Direct Oxidation of Benzene to Phenol by N2O over Fe-ZSM-5 Zeolites Obtained via Ammonia-Steaming Treatment
Abstract: Hierarchical Fe-ZSM-5 was synthesized with the aid of 3-glycidoxypropyltrimethoxysilane (GPTMS) and then was modified by the ammonia-steaming post treatment. Various techniques, such as XRD, SEM, N2 adsorption-desorption, UV-vis and NH3-TPD were used to characterize the as-obtained and modified hierarchical Fe-ZSM-5. The direct oxidation of benzene to phenol using N2O as the oxidizing agent was conducted on the ammonia-steaming treated Fe-ZSM-5. The results showed that compared to the steaming treated Fe-ZSM-5 catalysts, ammonia-steaming treated hierarchical Fe-ZSM-5 catalysts preserved more mediate strong acid sites and ex-framework iron active species, thus exhibited a higher catalytic activity in the catalytic oxidation of benzene to phenol with N2O, while the frame structure and pore structure of Fe-ZSM-5 was almost unchange.
文章引用: 李露露 , 孟庆伦 , 文俊俊 , 肖强 (2015) 氨水蒸气处理Fe-ZSM-5分子筛催化N2O氧化苯制苯酚。 物理化学进展， 4， 38-44. doi: 10.12677/JAPC.2015.42006
 Schmidt, R.J. (2005) Industrial catalytic processes-phenol production. Applied Catalysis A: General, 280, 89-103.
 Suzuki, E., Nakashiro, K. and Ono, Y. (1988) Hydroxylation of benzene with dinitrogen monoxide over H-ZSM-5 zeolite. Chemistry Letters, 17, 953-956.
 Panov, G., Sheveleva, G., Kharitonov, A.E.A., Romannikov, V. and Vostrikova, L. (1992) Oxidation of benzene to phenol by nitrous oxide over Fe-ZSM-5 zeolites. Applied Catalysis A: General, 82, 31-36.
 Hensen, E., Zhu, Q. and Van Santen, R. (2003) Extraframework Fe-Al-O species occluded in MFI zeolite as the active species in the oxidation of benzene to phenol with nitrous oxide. Journal of Catalysis, 220, 260-264.
 Hensen, E., Zhu, Q. and Van Santen, R. (2005) Selective oxidation of benzene to phenol with nitrous oxide over MFI zeolites: 2. On the effect of the iron and aluminum content and the preparation route. Journal of Catalysis, 233, 136- 146.
 Parmon, V., Panov, G., Uriarte, A. and Noskov, A. (2005) Nitrous oxide in oxidation chemistry and catalysis: application and production. Catalysis Today, 100, 115-131.
 Pérez-Ramírez, J., Kapteijn, F., Groen, J.C., Doménech, A., Mul, G. and Moulijn, J.A. (2003) Steam-activated FeMFI zeolites. Evolution of iron species and activity in direct N2O decomposition. Journal of Catalysis, 214, 33-45.
 汪树军, 梁娟, 郭文珪, 赵素琴, 汪荣慧 (1992) ZSM-5 沸石骨架铝迁移规律的研究. 催化学报, 13, 1r38.
 褚琳琳, 姚琼斯, 肖强 (2014) 硅烷偶联剂与介孔模板剂作用下合成多级孔结构ZSM-5分子筛. 石油学报(石油加工), 30, 415-420.
 Chu, L., Liu, G. and Xiao, Q. (2014) Direct construction of hierarchical ZSM-5 microspheres aided by 3-glycidoxy- propyltrimethoxysilane. Materials Research Bulletin, 60, 746-751.
 Xiao, Q., Yao, Q., Zhuang, J., Liu, G., Zhong, Y. and Zhu, W. (2013) A localized crystallization to hierarchical ZSM-5 microspheres aided by silane coupling agent. Journal of Colloid and Interface Science, 394, 604-610.
 Liu, G., Zhuang, J., Yang, F.F., Xiao, Q., Zhong, Y.J. and Zhu, W.D. (2012) N2O Direct Decomposition over Hierarchical FeZSM-5 Catalysts. Advanced Materials Research, 518-523, 2593-2596.
 Li, Y., Liu, S., Xie, S. and Xu, L. (2009) Promoted aromatization and isomerization performance over ZSM-5 zeolite modified by the combined alkali-steam treatment. Reaction Kinetics and Catalysis Letters, 98, 117-124.
 Pérez-Ramírez, J., Kapteijn, F., Mul, G. and Moulijn, J. (2001) Superior performance of ex-framework FeZSM-5 in direct N2O decomposition in tail-gases from nitric acid plants. Chemical Communications, 693-694.
 Xin, H., Koekkoek, A., Yang, Q., van Santen, R., Li, C. and Hensen, E.J. (2009) A hierarchical Fe/ZSM-5 zeolite with superior catalytic performance for benzene hydroxylation to phenol. Chemical Communications, 7590-7592.
 Rana, B.S., Singh, B., Kumar, R., Verma, D., Bhunia, M.K., Bhaumik, A. and Sinha, A.K. (2010) Hierarchical mesoporous Fe/ZSM-5 with tunable porosity for selective hydroxylation of benzene to phenol. Journal of Materials Chemistry, 20, 8575-8581.