctional reactor: Ruthenium oxide catalysed oxidation of benzyl alcohol
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DOI：
10.1016/j.apcata.2005.04.042
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发表时间：
2005-07-15
影响因子：
5.5
通讯作者：
Plucinski, PK
中科院分区：
文献类型：
--
作者：
Bavykin, DV;Lapkin, AA;Plucinski, PK
以分子氧选择氧化苯甲醇合成苯甲醛为模型反应，设计、建造和测试了多功能紧凑型反应器。该反应器由静态混合器、换热通道和毫米级固定床反应通道组成，集混合、换热和反应功能于一体。集成紧凑型反应堆技术应该对精细化工和制药行业特别有吸引力。由于强化了传质，该反应器在广泛的操作条件下都能在动力学状态下运行。尽管反应速率高，热效应明显，反应物浓度高(TOF=300h(-1)，H-r度=-183.7 kJmol(-1))，反应器仍能等温运行。为提高氧化反应的选择性，研究了沿反应器长度分段注氧的方法。分段喷射被证明是有益的；然而，这可能是由于沿填充反应通道发展了更均匀的两相流水动力状态。以Ru/Al_2O_3(0.9wt%Ru/Al_2O_3)为载体，研究了Ru(III)水合氧化物催化剂的催化性能。即使在反应物浓度接近工业条件(1molL-1)的情况下，仍能观察到高活性和选择性。(C)2005 Elsevier B.V.保留所有权利。
A multifunctional compact reactor was designed, built, and tested, using as a model reaction the selective oxidation of benzyl alcohol to benzaldehyde with molecular oxygen. The reactor contains static mixers, heat-transfer channels and mm-scale packed-bed reaction channels, i.e., integrating mixing, heat transfer and reaction functionalities. Integrated compact reactor technology should be particularly attractive to the fine chemistry and pharmaceutical industries. The reactor was shown to operate in the kinetic regime over a broad range of operating conditions due to intensified mass transfer. The reactor was also shown to operate isothermally despite high reaction rate, an appreciable heat effect and high reactant concentration (TOF = 300 h(-1), Delta H-r degrees = - 183.7 kJ mol(-1)). Staged injection of oxygen along the length of the reactor was investigated as a method of increasing the selectivity of oxidation reactions. Staged injection was shown to be beneficial; however, this was likely to be due to the development of a more uniform hydrodynamic regime of two-phase flow along the packed reaction channel. Experiments were performed with the ruthenium(III) hydrated oxide catalyst supported on alumina (0.9 wt% Ru/Al2O3). High activity and selectivity were observed even when working with reactant concentrations approaching industrial conditions (1 mol L-1). (c) 2005 Elsevier B.V. All rights reserved.