将Keggin型铁取代杂多阴离子PW11O39Fe(Ⅲ)(H2O)4-[ PW11Fe(Ⅲ)(H2O)]构成的类光-芬顿体系用于水体生物难降解有机污染物苯胺( ArNH2)的降解.研究了在紫外光照射和H2O2存在下,PW11Fe(Ⅲ)(H2O)对ArNH2降解的均相光催化作用.考察了ArNH2、H2O2和PW11Fe(Ⅲ)(H2O)浓度对光催化降解反应速率的影响.实验结果表明,0.1 mmol/L PW11Fe(Ⅲ)(H2O) +0.2 mmol/L H2O2 +0.1 mmol/L ArNH2的中性溶液在300 W汞灯照射下反应60 min,ArNH2的降解率达100%,总有机碳(TOC)去除约52%.同时讨论了PW11Fe(Ⅲ)(H2O)光催化H2O2产生羟基自由基的分子机制,并比较了酸性和中性条件下苯胺的光催化降解效果.
参考文献
[1] | ZHANG Lanying,LIU Na,SUN Libo.Modem Environment Microorganism Technology[M].Beijing:QingHua University Press,2005:7-9(in Chinese).张兰英,刘娜,孙立波.现代环境微生物技术[M].北京:清华大学出版社,2005:7-9. |
[2] | Haigler B E,Spain J C.Biotransformation of Nitrobenzene by Bacteria Containing Toluene Degradation Pathways[J].Appl Environ Microbiol,1991,57(11):3156-3161. |
[3] | Kamble S P,Sawant S B,Schouten J C,et al.Photocatalytic and Photochemical Degradation of Aniline Using Concentrated Solar Radiation[J].J Chem Technol Biotechnol,2003,78(7):865-872. |
[4] | Brillas E,Sires I,Oturan M A.Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton's Reaction Chemistry[J].Chem Rev,2009,109(12):6570-6631. |
[5] | Sanchez-Sanchez C M,Exposito E,Casado J,et al.Goethite as a More Effective Iron Dosage Source for Mineralization of Organic Pollutants by Electro-Fenton Process[J].Electrochem Commun,2007,9(1):19-24. |
[6] | Brillas E,Boye B,Sires I,et al.Electrochemical Destruction of Chlorophenoxy Herbicides by Anodic Oxidation and ElectroFenton Using a Boron-doped Diamond Electrode[J].Electrochim Acta,2004,49(25):4487-4496. |
[7] | Oturan M A,Peiroten J,Chartrin P,et al.Complete Destruction of p-Nitrophenol in Aqueous Medium by Electro-Fenton Method[J].Environ Sci Technol,2000,34(16):3474-3479. |
[8] | Zhao X K,Yang G P,Wang Y J,et al.Photochemical Degradation of Dimethyl Phthalate by Fenton Reagent[J].Photochem Photobiol,A Chem,2004,161 (3):215-220. |
[9] | Fukushima M,Tatsumi K,Morimoto K.The Fate of Aniline after a Photo-Fenton Reaction in an Aqueous System Containing Iron(Ⅲ),Humic Acid,and Hydrogen Peroxide[J].Environ Sci Technol,2000,34(10):2006-2013. |
[10] | WANG Chongtai,SUN Zhenfan,HUA Yingjie,et al.Photocatalytic Degradation of Nitrobenzene with Keggin-type Fe(Ⅲ)-Substituted Heteropolyanion PW11O39Fe(Ⅲ) (H2O)4-[J].Acta Chim Sin,2010,68(11):1037-1042(in Chinese).王崇太,孙振范,华英杰,等.Keggin型铁取代杂多阴离子PW11O39Fe(Ⅲ)(H2O)4-光催化降解硝基苯[J].化学学报,2010,68(11):1037-1042 |
[11] | Toth J E,Anson F C.Electrochemical Properties of Iron (Ⅲ)-substituted Heteropolytungstate Anions[J].J Electroanal Chem,1988,256(2):361-370. |
[12] | Toth J E,Anson F C. Electrocatalytic Reduction of Nitrite and Nitric Oxide to Ammonia with Iron-Substituted Polyoxotungstates[J].J Am Chem Soc,1989,111 (7):2444-2451. |
[13] | HUA Yingjie,WANG Chongtai,YANG Xue,et al.Adsorption Properties of Keggin-type Fe(Ⅲ)-substituted Heteropolyanion by D301 R Resin[J].Acta Chim Sin,2009,67 (5):355-360 (in Chinese).华英杰,王崇太,杨雪,等.D301R树脂对Keggin型铁取代杂多阴离子的吸附性能研究[J].化学学报,2009,67(5):355-360. |
[14] | Zonnevijlle F,Tourné C M,Tourné G F.Preparation and Characterization of Iron(Ⅲ)-and Rhodium(Ⅲ)-Containing Heteropolytungstates Identification of Novel Oxo-Bridged Iron (Ⅲ) Dimers[J].Inorg Chem,1982,21 (7):2751-2757. |
[15] | Brevard C,Schimpf R,Toumé G,et al.Tungsten-183 NMR:A Complete and Unequivocal Assignment of the Tungstentungsten Connectivities in Heteropolytungstates via Two-dimensional 183W NMR Techniques[J].J Am Chem Soc,1983,105(24):7059-7063. |
[16] | Oturan M A,Pinson J.Hydroxylation by Electrochemically Generated OH Radicals.Mono-and Polyhydroxylation of Benzoic Acid:Products and Isomers' Distribution[J].J Phys Chem B,1995,99 (38):13948-13954. |
[17] | Wang Chongtai,Hua Yingjie,Tong Yexiang.A Novel Electro-Fenton-Like System Using PW11O39Fe(Ⅲ) (H2O)4-as an Electrocatalyst for Wastewater Treatment[J].Electrochim Acta,2010,55 (22):6755-6760. |
[18] | Wang Chongtai,Hua Yingjie,Li Gaoren,et al.Indirect Cathodic Electrocatalytic Degradation of Dimethylphthalate with PW11O39Fe(Ⅲ)(H2O)4-and H2O2 in Neutral Aqueous Medium[J].Electrochim Acta,2008,53(16):5100-5105.. |
[19] | Diagne M,Oturan N,Oturan M A.Removal of Methyl Parathion from Water by Electrochemically Generated Fenton's Reagent[J].Chemosphere,2007,66 (5):841-848. |
[20] | Rong C Y,Pope M T.Lacunary Polyoxometalate Anions are-Π-Acceptor Ligands.Characterization of Some Tungstoruthenate (Ⅱ,Ⅲ,Ⅳ,Ⅴ) Heteropolyanions and Their Atom-transfer Reactivity[J].J Am Chem Soc,1992,114 (8):2932-2938. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%