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Characterization of C12A7-O- Catalyst and Mechanism of Phenol Formation by Hydroxylation of Benzene
Ting Dong,Zhao-xiang Wang,Tao Kan,Quan-xin Li*
Author NameAffiliationE-mail
Ting Dong Department of Chemical Physics, Lab of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China  
Zhao-xiang Wang Department of Chemical Physics, Lab of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China  
Tao Kan Department of Chemical Physics, Lab of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China  
Quan-xin Li* Department of Chemical Physics, Lab of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China liqx@ustc.edu.cn 
Abstract:
The benzene conversion and phenol selectivity from C6H6/O2/H2O over [Ca24Al28O64]4+·4O-(C12A7-O-) catalyst were investigated using a flow reactor. The benzene conversion increases with the increase of temperature, and the phenol selectivity mainly depends on both reaction temperature and the composition of the mixtures. The changes of the catalyst structure before and after the reactions and the intermediates on the catalyst surface and in the bulk were investigated by XRD, EPR and FT-IR. The catalytic reactions do not cause any damage to the structure of the positively charged lattice framework C12A7-O-, but part of the O- and O2- species in the bulk of C12A7-O- translate to OH- after the reactions. The neutral species and anion intermediate were investigated by Q-MS and TOF-MS respectively. It is suggested that the active O- and OH- species played a key role in the process of phenol formation.
Key words:  Benzene, Phenol, C12A7-O-, O-, OH-
FundProject:
C12A7-O-催化剂的表征以及苯羟基化合成苯酚的机理
董婷,王兆祥,阚涛,李全新*
摘要:
以[Ca24Al28O64]4+·4O-(C12A7-O-)为催化剂,在流动反应器中研究了苯羟基化合成苯酚的转化率以及苯酚的选择性.苯的转化率随反应温度增加而增加,苯酚的选择性与温度及反应物的组成有关.此外还通过XRD、EPR和FT-IR对催化剂的结构,表面及内部物种进行了考察.结果表明,C12A7-O-的电正性骨架结构在反应前后几乎没有任何差别,样品内部有部分O-和O2-在反应后转化为OH-.中性物种及负离子中间体分别由Q-MS和TOF-MS所检测.活性的O-和OH-被认为在苯酚形成过程中起了重要作用.
关键词:  苯,苯酚,C12A7-O-,O-,OH-
DOI:10.1088/1674-0068/20/03/297-304
分类号: