钼钒磷杂多酸有机盐催化下苯与双氧水羟基化制苯酚的动力学  

Kinetics of Hydroxylation of Benzene to Phenol with Hydrogen Peroxide over Organic Molybdovanadophosphoric Heteropolyacid Salt Catalysts

作　　者：徐文俊[1] 景丽[1] 张富民[1] 钟依均[1] 朱伟东[1] 

机构地区：[1]浙江师范大学物理化学研究所先进催化材料省部共建教育部重点实验室,浙江金华321004

出　　处：《高校化学工程学报》2012年第4期624-628,共5页Journal of Chemical Engineering of Chinese Universities

基　　金：国家自然科学基金项目(20806075);浙江省自然科学基金杰出青年团队项目(R4080084)资助

摘　　要：通过简单的酸碱中和法制备出一系列碳链长度不同的杂多酸有机盐催化剂,在苯与双氧水羟基化制苯酚的反应中比较了催化剂的性能,发现钼钒磷杂多酸三乙胺盐的活性最高。随后在该催化剂上研究了苯与双氧水羟基化制苯酚的本征动力学。结果表明,在消除内外扩散影响的前提下,该反应对于苯和双氧水的反应级数都为1级,反应活化能为93.3 kJ mol 1。研究工作为苯与双氧水羟基化制苯酚的过程开发提供了基础。A serial of organic molybdovanadophosphoric heteropolyacid salt catalysts with different organic carbon-chain lengths were prepared by a facile acid-base neutralization method, and then a comparison was made for their catalytic activities in the reaction of hydroxylation of benzene to phenol with hydrogen peroxide as oxidant. The results show that the triethylamine molybdovanadophosphoric heteropolyacid salt （TEA-PMoV） has the highest catalytic activity for the hydroxylation reaction. Additionally, the intrinsic kinetics of the hydroxylation of benzene to phenol with hydrogen peroxide over TEA-PMoV was systematically investigated, from which both the orders of reaction with respect to benzene and hydrogen peroxide were found to be first order and the activation energy is 93.3 kJ.mol^-1, when the internal and external diffusion limitations are excluded. The obtained kinetic data are essential for the process development of the hydroxylation of benzene with hydrogen peroxide over the TEA-PMoV catalyst.

关 键 词：钼钒磷杂多酸有机盐 苯 苯酚 羟基化 本征动力学 

分 类 号：TQ243.12[化学工程—有机化工] TQ426.91