Fe-ZSM-5催化剂的制备及其在芬顿体系中的应用研究
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摘要
利用过量浸渍法制备了Fe-ZSM-5催化剂,考察制备条件和反应条件对Fe-ZSM-5催化剂在甲基橙溶液中降解过程的影响,同时用XRD和XPS对催化剂的表面性质进行表征。结果表明,Fe2O3是催化剂的主要活性位,能够显著提高甲基橙催化降解的效果;制备条件和反应条件对Fe-ZSM-5催化降解反应均具有较大的影响。最佳制备条件为:煅烧温度为400℃,Fe负载量为1%;最佳反应工艺条件为:催化剂质量为1. 5 g,Fe与H2O2摩尔比为1∶6,pH为3。
Fe-ZSM-5 catalyst is prepared by means of overdose dip-molding method. The degradation process of methyl orange solution is used to evaluate the effects of preparation conditions for Fe-ZSM-5 catalyst and reaction conditions.Characterization on surface property of the catalyst is conducted by means of XRD and XPS. Experimental results show that Fe_2O_3 is the major active sites of the catalyst and can promote remarkably the degradation efficiency of methyl orange.The preparation conditions for Fe-ZSM-5 catalyst and reaction conditions both have significant influences on the degradation reaction. The optimal preparation conditions include a calcination temperature of 400℃ and 1% Fe loading amount,while the optimal reaction conditions are as follows: the adding amount of catalyst is 1. 5 g,the molar ratio of Fe to H_2O_2 is 1 ∶6 and p H is 3.
Fe-ZSM-5 catalyst is prepared by means of overdose dip-molding method. The degradation process of methyl orange solution is used to evaluate the effects of preparation conditions for Fe-ZSM-5 catalyst and reaction conditions.Characterization on surface property of the catalyst is conducted by means of XRD and XPS. Experimental results show that Fe_2O_3 is the major active sites of the catalyst and can promote remarkably the degradation efficiency of methyl orange.The preparation conditions for Fe-ZSM-5 catalyst and reaction conditions both have significant influences on the degradation reaction. The optimal preparation conditions include a calcination temperature of 400℃ and 1% Fe loading amount,while the optimal reaction conditions are as follows: the adding amount of catalyst is 1. 5 g,the molar ratio of Fe to H_2O_2 is 1 ∶6 and p H is 3.
引文
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[2]吴伟,吴程程,赵雅萍.非均相Fenton技术降解有机污染物的研究进展[J].环境科学与技术,2010,33(6):99-104.
[3]刘英.非均相Fenton法深度降解活性染料废水的研究[D].大连:大连理工大学,2011.
[4]Duan F,Yang Y Z,Li Y P.Heterogeneous Fenton-like degradation of 4-chlorophrnol using iron/ordered mesoporous carbon catalyst[J].Journal of Environmental Sciences,2014,26(5):1171-1179.
[5]陈培榕,吴耀国,刘保超,等.金属柱撑黏土催化非均相Fenton技术的研究[J].现代化工,2009,29(12):20-25.
[6]Bayat M,Sohrabi M,Royaee S J.Degradation of phenol by heterogeneous Fenton reaction using Fe/clinoptilolite[J]. Journal of industrial and Engineering Chemistry,2012,18(3):957-962.
[7]Zhang A,Wang N,Zhou J,et al. Heterogeneous Fenton-like catalytic removal of p-nitrophenol in water using acid-activated fly ash[J]. Journal of Hazardous Materials,2012,201-202(1):68-73.
[8]王帅军,赵朝成,刘其友,等.Fe-Ce/ZSM-5类Fenton催化剂降解甲基橙废水的影响因素研究[J].石油炼制与化工,2016,47(1):17-21.
[9]刘秀凤,徐凯,张宝泉.ZSM-5和Fe-ZSM-5分子筛膜的合成与表面改性[J].化工学报,2014,65(S2):304-309.
[10]张伟红,李苗苗,解立平,等.负载型Ti O2/MCM-41催化剂在光催化-膜分离耦合工艺中的性能[J].环境工程学报,2017,11(3):1533-1539.
[11]安良成,谢继东,张堃,等.简述ZSM-5分子筛水热合成工艺[J].石油化工应用,2014,33(2):113-116.
[12]白妮,孟桂花.纳米ZSM-5沸石合成方法及应用[J].纳米科技,2005,(6):53-56.
[13]郑恒.改性ZSM分子筛上苯和甲醇烷基化反应研究[D].北京:北京化工大学,2017.
[14]王守桂.NaOH处理对ZSM-5催化环己烯水合制环己醇反应性能影响的研究[D].天津:天津大学,2016.
[15]Cihanoˇglu A,Gündüz G,DükkancM.Degradation of acetic acid by heterogeneous Fenton-like oxidation over iron-containing ZSM-5 zeolites[J]. Applied Catalysis B:Environmental,2015,165:687-699.
[16]Rey A,Faraldos M,Casas J A,et al.Catalytic wet peroxide oxidation of phenol over Fe/AC catalysts:Influence of iron precursor and activated carbon surface[J]. Applied Catalysis B:Environmental,2009,86(1-2):69-77.
[17]Sashkina K A,Parkhomchuk E V,Rudina N A,et al.The role of zeolite Fe-ZSM-5 porous structure for heterogeneous Fenton catalyst activity and stability[J]. Microporous and Mesoporous Materials,2014,189:181-188.
[18]卢仁杰,张新艳,郝正平,等.不同硅铝比Fe-ZSM-5催化剂对氧化亚氮催化分解性能的研究[J].环境科学,2014,35(1):371-379.
[19]何莼,徐科峰,奚红霞,等.均相和非均相Fenton型催化剂催化氧化含酚废水[J].2003,31(5):51-55.
[20]池勇志,崔维花,习钰兰,等.Fe/Ce负载型非均相芬顿法催化剂的制备及优化[J].工业用水与废水,2012,43(3):52-57.
[21]赵银秋.非均相Fenton催化剂的制备、表征及性能研究[D].齐齐哈尔:齐齐哈尔大学,2012.
[22]杨春维,王栋,王坤,等.非均相Fenton反应催化剂的制备及其催化性能[J].化工环保,2011,31(6):557-560.