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Kinetics and reaction mechanism of phenol hydroxylation catalyzed by La-Cu_4FeAlCO_3

Science China Chemistry 2005年第6期48卷 530-537页

作者： CHEN Chunxia1,2, XU Chenghua1, FENG Liangrong1, SUO Jishuan1 & QIU Fali1 1. Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu 610041, China 2. Graduate School of the Chinese Academy of Sciences, Beijing 100039, China Chengdu Institute of Organic Chemistry Chinese Academy of Sciences Chengdu China Graduate School of the Chinese Academy of Sciences Beijing China

The present work synthesizes La-Cu4FeAlCO3 catalyst under microwave irradiation and characterizes its structure using XRD and IR techniques. The results show that the obtained La-Cu4FeAlCO3 has a hydrotalcite structure. In the phenol hydroxylation with H2O2 catalyzed by La-Cu4FeAlCO3, the effects of reaction time and phenol/H2O2 molar ratio on the phenol hy-droxylation, and relationships between the initial hydroxylation rate with concentration of the catalyst, phenol, H2O2 and reaction temperature are also investigated in details. It is shown the phenol conversion can reach 50.09% (mol percent) in the phenol hydroxylation catalyzed by La-Cu4FeAlCO3, under the reaction conditions of the molar ratio of phenol/H2O2 1/2, the amount ratio of phenol/catalyst 20, reaction temperature 343 K, reaction time 120 min, 10 mL distilled water as solvent. Moreover, a kinetic equation of v = k[La ? Cu 4 FeAlCO 3 ][C 6 H 5 OH][H 2 O 2]. and the activation energy of Ea=58.37 kJ/mol are obtained according to the kinetic studies. Due to the fact that the HO-Cu+-OH species are detected in La-Cu4FeAlCO3/H2O2 system by XPS, the new mechanism about the generation of hydroxyl free radicals in the phenol hydroxylation is pro-posed, which is supposed that HO-Cu+-OH species are transition state in this reaction.

关键词： rare earth, hydrotalcite, microwave irradiation, phenol hydroxylation, kinetics, reaction mechanism.

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