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A mechanistic investigation of the coupled reaction of n-hexane and methanol over HZSM-5

机译:HZSM-5上正己烷与甲醇偶联反应的机理研究

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摘要

The coupled reaction of n-hexane and methanol was studied and compared with the reactions of individual reactants over HZSM-5 zeolite catalyst. The catalytic reaction test results and the temperature-programmed surface reaction (TPSR) results showed an improvement of the initial n-hexane activity when methanol was used as co-reactant. The FT-IR analysis indicated that methanol was adsorbed on acid sites prior to n-hexane and immediately transformed into surface methoxy groups. These species acted as the active sites for the conversion of n-hexane and improved the initial activity of n-hexane by bimolecular hydride transfer. The catalytic test also suggested that alkenes resulting from the transformation of methanol further enhance the conversion of n-hexane, in addition to the improvement by methoxy groups. A faster conversion of methanol was also observed in the coupled system, which highlights a bidirectional promotion effect of the coupled reaction. A reaction mechanism is proposed to explain all observations.
机译:研究了正己烷与甲醇的偶联反应,并将其与单个反应物在HZSM-5沸石催化剂上的反应进行了比较。催化反应测试结果和程序升温表面反应(TPSR)结果表明,当甲醇用作共反应剂时,初始正己烷活性有所提高。 FT-IR分析表明,甲醇先于正己烷吸附在酸性位点上,然后立即转化为表面甲氧基。这些物质充当正己烷转化的活性位点,并通过双分子氢化物转移提高了正己烷的初始活性。催化试验还表明,除了通过甲氧基改进之外,由甲醇转化产生的烯烃进一步提高了正己烷的转化率。在偶联体系中还观察到甲醇的更快转化,这突出了偶联反应的双向促进作用。提出了一种反应机制来解释所有观察结果。

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