Visible light-activated N-F-codoped TiO2 nanoparticles for the photocatalytic degradation of microcystin-LR in water

被引:227
作者
Pelaez, Miguel [1 ]
de la Cruz, Armah A. [2 ]
Stathatos, Elias [3 ]
Falaras, Polycarpos [4 ]
Dionysiou, Dionysios D. [1 ]
机构
[1] Univ Cincinnati, Dept Civil & Environm Engn, Cincinnati, OH 45221 USA
[2] US EPA, Off Res & Dev, Cincinnati, OH 45268 USA
[3] Inst Educ Technol, Dept Elect Engn, Patras 26334, Greece
[4] NCSR Demokritos, Inst Phys Chem, Athens 15310, Greece
基金
美国国家科学基金会;
关键词
Visible light; Microcystin-LR; Titanium dioxide; Photocatalysis; Fluorine doping; Nitrogen doping; Sol-gel method; NITROGEN-DOPED TIO2; FLUORINATED SURFACTANT; DRIVEN PHOTOCATALYSIS; FILMS; POWDERS;
D O I
10.1016/j.cattod.2008.12.022
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
In this study, we developed nonmetal-doped TiO2 nanoparticles (N-F-TiO2) by a novel synthesis route employing a simple sol-gel method containing a nonionic fluorosurfactant as pore template material to tailor-design the structural properties of TiO2 and fluorine dopant as well as ethylenediamine as nitrogen source for the photocatalytic response towards visible light. The synthesized photocatalyst was characterized by XRD, UV-vis spectroscopy, XPS, HR-TEM, ESEM and porosimetry measurements. The resulting nanoparticles exhibited enhanced structural properties such as high surface area (141 m(2)/g), high porosity (49%), mesoporous structure (2-10 nm pore size) and low degree of agglomeration (1.07). A reduction in the effective band gap (2.75 eV) was observed compared with reference TiO2 (3.00 eV) due to the red-shift in the optical absorption spectrum of the nonmetal-doped TiO2 photocatalyst. We also focused on the environmental application of the prepared nanoparticles for the destruction of microcystin-LR (MC-LR) under visible light irradiation (lambda > 420 nm). Under acidic conditions (pH 3.0 +/- 0.1), the highest MC-LR degradation rate was achieved with N-F-TiO2. The electrostatic interactions between the toxin and the N-F-codoped TiO2 favored the photocatalytic degradation. Beneficial effects induced by codoping with nitrogen and fluorine are responsible for higher photocatalytic activity than TiO2 nanoparticles with only fluorine or nitrogen doping. Also, commercially available visible light-activated TiO2 showed lower degradation rate per unit surface area of the material. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:19 / 25
页数:7
相关论文
共 37 条
[21]   Structural and optoelectronic characterization of TiO2 films prepared using the sol-gel technique [J].
Jimenez Gonzalez, A. E. ;
Gelover Santiago, S. .
SEMICONDUCTOR SCIENCE AND TECHNOLOGY, 2007, 22 (07) :709-716
[22]  
Kissa E., 2001, Fluorinated Surfactants and Repellents, P233
[23]   Nitrogen modified nanostructured titania: electronic, structural and visible-light photocatalytic properties [J].
Kontos, A. I. ;
Kontos, A. G. ;
Raptis, Y. S. ;
Falaras, P. .
PHYSICA STATUS SOLIDI-RAPID RESEARCH LETTERS, 2008, 2 (02) :83-85
[24]   Origin of visible-light-driven photocatalysis:: A comparative study on N/F-doped and N-F-codoped TiO2 powders by means of experimental characterizations and theoretical calculations [J].
Li, D ;
Ohashi, N ;
Hishita, S ;
Kolodiazhnyi, T ;
Haneda, H .
JOURNAL OF SOLID STATE CHEMISTRY, 2005, 178 (11) :3293-3302
[25]   Visible-light-driven photocatalysis on fluorine-doped TIO2 powders by the creation of surface oxygen vacancies [J].
Li, D ;
Haneda, H ;
Labhsetwar, NK ;
Hishita, S ;
Ohashi, N .
CHEMICAL PHYSICS LETTERS, 2005, 401 (4-6) :579-584
[26]   Bactericidal activity of nitrogen-doped metal oxide nanocatalysts and the influence of bacterial extracellular polymeric substances (EPS) [J].
Liu, Yang ;
Li, Jin ;
Qiu, Xiaofeng ;
Burda, Clemens .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2007, 190 (01) :94-100
[27]   Destruction of cyanobacterial toxins by semiconductor photocatalysis [J].
Robertson, PKJ ;
Lawton, LA ;
Munch, B ;
Rouzade, J .
CHEMICAL COMMUNICATIONS, 1997, (04) :393-394
[28]   Synthesis, characterization, electronic structure, and photocatalytic activity of nitrogen-doped TiO2 nanocatalyst [J].
Sathish, M ;
Viswanathan, B ;
Viswanath, RP ;
Gopinath, CS .
CHEMISTRY OF MATERIALS, 2005, 17 (25) :6349-6353
[29]   Nanomaterials and water purification: Opportunities and challenges [J].
Savage, N ;
Diallo, MS .
JOURNAL OF NANOPARTICLE RESEARCH, 2005, 7 (4-5) :331-342
[30]  
Schubert U, 2005, J MATER CHEM, V15, P3701, DOI [10.1039/b504269k, 10.1039/B504269K]