流化床—石英光纤光催化装置的建立及其应用
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摘要
针对现有光催化反应器中光传输效率低、光子、反应物、催化剂三者不能有效接触的缺点,本论文开展了新型光催化反应器的设计,搭建了流化床-光纤光催化反应装置,进行了光催化反应器的性能优化和测试,利用该装置进行了甲醛光催化氧化的研究,并得到了一系列有意义的结果。研究内容主要包括:
(1)设计了流化床-光纤光催化反应系统,包括整体气路的设计、流化床设计和光纤光源设计。整体气路由气体发生器、气体混合室、光催化反应器、检测系统等组成。流化床反应器外形为圆柱形,流化床直径10mm、高度100mm;扩大段直径16mm、高度16mm;分离段高度120mm、出口段高度50mm;反应器总长426mm。以橡胶板固定光纤,光源系统的的组成为每平面8个光纤孔,上下间距3.4mm。气路中,对光催化反应器影响重要的有入口管路口径和气体分布板,分别选取了直径2mm和400目。
(2)对新设计和搭建的流化床-光纤光催化反应装置进行了性能优化和测试,主要从流化床流态影响、光强的影响等方面来进行优化,在催化剂粒径为60~120目、气体总流量为180mL/min、流化床的静床层高度为68mm时,流化床高度为90mm,得到最好的流态效果。以丙酮和TCE作为研究对象,在最优条件时进行光催化,得到丙酮的光催化降解率为69.9%、光量子效率为3.46%,反应速率为3.98μmol/(g催化剂·min)。三氯乙烯的光催化降解率可以达到100%、光量子效率为4.66%,反应速率为4.55μmol/(g催化剂·min)。与以往的固定床光纤光催化反应器和流化床光催化反应器进行了对比,流化床-光纤光催化反应器具有更优的光催化性能。
(3)利用流化床-光纤光催化反应系统进行了甲醛的光催化降解研究,降解率可以达到85.71%,光量子效率为7.95%,反应速率为6.44μmol/(g催化剂·min)。
The optical transmission efficiency of the present photo catalytic reactor is low and the contact of photon-reactants-catalyst is bad. In view of this situation, this paper aims at designing a new-type photocatalytic reactor to take a good contact among photo-reactants-catalyst. A fluidized-bed optical fiber photocatalytic reactor is set up, the performance optimizing and testing of the photocatalytic reactor have been carried out. Furethermore, this reactor can be applied to do the research in the photocatalytic oxidation of formaldehyde.The research can be summarized as following.
(1) Design of fluidized bed-optical fiber photo catalytic reactor, which includes the design of the overall gas route, and the light for optical fiber. The overall gas route consists of gas generator, gas mixing chamber, photo catalytic reactor and detection system. Fluidized-bed is cylindrical, the diameter of fluidized section is 10mm, and height is 100mm. The diameter and height of expanded section are both 16mm. The height of the other part of this reactor as following, the separate section is 120mm, and export section is 50mm. The totoal height of reactor is 426mm. The optical fibers are fixed on rubber plate. The light system is composed of 8 optical fibers in each plane, and the pitch between every two plane is 3.4mm. In gas route, diameter and the gas distribution plate have important impact to photo catalytic reactor. The diameter of the entrance pipe is 2mm and the gas distribution plate is 400 mesh.
(2) The performance of new photo catalytic reactor has been optimized and tested. The flow pattern and light intensity of the fluidized-bed are main optimizing factors. If the catalyst particle is 60~120 mesh the total flow of gas is 180mL/min, and the static bed height of fluidized-bed is 68mm, the optimal flow pattern can be known, and then, the height of fluidized-bed can be measured as 90mm. Choosing acetone and TCE as the object pollutants, under optimal conditions, the conversion of acetone is 69.9%, quantum efficiency is 3.46%, and steady-state reaction rate is 3.98μmol of acetone (g of catalyst)-1min-1.The conversion of TCE is 100%, the quantum efficiency is 4.66%, and the steady-state reaction rate is 4.55μmol of TCE (g of catalyst)-1min-1. Compared to traditional fixed optical fiber photo catalytic reactor and fluidized-bed photo catalytic reactor, the new reactor has more excellent photo catalytic properties.
(3) The application of this new reactor to degrade formaldehyde. The conversion of formaldehyde can reach 85.71%, the quantum efficiency is 7.95%, and steady-state reaction rate is 6.44μmol of formaldehyde (g of catalyst)-1min-1.
(1)设计了流化床-光纤光催化反应系统,包括整体气路的设计、流化床设计和光纤光源设计。整体气路由气体发生器、气体混合室、光催化反应器、检测系统等组成。流化床反应器外形为圆柱形,流化床直径10mm、高度100mm;扩大段直径16mm、高度16mm;分离段高度120mm、出口段高度50mm;反应器总长426mm。以橡胶板固定光纤,光源系统的的组成为每平面8个光纤孔,上下间距3.4mm。气路中,对光催化反应器影响重要的有入口管路口径和气体分布板,分别选取了直径2mm和400目。
(2)对新设计和搭建的流化床-光纤光催化反应装置进行了性能优化和测试,主要从流化床流态影响、光强的影响等方面来进行优化,在催化剂粒径为60~120目、气体总流量为180mL/min、流化床的静床层高度为68mm时,流化床高度为90mm,得到最好的流态效果。以丙酮和TCE作为研究对象,在最优条件时进行光催化,得到丙酮的光催化降解率为69.9%、光量子效率为3.46%,反应速率为3.98μmol/(g催化剂·min)。三氯乙烯的光催化降解率可以达到100%、光量子效率为4.66%,反应速率为4.55μmol/(g催化剂·min)。与以往的固定床光纤光催化反应器和流化床光催化反应器进行了对比,流化床-光纤光催化反应器具有更优的光催化性能。
(3)利用流化床-光纤光催化反应系统进行了甲醛的光催化降解研究,降解率可以达到85.71%,光量子效率为7.95%,反应速率为6.44μmol/(g催化剂·min)。
The optical transmission efficiency of the present photo catalytic reactor is low and the contact of photon-reactants-catalyst is bad. In view of this situation, this paper aims at designing a new-type photocatalytic reactor to take a good contact among photo-reactants-catalyst. A fluidized-bed optical fiber photocatalytic reactor is set up, the performance optimizing and testing of the photocatalytic reactor have been carried out. Furethermore, this reactor can be applied to do the research in the photocatalytic oxidation of formaldehyde.The research can be summarized as following.
(1) Design of fluidized bed-optical fiber photo catalytic reactor, which includes the design of the overall gas route, and the light for optical fiber. The overall gas route consists of gas generator, gas mixing chamber, photo catalytic reactor and detection system. Fluidized-bed is cylindrical, the diameter of fluidized section is 10mm, and height is 100mm. The diameter and height of expanded section are both 16mm. The height of the other part of this reactor as following, the separate section is 120mm, and export section is 50mm. The totoal height of reactor is 426mm. The optical fibers are fixed on rubber plate. The light system is composed of 8 optical fibers in each plane, and the pitch between every two plane is 3.4mm. In gas route, diameter and the gas distribution plate have important impact to photo catalytic reactor. The diameter of the entrance pipe is 2mm and the gas distribution plate is 400 mesh.
(2) The performance of new photo catalytic reactor has been optimized and tested. The flow pattern and light intensity of the fluidized-bed are main optimizing factors. If the catalyst particle is 60~120 mesh the total flow of gas is 180mL/min, and the static bed height of fluidized-bed is 68mm, the optimal flow pattern can be known, and then, the height of fluidized-bed can be measured as 90mm. Choosing acetone and TCE as the object pollutants, under optimal conditions, the conversion of acetone is 69.9%, quantum efficiency is 3.46%, and steady-state reaction rate is 3.98μmol of acetone (g of catalyst)-1min-1.The conversion of TCE is 100%, the quantum efficiency is 4.66%, and the steady-state reaction rate is 4.55μmol of TCE (g of catalyst)-1min-1. Compared to traditional fixed optical fiber photo catalytic reactor and fluidized-bed photo catalytic reactor, the new reactor has more excellent photo catalytic properties.
(3) The application of this new reactor to degrade formaldehyde. The conversion of formaldehyde can reach 85.71%, the quantum efficiency is 7.95%, and steady-state reaction rate is 6.44μmol of formaldehyde (g of catalyst)-1min-1.
引文
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2汪军.纳米二氧化钛的光催化机理及其应用研究.污染防治技术. 1998, 11(3):l57~160
3 J. E.R. Carraway, A.J. Hoffman, M.R. Hoffmann. Photocatalytic Oxidation of Organic-Acids on Quantum-Sized Semiconductor Colloids. Environmental Science & Technology. 1994, 28(5): 786~793
4 H. Gerischer, A. Heller. Photocatalytic Oxidation of Organic-Molecules at TiO2 Particles by Sunlight in Aerated Water. Journal of the Electrochemical Society. 1992, 139(1): 113~118
5王桂茹,张颖,杨凌霄. 98全国光催化化学学术论文摘要集.北京:中国化学会出版社, 1998:94~97
6 Kamat P V. Photochemistry on nonreactive and reactive (semiconductor) surfaces. Chem Rev. 1993, 93(1): 267~300
7 Andrew Mills, Slephen Le Hunte. An over View of Semiconductor photobiology. J.Photobiology A. 1997, 108:1~35
8郭建平,刘祖武,郭军等.纳米TiO2光催化氧化机理及研究.天津化工. 2003, 17(4):1~3
9 A.L. Linsebigler, G.Q. Lu, J.T. Yates. Photocatalysis on TiO2 Surfaces-Principles, Mechanism, and Selected Results. Chemical Reviews. 2005, 95(3): 735~758
10沈迅伟,袁春伟.基于二氧化钛多相光催化的环境净化技术研究及进展.东南大学学报(自然科学版). 2004, (6):872~878
11 Hong Fei Lin, Kalliat T. Valsaraj, et al. A titania thin film annular photocatalytic reactor for degradation of polycyclic aromatic hydrocarbons in dilute water streams. Journal of Hazardous Materials B. 2003, 99(2):203~219
12 Kuo Hua Wang, Yunghsu Hsieh, et al. The photocatalytic degradation of trichloroethane by chemical vapor deposition method prepared titanium dioxide catalyst. Journal of Hazardous Materials B, 2002, 95(1~2):161~174
13尹晓红,辛峰,张凤宝等.转筒式负载膜光催化反应器及用于降解4BS染料的研究.化学反应工程与工艺. 2005, 21(6):560~565
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