膜催化处理废气中一氧化氮的性能及机制
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摘要
以聚砜(PSF)中空纤维膜为载体采用溶胶-凝胶法制备了Fe-TiO_2/PSF中空纤维复合膜催化剂,考察其光催化模拟烟气中NO的脱除性能。实验条件下,紫外光照射时NO去除率可达35%。采用X-射线光电子能谱(XPS)和傅里叶变换红外光谱(FT-IR)表征了Fe-TiO_2/PSF中空纤维复合膜催化剂,结果表明,膜催化反应中存在·OH自由基、NO_3~-等物质。Fe-TiO_2/PSF膜催化处理NO的作用机制为NO经膜孔吸附到催化剂表面,被Fe-TiO_2膜光催化反应产生的自由基团氧化成NO_2及HNO_2,经进一步氧化形成最终产物HNO_3。Fe-TiO_2/PSF膜光催化处理NO气体遵循Langmuir-Hinshelwood动力学模型。
Fe-doped titanium dioxide( Fe-TiO_2) was prepared by the sol-gel method and was loaded on a polysulfone( PSF) hollow fiber membrane. Fe-TiO_2/PSF was used for the treatment of NOxunder light irradiation.NO removal efficiency reached 35% under ultraviolet( UV) irradiation. X-ray photoelectron spectroscopy( XPS) and Fourier transform infrared spectrometry( FT-IR) were used to characterize the prepared Fe-TiO_2/PSF. The results of FT-IR and XPS revealed that hydroxyl radicals( OH) and nitrate ions( NO_3~-) were found after the photocatalytic reaction. The membrane bioreactor degradation of NO can be described as a combination of membrane mass transfer and photocatalytic oxidation. NO was mass transferred through fenestrae to the surface of catalyst,then oxidized into NO_2 and HNO_2 by free radicals,which in turn became HNO_3. The membrane photocatalytic oxidation reaction of NO with the Fe-TiO_2/PSF catalyst followed Langmuir-Hinshelwood kinetics.
Fe-doped titanium dioxide( Fe-TiO_2) was prepared by the sol-gel method and was loaded on a polysulfone( PSF) hollow fiber membrane. Fe-TiO_2/PSF was used for the treatment of NOxunder light irradiation.NO removal efficiency reached 35% under ultraviolet( UV) irradiation. X-ray photoelectron spectroscopy( XPS) and Fourier transform infrared spectrometry( FT-IR) were used to characterize the prepared Fe-TiO_2/PSF. The results of FT-IR and XPS revealed that hydroxyl radicals( OH) and nitrate ions( NO_3~-) were found after the photocatalytic reaction. The membrane bioreactor degradation of NO can be described as a combination of membrane mass transfer and photocatalytic oxidation. NO was mass transferred through fenestrae to the surface of catalyst,then oxidized into NO_2 and HNO_2 by free radicals,which in turn became HNO_3. The membrane photocatalytic oxidation reaction of NO with the Fe-TiO_2/PSF catalyst followed Langmuir-Hinshelwood kinetics.
引文
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[3]LASEK J,YU Yihui,WU J C S.Removal of NOxby photocatalytic processes[J].Journal of Photochemistry and Photobiology C:Photochemistry Reviews,2013,14:29-52
[4]ZHANG Jinlong,WU Yongmei,XING Mingyang,et al.Development of modified N doped Ti O2photocatalyst with metals,nonmetals and metal oxides[J].Energy&Environmental Science,2010,3(6):715-726
[5]CHEN M S,GOODMAN D W.The structure of catalytically active gold on Titania[J].Science,2004,306(5694):252-255
[6]LEE Y,GARCIA M A,HULS N A F,et al.Synthetic tuning of the catalytic properties of Au-Fe3O4nanoparticles[J].Angewandte Chemie International Edition,2010,49(7):1271-1274
[7]WU Qingping,YANG C C,VAN DE KROL R.A dopant-mediated recombination mechanism in Fe-doped Ti O2nanoparticles for the photocatalytic decomposition of nitric oxide[J].Catalysis Today,2014,225:96-101
[8]GOEI R,LIM T T.Asymmetric Ti O2hybrid photocatalytic ceramic membrane with porosity gradient:Effect of structure directing agent on the resulting membranes architecture and performances[J].Ceramics International,2014,40(5):6747-6757
[9]LI Landong,SHEN Qun,CHENG Jie,HAO Zhengping.Catalytic oxidation of NO over Ti O2supported platinum clusters.II:Mechanism study by in situ FTIR spectra[J].Applied Catalysis B:Environmental,2010,93(3/4):259-266
[10]ZHAO Ya,LIU Zhijun,LIU Fengxia,et al.Cometabolic degradation of trichloroethylene in a hollow fiber membrane reactor with toluene as a substrate[J].Journal of Membrane Science,2011,372(1/2):322-330
[11]ZHANG Dieqing,WEN Meicheng,ZHANG Shanshan,et al.Au nanoparticles enhanced rutile Ti O2nanorod bundles with high visible-light photocatalytic performance for NO oxidation[J].Applied Catalysis B:Environmental,2014,147:610-616
[12]DEVAHASDIN S,FAN JR C,LI K,et al.Ti O2photocatalytic oxidation of nitric oxide:Transient behavior and reaction kinetics[J].Journal of Photochemistry and Photobiology A:Chemistry,2003,156(1/2/3):161-170
[13]WANG Haiqiang,WU Zhongbiao,ZHAO Weirong,et al.Photocatalytic oxidation of nitrogen oxides using Ti O2loading on woven glass fabric[J].Chemosphere,2007,66(1):185-190
[14]SOYLU A M,POLAT M,ERDOGAN D A,et al.Ti O2-Al2O3binary mixed oxide surfaces for photocatalytic NOxabatement[J].Applied Surface Science,2014,318:142-149
[15]DE MELO J V S,TRICHêS G,GLEIZE P J P,et al.Development and evaluation of the efficiency of photocatalytic pavement blocks in the laboratory and after one year in the field[J].Construction and Building Materials,2012,37:310-319
[16]NAKAMURA I,NEGISHI N,KUTSUNA S,et al.Role of oxygen vacancy in the plasma-treated Ti O2photocatalyst with visible light activity for NO removal[J].Journal of Molecular Catalysis A:Chemical,2000,161(1/2):205-212
[17]KRUSE N,CHENAKIN S.XPS characterization of Au/Ti O2catalysts:Binding energy assessment and irradiation effects[J].Applied Catalysis A:General,2011,391(1/2):367-376
[18]AMBRUS Z,BALáZS N,ALAPI T,et al.Synthesis,structure and photocatalytic properties of Fe(Ⅲ)-doped Ti O2prepared from Ti Cl3[J].Applied Catalysis B:Environmental,2008,81(1/2):27-37
[19]SHIN J J,LANGFORD S C,DICKINSON J T,et al.Electron stimulated neutral and ion emission from single crystal Na NO3[J].Nuclear Instruments and Methods in Physics Research Section B:Beam Interactions with Materials and Atoms,1995,103(3):284-296
[20]YAN Hongjian,XIE Xionghui,LIU Kewei,et al.Facile preparation of Co3O4nanoparticles via thermal decomposition of Co(NO3)2loading on C3N4[J].Powder Technology,2012,221:199-202
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[23]ANGELO J,ANDRADE L,MADEIRA L M,et al.An overview of photocatalysis phenomena applied to NOxabatement[J].Journal of Environmental Management,2013,129:522-539
[24]ASILTüRK M,SAYILKAN F,ARPAC E.Effect of Fe3+ion doping to Ti O2on the photocatalytic degradation of Malachite Green dye under UV and vis-irradiation[J].Journal of Photochemistry and Photobiology A:Chemistry,2009,203(1):64-71
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