以Keggin型铜取代杂多阴离子PW11O39Cu(Ⅱ)(H2O)5-[PW11Cu]为可见光催化剂,有机染料罗丹明B(RhB)为模型污染物,研究了在可见光照射下PW11Cu对RhB的可见光催化降解作用,提出了PW11 Cu可见光催化作用的反应机理,同时考察了RhB初始浓度、PW11Cu初始浓度和溶液pH值对RhB光催化降解速率的影响.实验结果表明,含有15.6 μmol/L PW11Cu+ 10 μmol/L RhB的水溶液在可见光照射下反应80 min,RhB的降解率达100%,总有机碳去除率约33%.RhB的可见光催化降解服从准一级动力学方程,在RhB初始浓度为20、30和40 μmol/L的情况下,其表观一级速率常数分别为3.1 ×10-2、2.0×10-2和1.5×10-2 min-1.
参考文献
[1] | Mills A,Hunte S L.An Overview of Semiconductor Photocatalysis[J].J Photochem Photobiol A,1997,108:1-35. |
[2] | Chen C,Zhao W,Lei P,et al.Photosensitized Degradation of Dyes in Polyoxometalate Solutions versus TiO2 Dispersions under Visible-Light Irradiation:Mechanistic Implications[J].Chem Eur J,2004,10:1956-1965. |
[3] | Huang H Y,Gu X T,Zhou J H,et al.Photocatalytic Degradation of Rhodamine B on TiO2 Nanoparticles Modified with Porphyrin and Iron-porphyrin[J].Catal Commun,2009,11:58-61. |
[4] | Yin M C,Li Z S,Kou J H,et al.Mechanism Investigation of Visible Light-Induced Degradation in a Heterogeneous TiO2/Eosin Y/Rhodamine B System[J].Environ Sci Technol,2009,43:8361-8366. |
[5] | Zhao D,Chen C C,Wang Y F,et al.Enhanced Photocatalytic Degradation of Dye Pollutants under Visible Irradiation on Al (Ⅲ)-Modified TiO2:Structure,Interaction,and Interfacial Electron Transfer[J].Environ Sci Technol,2008,42:308-314. |
[6] | Aarthi T,Madras G.Photocatalytic Degradation of Rhodamine Dyes with Nano-TiO2[J].Ind Eng Chem Res,2007,46:7-14. |
[7] | Lu S Y,Wu D,Wang Q L,et al.Photocatalytic Decomposition on Nano-TiO2:Destruction of Chloroaromatic Compounds[J].Chemosphere,2011,82:1215-1224. |
[8] | Yu H T,Quan X,Chen S,et al.TiO2-Carbon Nanotube Heterojunction Arrays with a Controllable Thickness of TiO2 Layer and Their First Application in Photocatalysis[J].J Photochem Photobiol A,2008,200:301-306. |
[9] | Slimen H,Houas A,Nogier J P.Elaboration of Stable Anatase TiO2 Through Activated Carbon Addition with High Photocatalytic Activity under Visible Light[J].J Photochem Photobiol A,2011,221:13-21. |
[10] | Wang F,Zhang K.Reduced Graphene Oxide-TiO2 Nanocomposite with High Photocatalystic Activity for the Degradation of Rhodamine B[J].J Mol Catal A,2011,345:101-107. |
[11] | Yu K,Yang S G,He H,et al.Visible Light-Driven Photocatalytic Degradation of Rhodamine B over NaBiO3:Pathways and Mechanism[J].J Phys Chem A,2009,113:10024-10032. |
[12] | Li W J,Li D Z,Chen Z X,et al.High-efficient Degradation of Dyes by Znx Cd1-xS Solid Solutions under Visible Light Irradiation[J].J Phys Chem C,2008,112:14943-14947. |
[13] | Wu K Q,Xie Y D,Zhao J C,et al.Photo-Fenton Degradation of a Dye under Visible Light Irradiation[J].J Mol Catal A,1999,144:77-84. |
[14] | Fukushima M,Tatsumi K.Degradation Pathways of Pentachlorophenol by Photo-Fenton Systems in the Presence of Iron (Ⅲ),Humic Acid,and Hydrogen Peroxide[J].Environ Sci Technol,2001,35:1771-1778. |
[15] | Chambers R,Hill C.Comparative Study of Polyoxometalates and Semiconductor Metal Oxides as Catalysts:PhotochemicalOxidative Degradation of Thioethers[J].Inorg Chem,199l,30(13):2776-2781. |
[16] | Hiskia A,Mylonas A,Papaconstantinou E.The Comparison of the Photoredox Properties of Polyoxometallates and Semiconducting Particles[J].Chem Soc Rev,2001,30:62-69. |
[17] | Hiskia A,Ecke M,Troupis A,et al.Sonolytic,Photolytic,and Photocatalytic Decomposition of Atrazine in the Presence of Polyoxometalates[J].Environ Sci Technol,2001,35 (11):2358-2364. |
[18] | Troupis A,Triantis T M,Gkika E,et al.Photocatalytic Reductive-Oxidative Degradation of Acid Orange 7 by Polyoxometalates[J].Appl Catal B,2009,86(2):98-107. |
[19] | WANG Chongtai,SUN Zhengfan,HUA Yingjie,et al.Photocatalytic Degradation of Nitrobenzene with Keggin-type Fe(Ⅲ)-Substituted Heteropolyanion PW11O39 Fe (Ⅲ) (H2 O) 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PW11 O39Fe(Ⅲ)(H2O)4-光催化降解硝基苯[J].化学学报,2010,68(11):1037-1042. |
[20] | Hu X F,Mohamood T,Ma W H,et al.Oxidative Decomposition of Rhodamine B Dye in the Presence of VO+2 and/or Pt(Ⅳ) under Visible Light Irradiation:N-Deethylation,Chromophore Cleavage,and Mineralization[J].J Phys Chem B,2006,110:26012-26018. |
[21] | Chong Meng Nan,Jin Bo,Chow Christopher W K,et al.Recent Developments in Photocatalytic Water Treatment Technology:A Review[J].Water Res,2010,44:2997-3027. |
[22] | Zonnevijlle F,Tournè C M,Toumè G F.Preparation and Characterization of Iron (Ⅲ)-and Rhodium (Ⅲ)-containing Heteropolytungstates:Identification of Novel oxo-Bridged Iron (Ⅲ) Dimmers[J].Inorg Chem,1982,21 (7):2751-2757. |
[23] | WANG Enbo,HU Changwen,XU Lin.An Introduction to Polyacid Chemistry[M].Bejing:Chemical Industry Press,1998:16(in Chinese).王恩波,胡长文,许林著.多酸化学导论[M].北京:化工出版社,1998:16. |
[24] | Wang C T,Hua Y J,Li G R,et al.Indirect Cathodic Electrocatalytic Degradation of Dimethylphthalate with PW11O39Fe(Ⅲ) (H2O)4-and H2O2 in Neutral Aqueous Medium[J].Electrochim Acta,2008,53:5100-5105. |
[25] | HUA Yingjie,WANG Chongtai,TONG Yexiang,et al.Electrocatalytic Degradation of Nitrobenzene with Keggin-type PW11 O39 Fe (Ⅲ) (H2O) 4-[J].Acta Chim Sin,2009,67 (23):2650-2654 (in Chinese).华英杰,王崇太,童叶翔,等.Keggin型杂多阴离子PW11O33Fe(Ⅲ)(H2O)4-电催化降解硝基苯[J].化学学报,2009,67 (23):2650-2654. |
[26] | Wang C T,Hua Y J,Tong Y X,et al.A Novel Electro-Fenton-Like System Using PW11 O39 Fe (Ⅲ) (H2 O)4-as an Electrocatalyst for Wastewater Treatment[J].Electrochim Acta,2010,55 (22):6755-6760. |
[27] | Rong C Y,Pope M T.Lacunary Polyoxometalate Anions are Ⅱ-Acceptor Ligands.Characterization of Some Tungstoruthenate (Ⅱ,Ⅲ,Ⅳ,Ⅴ) Heteropolyanions and Their Atom-transfer Reactivity[J].J Am Chem Soc,1992,114:2932-2938. |
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%