介孔Cu/MS-1催化羟基化苯酚合成苯二酚
收稿日期: 2020-08-27
网络出版日期: 2021-02-06
基金资助
贵州师范大学2014年博士科研启动资助项目(600204)
Synthesis of dihydroxybenzenes by hydroxylation of phenol over Cu/ MS-1 with mesoporous
Received date: 2020-08-27
Online published: 2021-02-06
以十六烷基三甲基溴化铵（CTAB）为模板剂,采用溶胶凝胶法合成具有介孔的S-1载体（MS-1）,浸渍法制备Cu/MS-1催化剂,用于以双氧水为氧化剂、苯酚直接羟基化合成苯二酚的反应,运用正交实验法[L25（56）]对反应条件进行优化。使用X射线电子能谱（XPS）、N2的等温吸附-脱附和 H2的程序升温还原等方法对催化剂的结构和性能做了表征。结果表明：具有介孔的Cu/MS-1有利于反应物和生成物的快速扩散,催化性能明显优于Cu/S-1;高分散CuO相对质量分数最高的5.5% Cu/MS-1的催化活性最好,在优化条件下,苯二酚的产率达到47.2%,选择性为86.7%。具有介孔和MFI结构的Cu/MS-1稳定性强,重复使用5次后,苯二酚的产率仍达43.2%。
余天华 , 黄启朋 , 司徒成 . 介孔Cu/MS-1催化羟基化苯酚合成苯二酚[J]. 无机盐工业, 2021 , 53(2) : 94 -99 . DOI: 10.11962/1006-4990.2020-0110
The mesoporous S-1（MS-1） supporter was synthesized by sol-gel method with cetyltrimethyl-ammonium bromide（CTAB） as template.Cu/MS-1 catalyst was prepared by impregnation method,and then it was used to synthesis dihydroxy-benzenes directly by hydroxylation phenol with H2O2 as oxidation.The experimental conditions were optimized by orthogonal experimental[L25（56）].The structure and properties of catalyst were characterized by means of X-ray photoelectron spectro-scopy（XPS）,N2 adsorption-desorption and H2 temperature programmed reduction et al.The results showed that Cu/ MS-1 with mesoporous promised to rapid diffusion in pore of reactants and products,and was better catalytic performance than that of Cu/S-1.Under optimal conditions,the 5.5% Cu/MS-1 with the highest relative mass fraction of highly dispersed CuO pos-sessed the best catalytic activity among the catalysts; the yield of dihydroxybenzenes was 47.2% with the selectivity of 86.7%.The catalysts with mesoporous and MFI structure had a good sustainability,and its dihydroxybenzenes yield was 43.2% after recycle 5 times.
Key words： dihydroxybenzenes; CTAB; catalyst; phenol; hydrogen peroxide
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