JPH09215910A - Method and apparatus for removing harmful gas - Google Patents
Method and apparatus for removing harmful gasInfo
- Publication number
- JPH09215910A JPH09215910A JP8046887A JP4688796A JPH09215910A JP H09215910 A JPH09215910 A JP H09215910A JP 8046887 A JP8046887 A JP 8046887A JP 4688796 A JP4688796 A JP 4688796A JP H09215910 A JPH09215910 A JP H09215910A
- Authority
- JP
- Japan
- Prior art keywords
- photocatalyst
- light
- harmful gas
- gas
- thickness
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 238000000034 method Methods 0.000 title claims abstract description 29
- 239000007789 gas Substances 0.000 claims abstract description 57
- 230000001678 irradiating effect Effects 0.000 claims abstract description 6
- 239000011941 photocatalyst Substances 0.000 claims description 75
- 229930195733 hydrocarbon Natural products 0.000 abstract description 18
- 150000002430 hydrocarbons Chemical class 0.000 abstract description 13
- 239000003054 catalyst Substances 0.000 abstract description 8
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 abstract description 6
- 229910052753 mercury Inorganic materials 0.000 abstract description 6
- 241000208125 Nicotiana Species 0.000 abstract description 3
- 235000002637 Nicotiana tabacum Nutrition 0.000 abstract description 3
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 abstract description 3
- 238000006303 photolysis reaction Methods 0.000 abstract 2
- 230000015843 photosynthesis, light reaction Effects 0.000 abstract 2
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 43
- 239000010408 film Substances 0.000 description 21
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 14
- 229910010413 TiO 2 Inorganic materials 0.000 description 14
- 239000000463 material Substances 0.000 description 13
- 230000000694 effects Effects 0.000 description 12
- 239000000047 product Substances 0.000 description 12
- 239000010419 fine particle Substances 0.000 description 10
- 238000010586 diagram Methods 0.000 description 9
- 239000011521 glass Substances 0.000 description 9
- 239000004215 Carbon black (E152) Substances 0.000 description 8
- 229910021529 ammonia Inorganic materials 0.000 description 8
- 238000005342 ion exchange Methods 0.000 description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 7
- 239000004065 semiconductor Substances 0.000 description 7
- 239000000126 substance Substances 0.000 description 7
- 235000012431 wafers Nutrition 0.000 description 7
- -1 P bO Inorganic materials 0.000 description 6
- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical compound CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 description 6
- 238000004140 cleaning Methods 0.000 description 6
- 238000011109 contamination Methods 0.000 description 6
- 230000007423 decrease Effects 0.000 description 6
- 239000002245 particle Substances 0.000 description 6
- 239000000758 substrate Substances 0.000 description 6
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 5
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Natural products C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 5
- 229910017604 nitric acid Inorganic materials 0.000 description 5
- 229910052815 sulfur oxide Inorganic materials 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- WZJUBBHODHNQPW-UHFFFAOYSA-N 2,4,6,8-tetramethyl-1,3,5,7,2$l^{3},4$l^{3},6$l^{3},8$l^{3}-tetraoxatetrasilocane Chemical compound C[Si]1O[Si](C)O[Si](C)O[Si](C)O1 WZJUBBHODHNQPW-UHFFFAOYSA-N 0.000 description 4
- 230000005684 electric field Effects 0.000 description 4
- 239000000835 fiber Substances 0.000 description 4
- 230000001699 photocatalysis Effects 0.000 description 4
- 230000000391 smoking effect Effects 0.000 description 4
- 239000010936 titanium Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
- 230000002265 prevention Effects 0.000 description 3
- 239000011265 semifinished product Substances 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 229920000049 Carbon (fiber) Polymers 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 230000002378 acidificating effect Effects 0.000 description 2
- 150000001299 aldehydes Chemical class 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 235000019504 cigarettes Nutrition 0.000 description 2
- 239000011362 coarse particle Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000007796 conventional method Methods 0.000 description 2
- 239000007772 electrode material Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000003365 glass fiber Substances 0.000 description 2
- 150000002576 ketones Chemical class 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 230000007935 neutral effect Effects 0.000 description 2
- 229920000620 organic polymer Polymers 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 238000007788 roughening Methods 0.000 description 2
- 239000002356 single layer Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical class S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 2
- 239000010409 thin film Substances 0.000 description 2
- VXUYXOFXAQZZMF-UHFFFAOYSA-N titanium(IV) isopropoxide Chemical compound CC(C)O[Ti](OC(C)C)(OC(C)C)OC(C)C VXUYXOFXAQZZMF-UHFFFAOYSA-N 0.000 description 2
- 229910052721 tungsten Inorganic materials 0.000 description 2
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 1
- RZVAJINKPMORJF-UHFFFAOYSA-N Acetaminophen Chemical compound CC(=O)NC1=CC=C(O)C=C1 RZVAJINKPMORJF-UHFFFAOYSA-N 0.000 description 1
- 229910017115 AlSb Inorganic materials 0.000 description 1
- 229910015902 Bi 2 O 3 Inorganic materials 0.000 description 1
- 206010007269 Carcinogenicity Diseases 0.000 description 1
- 229910020599 Co 3 O 4 Inorganic materials 0.000 description 1
- QPLDLSVMHZLSFG-UHFFFAOYSA-N CuO Inorganic materials [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910005542 GaSb Inorganic materials 0.000 description 1
- 229910001218 Gallium arsenide Inorganic materials 0.000 description 1
- 206010037660 Pyrexia Diseases 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910002367 SrTiO Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 238000004887 air purification Methods 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 1
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 1
- 235000011130 ammonium sulphate Nutrition 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- 239000011324 bead Substances 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- UHYPYGJEEGLRJD-UHFFFAOYSA-N cadmium(2+);selenium(2-) Chemical compound [Se-2].[Cd+2] UHYPYGJEEGLRJD-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000007670 carcinogenicity Effects 0.000 description 1
- 231100000260 carcinogenicity Toxicity 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000003486 chemical etching Methods 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000007872 degassing Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 231100000676 disease causative agent Toxicity 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- WPYVAWXEWQSOGY-UHFFFAOYSA-N indium antimonide Chemical compound [Sb]#[In] WPYVAWXEWQSOGY-UHFFFAOYSA-N 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- NJPPVKZQTLUDBO-UHFFFAOYSA-N novaluron Chemical compound C1=C(Cl)C(OC(F)(F)C(OC(F)(F)F)F)=CC=C1NC(=O)NC(=O)C1=C(F)C=CC=C1F NJPPVKZQTLUDBO-UHFFFAOYSA-N 0.000 description 1
- 238000006864 oxidative decomposition reaction Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000005297 pyrex Substances 0.000 description 1
- 150000003222 pyridines Chemical class 0.000 description 1
- 150000003233 pyrroles Chemical class 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000002940 repellent Effects 0.000 description 1
- 239000005871 repellent Substances 0.000 description 1
- 238000012552 review Methods 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 230000001953 sensory effect Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000005361 soda-lime glass Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 239000000341 volatile oil Substances 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
Landscapes
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Catalysts (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、有害ガスの除去方
法及び装置に係り、特に、大気中や各種の気体中の有害
ガスを除去する方法及び装置に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method and apparatus for removing harmful gas, and more particularly to a method and apparatus for removing harmful gas in the atmosphere and various gases.
【０００２】[0002]
【従来の技術】従来の技術を各種の工業や産業における
ＮＯｘ、ＳＯｘ及びタバコ臭等の有害ガスを例に説明す
る。先ず、各種の工業及び産業における排ガス及び自動
車の排ガスの大気中への放出については、公害防止の観
点から法的その他の規制措置がとられており、特に窒素
酸化物及び硫黄酸化物については、酸性雨や光化学スモ
ッグの原因物質としてその排出は厳しく制限されてい
る。排出規制の対象とされている排ガス中の窒素酸化物
（ＮＯｘ）や硫黄酸化物（ＳＯｘ）の処理技術は、従来
多くの方式が提案されているが、実用的には種々の課題
がある。たとえば、従来の排ガスの脱硝技術としては、
アンモニア添加による還元法、触媒を使用する還元法、
放射線照射法等が提案されている。2. Description of the Related Art The prior art will be explained by taking harmful gases such as NOx, SOx and tobacco odor in various industries and industries as an example. First of all, regarding the release of exhaust gas from various industries and industries and exhaust gas of automobiles into the atmosphere, legal and other regulatory measures have been taken from the viewpoint of pollution prevention, especially regarding nitrogen oxides and sulfur oxides, Its emission is severely restricted as a causative agent of acid rain and photochemical smog. Many methods have hitherto been proposed for treating nitrogen oxides (NOx) and sulfur oxides (SOx) in exhaust gas, which are subject to emission regulations, but there are various practical problems. For example, as a conventional exhaust gas denitration technology,
Reduction method by adding ammonia, reduction method using catalyst,
Radiation irradiation method and the like have been proposed.
【０００３】従来のこれらの方法は、夫々次のような問
題点がある。 アンモニア添加による還元法：脱硝効
果が低い。 触媒を使用する還元法：連続的に使用し
た場合触媒性能が低下する。触媒として金属、貴金属を
用いているので、省資源の観点から見直す必要がある。
ダストの酸性物質の影響を受けやすい。 放射線照射
法：硝安や硫安のような二次生成物を大量に生ずるの
で、別途副生成物の処理が必要である。また、これらの
いずれの方法もアンモニアの添加を行うので、脱硝反応
で消費されないアンモニアはリークアンモニアとして排
出され、二次公害となる。また、アンモニアの使用、省
資源の観点から見直す必要がある。[0003] Each of these conventional methods has the following problems. Reduction method by adding ammonia: Denitration effect is low. Reduction method using a catalyst: When used continuously, the catalyst performance decreases. Since metals and precious metals are used as catalysts, they need to be reviewed from the viewpoint of resource saving.
Susceptible to acidic substances in dust. Irradiation method: Since secondary products such as ammonium nitrate and ammonium sulfate are generated in large quantities, it is necessary to separately treat by-products. Moreover, since ammonia is added in any of these methods, ammonia that is not consumed in the denitration reaction is discharged as leaked ammonia, which causes secondary pollution. In addition, it is necessary to review the use of ammonia and resource saving.
【０００４】また、これらの有害ガスは一度大気中へ放
出されると、除去困難であり、大気中においても除去で
きる新規方法及び装置の出現が期待されている。次に、
家庭や事務所において喫煙により発生したＮＯｘを含む
有害ガス（臭気性ガスを含む）について説明する。これ
らの物質は、一般にいわゆるタバコ臭として問題にされ
ており、臭気はもちろんその有害性（例、発ガン性）の
ため捕集・除去の要求が近年特に高まっている。これら
の捕集・除去には、活性炭や植物精油を使用したもの等
種々の除去材を使用する方法や装置の提案があるが、こ
れらの除去材はいずれも性能が不十分であり、新規方法
・装置の出現が期待されている。Further, once these harmful gases are released into the atmosphere, it is difficult to remove them, and a new method and apparatus capable of removing them even in the atmosphere are expected to appear. next,
The harmful gas containing NOx (including odorous gas) generated by smoking at home or office will be described. These substances are generally regarded as a so-called cigarette odor, and in recent years, the demand for collection and removal is particularly high because of their harmfulness (eg, carcinogenicity) as well as odor. For the collection and removal of these, there are proposals for methods and devices that use various types of removal materials such as those that use activated carbon and plant essential oils, but these removal materials all have insufficient performance and new methods.・ The appearance of devices is expected.
【０００５】[0005]
【発明が解決しようとする課題】本発明は、上記した従
来技術の問題点を解決し、取扱い易く、コンパクトで安
価で、しかも利用先によっては大気中においても効果的
な有害ガスの除去ができる除去方法とその装置を提供す
ることを目的とする。The present invention solves the above-mentioned problems of the prior art, is easy to handle, is compact and inexpensive, and can effectively remove harmful gas even in the atmosphere depending on the user. It is an object of the present invention to provide a removal method and its device.
【０００６】[0006]
【課題を解決するための手段】上記課題を解決するため
に、本発明では、気体中の有害ガスを除去する方法にお
いて、該気体を、表面に２０〜２００ｎｍ、好ましく
は、５０〜１００ｎｍの厚さの光触媒を担持させた光透
過性支持体の表面に、裏面から光を照射させながら接触
させることとしたものである。また、本発明では、気体
中の有害ガスを除去する装置において、表面に２０〜２
００ｎｍ、好ましくは、５０〜１００ｎｍの厚さの光触
媒を担持させた光透過性支持体と、該支持体の裏面から
光を照射する光源とを有することとしたものである。In order to solve the above problems, in the present invention, in a method for removing harmful gas in a gas, the gas has a thickness of 20 to 200 nm, preferably 50 to 100 nm on the surface. The surface of the light transmissive support supporting the photocatalyst is contacted while irradiating light from the back surface. Further, according to the present invention, in the device for removing harmful gas in the gas, 20 to 2 is provided on the surface.
It has a light-transmissive support having a thickness of 00 nm, preferably 50-100 nm, carrying a photocatalyst, and a light source for irradiating light from the back surface of the support.
【０００７】このように、本発明では、光透過性支持体
の表面に光触媒を担持させ、該裏面より光触媒に光を照
射するものであり、この際の光触媒の厚さが２０〜２０
０ｎｍ、好ましくは５０〜１００ｎｍとした点にある。
すなわち、裏面から光照射を行う本発明の表面の光触媒
膜の厚みは、薄すぎると、光を十分に吸収できない。一
方、厚すぎると、膜中で生じた光キャリヤーが表面まで
拡散できないために、触媒活性が低下する。従って、最
適値が存在することになる。この最適範囲について、本
発明者らは鋭意研究したところ２０〜２００ｎｍ、特に
５０〜１００ｎｍで顕著な活性があることを見い出し本
発明に至った。As described above, in the present invention, the photocatalyst is carried on the surface of the light transmissive support, and the photocatalyst is irradiated with light from the back surface. The thickness of the photocatalyst at this time is 20 to 20.
It is 0 nm, preferably 50 to 100 nm.
That is, if the thickness of the photocatalytic film on the front surface of the present invention in which light is irradiated from the back surface is too thin, light cannot be sufficiently absorbed. On the other hand, if it is too thick, the photocarriers generated in the film cannot diffuse to the surface, and the catalytic activity decreases. Therefore, the optimum value exists. The inventors of the present invention conducted extensive studies on this optimum range and found that the activity was remarkable at 20 to 200 nm, particularly 50 to 100 nm, and the present invention was completed.
【０００８】[0008]
【発明の実施の形態】次に、本発明の各構成を詳細に説
明する。本発明において、照射する光は紫外光及び／又
は可視光が使用でき、太陽光でも人工光でもよい。ここ
での光の照射は、下記支持体の表面に被覆した光触媒
に、該支持体内部に導入した光、すなわち被覆した光触
媒に対して裏面から光照射するものである。光透過性支
持体の材料としては、紫外光及び／又は可視光透過率が
大きなもので有れば何でも用いることができるが、特に
耐光性に優れた石英ガラス、パイレックスガラス、ソー
ダライムガラスなどのガラス材を好適に用いることがで
きる。形状は、板状、シート状、曲面状、柱状、棒状、
線状、網状、格子状、ファイバー状等が使用できる。光
透過性支持体の厚さや太さは、薄いほどあるいは細けれ
ば細い程良いが、強度的には０．１ｍｍ以上の厚さ、あ
るいはφ０．１ｍｍ以上であることが望ましい。また、
上限は無いが、厚いほど、また太くなるほどファイバー
の体積当りの光反応効率は低下することになるが、用途
によっては１０ｍｍ程度でも使用することができる。BEST MODE FOR CARRYING OUT THE INVENTION Next, each structure of the present invention will be described in detail. In the present invention, the irradiation light may be ultraviolet light and / or visible light, and may be sunlight or artificial light. The light irradiation here is to irradiate the photocatalyst coated on the surface of the following support with the light introduced into the support, that is, the coated photocatalyst from the back. As the material of the light-transmissive support, any material having a large transmittance for ultraviolet light and / or visible light can be used, and particularly, quartz glass, Pyrex glass, soda lime glass and the like having excellent light resistance are used. A glass material can be preferably used. The shapes are plate, sheet, curved, columnar, rod-shaped,
A linear shape, a net shape, a lattice shape, a fiber shape or the like can be used. The thickness or thickness of the light transmissive support is better as it is thinner or thinner, but in terms of strength, it is preferably 0.1 mm or more or φ0.1 mm or more. Also,
Although there is no upper limit, the thicker or thicker the photoreaction efficiency per volume of the fiber is lowered, but depending on the application, it can be used even at about 10 mm.
【０００９】また、これらの材料の表面形状は、本発明
者らが既に提案したように、該表面を凹凸状（粗面化）
とすることもできる（特願平６−１７４８９８号）。す
なわち、粗面化により反応速度が向上するので、利用分
野や装置形状、規模、要求性能などによっては好適に用
いることができる。上記の粗面化支持体を用いた光触媒
による作用が効果的になる理由は次の２つの効果に起因
するものである。１つは、平滑表面支持体を用いる場合
に比べて、本発明では表面の凹凸状支持体によって光反
応面積が一層増大することである。他の１つは、光が該
表面の凹凸で散乱されるために、有効に光触媒としての
半導体によって吸収されることである。Further, the surface shapes of these materials are uneven (roughened), as proposed by the present inventors.
(Japanese Patent Application No. 6-174898). That is, since the reaction rate is improved by roughening, it can be preferably used depending on the field of use, the shape of the apparatus, the scale, the required performance and the like. The reason why the action of the photocatalyst using the roughened support is effective is due to the following two effects. One is that in the present invention, the photoreactive area is further increased by the uneven support of the surface, as compared with the case of using the smooth surface support. The other is that the light is effectively absorbed by the semiconductor as a photocatalyst because it is scattered by the unevenness of the surface.
【００１０】なお、光透過性支持体表面の粗面化法とし
ては、特に限定されず、ＨＦ水溶液による化学的エッチ
ング及び研磨材による物理的なスリ加工などを用いれば
良い。凹凸のディメンジョンとしては、紫外及び／又は
可視光を散乱するために、約２００ｎｍ以上が必要にな
る。しかし、凹凸サイズが大きすぎると、反応表面積が
小さくなることから、効率は低下することになる。その
結果、上限は０．１ｍｍであることが望ましい。光透過
性支持体上に担持する光触媒の種類は、対象となる有害
ガス及び光源の種類などを考慮の上、選定することがで
きる。光触媒活性の高さと化学的な安定性から、現在最
も広範に用いられている光触媒はＴｉＯ2 であり、本発
明に好適に使用することができる。しかしながら、本発
明に使用される光触媒はこれに限定されることなく、従
来光触媒として知られているものは如何なるものでも使
用することができる。The method for roughening the surface of the light transmissive support is not particularly limited, and chemical etching with an HF aqueous solution and physical shaving with an abrasive may be used. The dimension of the unevenness needs to be about 200 nm or more in order to scatter ultraviolet and / or visible light. However, if the irregularity size is too large, the reaction surface area becomes small, resulting in a decrease in efficiency. As a result, the upper limit is preferably 0.1 mm. The type of the photocatalyst supported on the light transmissive support can be selected in consideration of the types of target harmful gas and light source. Due to its high photocatalytic activity and chemical stability, the most widely used photocatalyst at present is TiO 2 , which can be suitably used in the present invention. However, the photocatalyst used in the present invention is not limited to this, and any photocatalyst conventionally known as a photocatalyst can be used.
【００１１】通常半導体材料が効果的であり容易に入手
出来、加工性も良いことから好ましい。効果や経済性の
面から、Ｓｅ，Ｇｅ，Ｓｉ，Ｔｉ，Ｚｎ，Ｃｕ，Ａｌ，
Ｓｎ，Ｇａ，Ｉｎ，Ｐ，Ａｓ，Ｓｂ，Ｃ，Ｃｄ，Ｓ，Ｔ
ｅ，Ｎｉ，Ｆｅ，Ｃｏ，Ａｇ，Ｍｏ，Ｓｒ，Ｗ，Ｃｒ，
Ｂａ，Ｐｂのいずれか、又はこれらの化合物、又は合
金、又は酸化物が好ましく、これらは単独で、また二種
類以上を複合して用いる。例えば、元素としてはＳｉ，
Ｇｅ，Ｓｅ、化合物としてはＡｌＰ，ＡｌＡｇ，Ｇａ
Ｐ，ＡｌＳｂ，ＧａＡｓ，ＩｎＰ，ＧａＳｂ，ＩｎＡ
ｓ，ＩｎＳｂ，ＣｄＳ，ＣｄＳｅ，ＺｎＳ，ＭｏＳ2 ，
ＷＴｅ2 ，Ｃｒ2 Ｔｅ3 ，ＭｏＴｅ，Ｃｕ2 Ｓ，Ｗ
Ｓ2 、酸化物としてはＴｉＯ2 ，Ｂｉ2 Ｏ3 ，ＣｕＯ，
Ｃｕ2 Ｏ，ＺｎＯ，ＭｏＯ3 ，ＩｎＯ3 ，Ａｇ2 Ｏ，Ｐ
ｂＯ，ＳｒＴｉＯ3 ，ＢａＴｉＯ3 ，Ｃｏ3Ｏ4 ，Ｆｅ
2 Ｏ3 ，ＮｉＯ等がある。Usually, semiconductor materials are preferable because they are effective, easily available, and have good workability. From the viewpoint of effect and economy, Se, Ge, Si, Ti, Zn, Cu, Al,
Sn, Ga, In, P, As, Sb, C, Cd, S, T
e, Ni, Fe, Co, Ag, Mo, Sr, W, Cr,
One of Ba and Pb, or a compound, alloy, or oxide thereof is preferable, and these are used alone or in combination of two or more. For example, the element is Si,
Ge, Se, as compounds AlP, AlAg, Ga
P, AlSb, GaAs, InP, GaSb, InA
s, InSb, CdS, CdSe, ZnS, MoS 2 ,
WTe 2 , Cr 2 Te 3 , MoTe, Cu 2 S, W
S 2 , oxides such as TiO 2 , Bi 2 O 3 , CuO,
Cu 2 O, ZnO, MoO 3 , InO 3 , Ag 2 O, P
bO, SrTiO 3 , BaTiO 3 , Co 3 O 4 , Fe
2 O 3 , NiO and the like.
【００１２】これらの光触媒の使用においては、白金、
金、パラジウム、銀より選択された１種類以上の貴金属
を０．０１〜２０重量％、好ましくは０．１〜２．５重
量％加えると、効果的となるので、利用先装置規模、形
状、構造、要求性能によっては適宜予備実験を行い用い
ることができる。上記の光触媒の使用においては、電場
下で行うと効果的である。電場の強さは、１Ｖ／ｃｍ〜
１０ＫＶ／ｃｍ、通常１０Ｖ／ｃｍ〜１ｋＶ／ｃｍであ
る。電場は、光触媒の近傍に線状、網状、棒状、格子状
など、適宜の電極材を設置し、該光触媒との間に電圧を
印加することにより設定でき、光触媒や電極材の形状な
どにより、適宜予備試験を行い、適正条件を選び行うこ
とができる。光触媒や支持体の種類、形状、電場の有無
やその強さは、利用分野、処理対象物質の種類や濃度、
光源の種類、要求性能等により適宜予備試験を行い決め
ることができる。In the use of these photocatalysts, platinum,
Addition of 0.01 to 20% by weight, preferably 0.1 to 2.5% by weight, of one or more noble metals selected from gold, palladium, and silver will be effective, and therefore the scale of equipment to be used, shape, Depending on the structure and the required performance, preliminary experiments can be appropriately performed and used. It is effective to use the above-mentioned photocatalyst under an electric field. Electric field strength is 1 V / cm ~
It is 10 KV / cm, usually 10 V / cm to 1 kV / cm. The electric field can be set in the vicinity of the photocatalyst by setting an appropriate electrode material such as a linear shape, a net shape, a rod shape, or a lattice shape, and applying a voltage between the photocatalyst and the shape of the photocatalyst or electrode material. Preliminary tests can be conducted as appropriate to select appropriate conditions. The type and shape of the photocatalyst or support, the presence or absence of an electric field, and their strength are
Preliminary tests can be appropriately performed and determined depending on the type of light source, required performance, and the like.
【００１３】次に、光を照射する光源について説明す
る。光源は、光触媒を励起する波長を有するものであれ
ば、何れでも良く、低圧水銀灯、中圧水銀灯、高圧水銀
灯、キセノン灯等が使用でき、また利用先によっては、
太陽光が適宜利用できる。光源の位置は、適用分野、光
源の種類、装置形状により適宜に選択することができ
る。通常、反応器の中心部に光源を設置すると、光源か
ら放射状に放出される光が全て有効利用されるので好ま
しい。また、利用先によっては、適宜周知の有害ガス除
去手段と組合せて用いることができる。周知の有害ガス
除去手段としては、活性炭、活性炭素繊維、ゼオライ
ト、イオン交換フィルター（繊維）、有機高分子ポリマ
ー（有機高分子ビーズ）などがある。Next, the light source that emits light will be described. The light source may be any as long as it has a wavelength that excites the photocatalyst, and a low-pressure mercury lamp, a medium-pressure mercury lamp, a high-pressure mercury lamp, a xenon lamp, etc. can be used, and depending on the user,
Sunlight can be used as appropriate. The position of the light source can be appropriately selected depending on the application field, the type of light source, and the shape of the device. Usually, it is preferable to install a light source in the center of the reactor because all the light emitted radially from the light source can be effectively used. In addition, depending on the place of use, it can be used in combination with well-known harmful gas removing means as appropriate. Known means for removing harmful gases include activated carbon, activated carbon fiber, zeolite, ion exchange filters (fibers), organic polymer (organic polymer beads), and the like.
【００１４】また、本発明者らがすでに提案した複合酸
化物系触媒を用いる手段（特願平４−３３２１６７号、
特願平４−３５７７８０号、特願平５−２１６８５９
号）も、利用分野によっては適宜に用いることができ
る。これらの用い方として、通常処理有害ガスが比較的
高い場合、あるいは処理ガスの種類が多い場合、予めこ
れらの手段である程度有害ガスの除去を行い、次に本発
明の手段により除去を行う。これにより、濃度の高い被
処理気体や、多成分系の複雑な有害ガスも高効率に処理
でき、超清浄な気体や空間を効果的に得ることができ
る。Means for using the complex oxide type catalyst already proposed by the present inventors (Japanese Patent Application No. 4-332167,
Japanese Patent Application No. 4-357780, Japanese Patent Application No. 5-216859
No.) can be appropriately used depending on the field of use. As a method of using these, when the treated harmful gas is usually relatively high or the number of kinds of treated gas is large, the harmful gas is removed to some extent by these means in advance, and then removed by the means of the present invention. This makes it possible to highly efficiently treat a high-concentration gas to be treated and a complex harmful gas of a multi-component system, and effectively obtain a super-clean gas or space.
【００１５】[0015]
【実施例】以下、本発明を実施例により具体的に説明す
るが、本発明はこれらの実施例に限定されるものではな
い。 実施例１ 本発明の有害ガス除去装置の基本構成図を図１に示し、
これを用いて病院における空気清浄について説明する。
図１において、喫煙２等に起因した微粒子（粒子状物
質）及び有害ガス（臭気性ガスを含み、例えば、タール
などの炭化水素類、アルデヒド類、ケトン類、ピリジン
類、ピロール類、ニトリル類、窒素酸化物、アンモニア
等）３が発生している。空気清浄は、室の側面の中央部
に設置された前処理フィルタ４、静電フィルタ５、活性
炭６、イオン交換フィルタ７、及び本発明の光触媒を担
持させた光触媒担持体８、紫外線ランプ９、ファン１０
よりなる空気清浄器１１にて実施される。EXAMPLES The present invention will be specifically described below with reference to examples, but the present invention is not limited to these examples. Example 1 A basic configuration diagram of the harmful gas removing apparatus of the present invention is shown in FIG.
Air purification in a hospital will be described using this.
In FIG. 1, fine particles (particulate matter) and harmful gas (including odorous gas) caused by smoking 2, etc., such as hydrocarbons such as tar, aldehydes, ketones, pyridines, pyrroles, nitriles, Nitrogen oxide, ammonia, etc.) 3 is generated. The air cleaning is performed by a pretreatment filter 4, an electrostatic filter 5, an activated carbon 6, an ion exchange filter 7, and a photocatalyst carrier 8 carrying the photocatalyst of the present invention, an ultraviolet lamp 9, which is installed in the center of the side surface of the chamber. Fan 10
It is implemented in the air purifier 11.
【００１６】上記光触媒担持体８は、多数の棒状（ロッ
ド）石英ガラス表面に、８０ｎｍの厚さでＴｉＯ2 を被
覆したもので、紫外線ランプ９からの紫外線は棒状石英
ガラスの中を通して、該石英ガラス表面のＴｉＯ2 を励
起し、光触媒として活性化する。図１（ｂ）に図１
（ａ）のＡ−Ａ′断面図を示す。１２は汚染空気の流
れ、１３は空気清浄器１１により清浄化された清浄空気
を示す。この空気清浄器１１においては、喫煙等に起因
した微粒子は、前処理フィルタ４で先ず粗い粒子状物質
が除去され、次いで静電フィルタ５で残った微粒子が除
去される。一方、喫煙に起因する有害ガスは先ず活性炭
６でアルデヒド類やケトン類のような主として活性炭で
捕集し得る分子構造を有する中性物質及び酸性物質が除
去される。次に、イオン交換フィルタ（カチオン型）７
でアンモニアのような主としてアルカリ性物質が除去さ
れる。The photocatalyst carrier 8 is composed of a large number of rod-shaped quartz glass surfaces coated with TiO 2 with a thickness of 80 nm. TiO 2 on the glass surface is excited and activated as a photocatalyst. In FIG.
A sectional view taken along the line AA ′ of FIG. Reference numeral 12 represents a flow of contaminated air, and 13 represents clean air cleaned by the air cleaner 11. In the air purifier 11, coarse particles are first removed by the pretreatment filter 4 from fine particles caused by smoking, and then the remaining fine particles are removed by the electrostatic filter 5. On the other hand, the harmful gas caused by smoking is first removed by the activated carbon 6 such as neutral substances and acidic substances having a molecular structure such as aldehydes and ketones which can be captured mainly by the activated carbon. Next, an ion exchange filter (cation type) 7
At this, mainly alkaline substances such as ammonia are removed.
【００１７】イオン交換フィルタは、本発明者らがすで
に提案したものを適宜用いることができる。（例、特開
昭６３−１２３１５号、特開昭６３−７７５５７号、特
開昭６３−９７２４６号、特開平２−５９０１８号各公
報） 次に、これらのフィルタでは除去できないＮＯｘ及びリ
ークした前記の有害ガスが光触媒にて除去される。光触
媒におけるＮＯｘは、硝酸に変換され固定化されること
により除去される。光触媒担持体８の光触媒上でＮＯｘ
から変換された硝酸は、長時間運転した場合、光触媒の
性能を、劣化させ、かつ長時間運転により、後方に飛散
する場合があるので、光触媒の近傍及び／又はその後方
に生成物である硝酸の捕集フィルタ（捕集材）、例えば
イオン交換繊維（アニオン型）、活性炭、活性炭素繊
維、ガラス繊維を適宜設置すると、光触媒の効果が持続
し、かつ、万一後方へ流出した場合でも捕集できるの
で、装置の種類、処理有害ガスの濃度、用いる他の有害
成分の除去材の種類、要求性能などによっては好まし
い。リークした炭化水素や分子量の大きい中性の炭化水
素は、光触媒で効果的に除去される。As the ion exchange filter, those already proposed by the present inventors can be appropriately used. (Examples of JP-A-63-12315, JP-A-63-77557, JP-A-63-97246, and JP-A-2-59018) Next, NOx that cannot be removed by these filters and the leaked gas The harmful gas of is removed by the photocatalyst. NOx in the photocatalyst is removed by being converted into nitric acid and fixed. NOx on the photocatalyst of the photocatalyst carrier 8
The nitric acid converted from the product deteriorates the performance of the photocatalyst when it is operated for a long time, and may scatter backwards due to long-time operation. Therefore, nitric acid, which is a product near the photocatalyst and / or behind it, is a product. If a collection filter (collection material) such as ion exchange fiber (anion type), activated carbon, activated carbon fiber, or glass fiber is properly installed, the effect of the photocatalyst is maintained and even if it flows out backward Since it can be collected, it is preferable depending on the type of apparatus, the concentration of treated harmful gas, the type of other harmful component removing material used, required performance, and the like. Leaked hydrocarbons and neutral hydrocarbons with a large molecular weight are effectively removed by the photocatalyst.
【００１８】上記捕集フィルタの設置は適宜予備実験を
行い、決めることができる。光触媒は、低濃度の有害ガ
スを、極低濃度あるいは検出限界濃度以下まで、処理す
るのに好適である。そのために、本例のように周知の方
法で予め低濃度まで処理し、最終処理を光触媒で行うと
実用上効果的に処理できる。空気清浄器１１により、臭
気濃度（官能試験の値）１５０〜１，０００、非メタン
炭化水素濃度３〜１０ｐｐｍのタバコ臭を含む空気１２
は、臭気濃度１０以下、及び有害ガスとしてのＮＯｘは
５ｐｐｂ以下、ＮＨ3 は１０ｐｐｂ以下、非メタン炭化
水素濃度０．１ｐｐｍ以下となり、清浄空気１３が得ら
れる。The installation of the above-mentioned collecting filter can be determined by conducting a preliminary experiment as appropriate. The photocatalyst is suitable for treating a low concentration of harmful gas to an extremely low concentration or below the detection limit concentration. Therefore, if the treatment is carried out to a low concentration in advance by a known method as in this example and the final treatment is carried out with a photocatalyst, the treatment can be practically and effectively performed. By the air purifier 11, air 12 containing tobacco odor having an odor concentration (sensory test value) of 150 to 1,000 and a non-methane hydrocarbon concentration of 3 to 10 ppm.
Has an odor concentration of 10 or less, NOx as a harmful gas is 5 ppb or less, NH 3 is 10 ppb or less, and a non-methane hydrocarbon concentration is 0.1 ppm or less, and clean air 13 is obtained.
【００１９】実施例２ 図２に、半導体工場におけるクリーンルーム内の微量有
害ガスを除去する、本発明の除去装置を用いた空気清浄
の概略構成図を示す。図２において、クラス１，０００
（０．１μｍ以上の粒子数）のクリーンルーム３０に
は、作業３１により有害ガスとしてＮＯｘ、ＮＨ3 及び
微粒子３２が発生しており、また、クリーンルーム空気
には炭化水素（非メタン炭化水素）が１．０〜１．２０
ｐｐｍ存在する。これらの汚染物（これらのガス状汚染
物質・微粒子）は、半導体工場の原料や製品、半製品を
汚染するので、空気清浄装置１１が設置され、該有害ガ
スと微粒子の捕集・除去が行われている。Embodiment 2 FIG. 2 shows a schematic configuration diagram of air cleaning using the removing apparatus of the present invention for removing a trace amount of harmful gas in a clean room in a semiconductor factory. In FIG. 2, the class 1,000
NOx, NH 3 and fine particles 32 are generated as harmful gas by the work 31 in the clean room 30 (particle number of 0.1 μm or more), and hydrocarbon (non-methane hydrocarbon) is 1 in the clean room air. .0-1.20
ppm present. Since these pollutants (these gaseous pollutants and fine particles) pollute the raw materials, products and semi-finished products of the semiconductor factory, the air cleaning device 11 is installed to collect and remove the harmful gas and fine particles. It is being appreciated.
【００２０】該装置１１は、主に前処理フィルタ４、フ
ァン１０、イオン交換フィルタ（カチオン型）７、ＵＬ
ＰＡフィルタ５-1、５-2、光触媒担持体８及び紫外線ラ
ンプ９より構成されている。図２（ａ）のＢ−Ｂ′断面
図を図２（ｂ）に示す。有害ガスを含む被処理空気１２
はファン１０により、吸引され、処理された清浄空気は
矢印１３の方向に吐出される。それぞれの構成について
説明する。前処理フィルタ４は、空気抵抗の少ないガラ
ス繊維を主体としたフィルタであり、ここで、先ず吸引
空気１２中の粗い粒子（比較的粒径の大きい粒子）が除
去される。イオン交換フィルタ７は、作業３１により発
生したＮＨ3 などクリーンルーム中のＮＨ3 の除去用フ
ィルタであり、本発明者らがすでに提案したもの（前
記）を適宜に用いることができ、これによりＮＨ3 は１
０ｐｐｂ以下にまで除去される。The apparatus 11 mainly comprises a pretreatment filter 4, a fan 10, an ion exchange filter (cation type) 7, and a UL.
It is composed of PA filters 5-1 and 5-2 , a photocatalyst carrier 8 and an ultraviolet lamp 9. A cross-sectional view taken along the line BB ′ of FIG. 2A is shown in FIG. Air to be treated 12 containing harmful gas
The clean air that has been sucked and processed by the fan 10 is discharged in the direction of arrow 13. Each configuration will be described. The pretreatment filter 4 is a filter mainly made of glass fiber having a low air resistance, and first, coarse particles (particles having a relatively large particle size) in the suction air 12 are removed. The ion exchange filter 7 is a filter for removing NH 3 in the clean room such as NH 3 generated by the work 31, and the one already proposed by the present inventors (above) can be appropriately used, whereby the NH 3 Is 1
It is removed to 0 ppb or less.
【００２１】ＵＬＰＡフィルタ５-1は、作業３１により
発生した微粒子などクリーンルーム中の微粒子の除去フ
ィルタである。これにより、クラス１，０００のクリー
ンルーム中の微粒子、作業３１により発生した微粒子及
びファン１０の作動により発生した微粒子がクラス１０
以下まで除去される。光触媒担持体８は、主に作業３１
により発生したＮＯｘの除去及び接触角の増加をもたら
す炭化水素の分解を行うもので、多数のファイバー状石
英ガラス表面に８０ｎｍの厚さのＴｉＯ2 を被覆したも
のである。紫外線ランプ９は、ＴｉＯ2 を被覆した石英
ガラスの内部を通り石英ガラス表面に被覆したＴｉＯ2
を照射し、光触媒として作用させるものである。これに
より、クリーンルーム中のＮＯｘ及び作業３１により発
生したＮＯｘが、５ｐｐｂ以下まで除去される。また、
炭化水素は、接触角の増加に影響しない安定な形に変換
される。ＵＬＰＡフィルタ５-2は、光触媒及びその近傍
からの発生微粒子の除去フィルタであり、通常不用であ
るが、緊急時を想定して設置されている。The ULPA filter 5 -1 is a particulate removal filter in a clean room, such as particles generated by the work 31. As a result, the fine particles in the class 1,000 clean room, the fine particles generated by the operation 31 and the fine particles generated by the operation of the fan 10 are classified into the class 10
The following are removed. The photocatalyst carrier 8 is mainly used for work 31.
The removal of NOx generated by the above and the decomposition of hydrocarbons that increase the contact angle are performed, and a large number of fibrous quartz glass surfaces are coated with TiO 2 having a thickness of 80 nm. The ultraviolet lamp 9 is composed of TiO 2 coated on the surface of the quartz glass through the inside of the quartz glass coated with TiO 2.
Is irradiated to act as a photocatalyst. As a result, NOx in the clean room and NOx generated by the work 31 are removed to 5 ppb or less. Also,
Hydrocarbons are converted to a stable form that does not affect the increase in contact angle. ULPA filters 5-2 is a filter for removing generated particles from the photocatalyst and its vicinity, is usually unnecessary, and is placed on the assumption emergency.
【００２２】これらにより、ＮＯｘ濃度は５ｐｐｂ以
下、非メタン炭化水素は０．２ｐｐｍ以下、ＮＨ3 濃度
は１０ｐｐｎ以下、微粒子濃度クラス１０以下の接触角
を増加させない清浄空気１３が得られる。クリーンルー
ム内で有害ガスが発生すると、製品や半製品に付着し、
接触角の増加をもたらし歩留まりの低下をひき起こす
（生産性が下がる。）。従って、該有害ガスを一定濃度
以下にすることはクリーンルームの管理上重要である。
なお、実施例における光触媒、周知の有害ガス除去手段
の組合せ順序は、何ら限定されるものではなく予備試験
を行い適宜に決めることができる。なお、接触角とは、
固体表面の汚染の程度を示す指標であり、固体表面が汚
染されると、水の接触角がその汚染状態をよく反映し、
汚染の程度が大きいと接触角が大きく、逆に汚染の程度
が小さいと接触角が小さい。As a result, clean air 13 having a NOx concentration of 5 ppb or less, a non-methane hydrocarbon of 0.2 ppm or less, an NH 3 concentration of 10 ppn or less, and a particle concentration class of 10 or less, which does not increase the contact angle, can be obtained. When harmful gas is generated in the clean room, it adheres to products and semi-finished products,
It causes an increase in contact angle and causes a decrease in yield (productivity decreases). Therefore, it is important for clean room management to keep the harmful gas below a certain concentration.
The order of combining the photocatalyst and the known harmful gas removing means in the examples is not limited at all and can be appropriately determined by performing a preliminary test. The contact angle is
It is an index showing the degree of contamination of the solid surface, and when the solid surface is contaminated, the contact angle of water well reflects the contamination state,
When the degree of contamination is large, the contact angle is large, and conversely, when the degree of contamination is small, the contact angle is small.
【００２３】実施例３ 図３にクラス１，０００の半導体工場のクリーンルーム
に設置されたウェハの接触角増加防止を図るストッカ３
３の概略構成図を示す。クリーンルーム空気には、炭化
水素（非メタン炭化水素）が１．１〜１．３ｐｐｍ存在
する。この炭化水素の起因は外気から導入されたもの、
並びにクリーンルーム構成材からの脱ガスである。ちな
みに、クリーンルームの外（外気）の炭化水素濃度は
０．９〜１．０ｐｐｍであり、クリーンルームの中より
低い。これは、クリーンルーム内ではクリーンルーム構
成材などから炭化水素の発生があるためである（ウルト
ラクリーンテクノロジー、７巻、４号、ｐ．１５〜２
０、１９９５）。Example 3 FIG. 3 shows a stocker 3 installed in a clean room of a class 1,000 semiconductor factory for preventing an increase in contact angle of wafers.
The schematic block diagram of 3 is shown. The clean room air contains 1.1 to 1.3 ppm of hydrocarbons (non-methane hydrocarbons). The cause of this hydrocarbon is that introduced from the outside air,
Also, it is degassing from clean room components. Incidentally, the hydrocarbon concentration outside the clean room (outside air) is 0.9 to 1.0 ppm, which is lower than in the clean room. This is because hydrocarbons are generated from the clean room components in the clean room (Ultra Clean Technology, Vol. 7, No. 4, p. 15-2).
0, 1995).
【００２４】これらの炭化水素は、ウェハ基板表面に付
着し、歩留まりの低下をもたらす。この炭化水素による
汚染の程度は、接触角によって表わすことができる（空
気清浄、３３巻、１号、ｐ．１６−２１、１９９５）。
ストッカ３３は、上記ウェハなど基板の汚染防止（接触
角増加防止）を図る装置で、ガラス板上に８０ｎｍＴｉ
Ｏ2 光触媒を担持させた光触媒担持体８、紫外線ランプ
９、紫外線ランプからの紫外線を効率よく光触媒担持体
８に照射するため反射面１５、ウェハなど製品や半製品
への直接の紫外線照射を避けるためのしゃ光材１４より
構成される。１６は、ストッカ内の気流の方向であり、
紫外線ランプ９の照射により生ずる光触媒担持体８上下
のわずかな温度差により生ずる。Ａは、ストッカ３３の
ウェハの収納部である。These hydrocarbons adhere to the surface of the wafer substrate and cause a reduction in yield. The degree of contamination by this hydrocarbon can be expressed by the contact angle (Air cleaning, Vol. 33, No. 1, p. 16-21, 1995).
The stocker 33 is a device for preventing contamination of the substrate such as the wafer (prevention of increase in contact angle), and 80 nm Ti on a glass plate.
The photocatalyst carrier 8 carrying the O 2 photocatalyst, the ultraviolet lamp 9, and in order to efficiently irradiate the photocatalyst carrier 8 with the ultraviolet rays from the ultraviolet lamp, avoid the direct irradiation of the reflecting surface 15, the wafer and other products or semi-finished products with the ultraviolet rays. The light shielding material 14 for 16 is the direction of the air flow in the stocker,
It is caused by a slight temperature difference between the upper and lower sides of the photocatalyst carrier 8 caused by the irradiation of the ultraviolet lamp 9. A is a wafer storage unit of the stocker 33.
【００２５】実施例４ ホテルのロビーの照明との組合せで、ＮＯｘ除去を行う
概略図を図４に示す。本例はアメニティとしての利用の
例である。図４において、ホテルのロビー４０には、２
つの照明器具１１があり、近傍を明るくしている。照明
器具１１の主たる構成は、内側の光源９、外側のガラス
より成り、該ガラスの表面に８０ｎｍ厚さのＴｉＯ2 が
被覆された光触媒担持体８となっている。光触媒担持体
の近傍のＮＯｘ、ＳＯｘは、光源９により活性化された
光触媒表面で除去される。１７は、電源コードである。Example 4 FIG. 4 shows a schematic diagram of NOx removal in combination with lighting in a hotel lobby. This example is an example of use as an amenity. As shown in FIG.
There are two lighting fixtures 11 to brighten the vicinity. The main structure of the luminaire 11 is a photocatalyst carrier 8 which comprises an inner light source 9 and an outer glass, and the surface of the glass is coated with TiO 2 having a thickness of 80 nm. NOx and SOx in the vicinity of the photocatalyst carrier are removed on the photocatalyst surface activated by the light source 9. Reference numeral 17 is a power cord.
【００２６】実施例５ 高速道路の壁面に光触媒を組込み有害ガスを除去する概
略図を図５に示す。図５において、高速道路５０では、
高速で走行する車１８からＮＯｘが排出されている。該
道路５０には壁面１９があり、壁面の一部はガラスで成
り、該ガラス表面は８０ｎｍ厚さのＴｉＯ2 が被覆され
た光触媒担持体８となっている。該光触媒担持体８に
は、その裏面及び／又は表面から太陽光２０が照射さ
れ、ＮＯｘが除去される。ＮＯｘは、光触媒により硝酸
に変換し、光触媒表面に付着するが、時々の降雨により
該硝酸は光触媒上より洗い流され、ピット２１より回収
され、別途水処理装置により、周知の方法でＮ2 にまで
還元される。２２は、高速道路を支える架台である。太
陽光による光触媒への照射２０の位置には、時間経過に
より変化するが、本触媒は表面照射、裏面照射いずれで
も効果があるので、太陽光が有効利用できる。Example 5 FIG. 5 shows a schematic diagram of removing a harmful gas by incorporating a photocatalyst on the wall surface of an expressway. In FIG. 5, on the highway 50,
NOx is emitted from the vehicle 18 traveling at high speed. The road 50 has a wall surface 19, a part of the wall surface is made of glass, and the glass surface is a photocatalyst carrier 8 coated with TiO 2 having a thickness of 80 nm. The photocatalyst carrier 8 is irradiated with sunlight 20 from its back surface and / or front surface to remove NOx. NOx is converted into nitric acid by the photocatalyst and adheres to the photocatalyst surface, but due to occasional rainfall, the nitric acid is washed off from the photocatalyst and collected from the pit 21, and is separated into N 2 by a well-known method by a separate water treatment device. Be reduced. Reference numeral 22 is a pedestal that supports an expressway. The position of irradiation 20 of the photocatalyst by sunlight changes with the passage of time, but since the present catalyst is effective for both front irradiation and back irradiation, sunlight can be effectively used.
【００２７】実施例６ 上記実施例における光触媒の膜厚について検討し、実施
例３の図３のストッカに下記光触媒を設置し、光触媒の
効果について試験・評価した。 （１）光触媒の膜厚の検討 ８５．６ｇ（０．３モル）のチタンテトライソプロポキ
シド（Ｔｉ（ＯｉＰｒ）4 ）に攪拌しながら６０．３ｇ
（０．６モル）のアセチルアセトン（ＡｃＡｃ）をビュ
レットを用いて徐々に滴下し、約１時間攪拌することに
より安定なＴｉ（ＡｃＡｃ）2 （ＯｉＰｒ）2 錯体溶液
を得た。この溶液３０ｍｌを分取し、無水エタノールで
１００ｍｌに希釈することにより、コーティング液を得
た。ディッピング法を用いて、片面をテープでマスキン
グした石英基板（２０ｍｍ幅×５０ｍｍ長×１ｍｍ厚）
上に薄膜を形成させた（基板引き上げ速度＝４．６ｃｍ
／ｍｉｎ）。約３０分放置した後に、５００℃で１０分
間焼成した。以上のプロセスを繰り返す（繰り返し回数
＝ｎ）ことにより膜厚の異なる７種類のサンプルを得
た。Example 6 The film thickness of the photocatalyst in the above example was examined, the following photocatalyst was installed in the stocker of FIG. 3 of Example 3, and the effect of the photocatalyst was tested and evaluated. (1) Examination of film thickness of photocatalyst 60.3 g of titanium tetraisopropoxide (Ti (OiPr) 4 ) of 85.6 g (0.3 mol) while stirring
(0.6 mol) of acetylacetone (AcAc) was gradually added dropwise using a buret and stirred for about 1 hour to obtain a stable Ti (AcAc) 2 (OiPr) 2 complex solution. 30 ml of this solution was collected and diluted with absolute ethanol to 100 ml to obtain a coating liquid. Quartz substrate (20mm width x 50mm length x 1mm thickness) with one side masked with tape using dipping method
A thin film was formed on the substrate (substrate pulling rate = 4.6 cm)
/ Min). After leaving it for about 30 minutes, it was baked at 500 ° C. for 10 minutes. By repeating the above process (the number of repetitions = n), seven types of samples having different film thicknesses were obtained.
【００２８】走査型電子顕微鏡による膜厚分析の結果
（測定精度＝約１０％）、２０ｎｍ（ｎ＝２）、５０ｎ
ｍ（ｎ＝２）、８０ｎｍ（ｎ＝２）、１００ｎｍ（ｎ＝
３）、１４０ｎｍ（ｎ＝２）、１５８ｎｍ（ｎ＝３）、
２２０ｎｍ（ｎ＝４）なる値が得られた。Ｘ−線回折の
結果、アナタース形のＴｉＯ2 結晶性薄膜が基板上に形
成されていることが確認された。７種類のサンプルをア
ルカリ洗浄した後に、真空デシケータ中にセットし、真
空ポンプで約１０Ｔｏｒｒに減圧してから内部温度を８
０℃に保持した。系を閉じてから、２００μＬの１，
３，５，７−テトラメチルシクロテトラシロキサン（Ｔ
ＭＣＴＳ）を注射器で注入後、３０分間加熱した。さら
に、真空ポンプで減圧しながら、１００℃に昇温し３０
分間加熱することにより未反応のＴＭＣＴＳをコールド
トラップした。これにより、ＴｉＯ2表面にＴＭＣＴＳ
単分子膜を形成させた。この時点で、表面は親水性から
撥水性に変化した。Results of film thickness analysis by a scanning electron microscope (measurement accuracy = about 10%), 20 nm (n = 2), 50 n
m (n = 2), 80 nm (n = 2), 100 nm (n =
3), 140 nm (n = 2), 158 nm (n = 3),
A value of 220 nm (n = 4) was obtained. As a result of X-ray diffraction, it was confirmed that an anatase type TiO 2 crystalline thin film was formed on the substrate. After cleaning 7 kinds of samples with alkali, set them in a vacuum desiccator, reduce the pressure to about 10 Torr with a vacuum pump, and then set the internal temperature to 8
Hold at 0 ° C. After closing the system, 200 μL of 1,
3,5,7-Tetramethylcyclotetrasiloxane (T
MCTS) was injected with a syringe and heated for 30 minutes. Furthermore, while reducing the pressure with a vacuum pump, the temperature is raised to 100 ° C.
Unreacted TMCTS was cold trapped by heating for a minute. As a result, TMCTS is formed on the TiO 2 surface.
A monolayer was formed. At this point, the surface changed from hydrophilic to water repellent.
【００２９】高圧水銀灯を用いてＴｉＯ2 膜の裏面から
光照射することにより、ＴＭＣＴＳ単分子膜のメチル基
が酸化分解され、表面の親水性が徐々に増加した。ＴＭ
ＣＴＳ単分子膜の酸化分解速度によりＴｉＯ2 膜の光触
媒活性を評価した。膜厚と分解速度定数の関係を図６に
示す。これにより、膜厚の増加と共に光触媒活性は高く
なり、５０ｎｍから１００ｎｍで最大に達した後に、再
び低下することがわかる。すなわち、膜厚が２０ｎｍ〜
２００ｎｍ、特に好ましくは５０〜１００ｎｍの範囲
で、表面の光触媒に顕著に光吸収量が増大するために活
性が高くなる。これに対して、２００ｎｍ以上の範囲で
は、膜中で発生したフォトキャリヤーが表面まで到達す
る確率が減少するために、逆に活性は低下するものと考
えられる。By irradiating the back surface of the TiO 2 film with a high pressure mercury lamp, the methyl groups of the TMCTS monomolecular film were oxidized and decomposed, and the hydrophilicity of the surface was gradually increased. TM
The photocatalytic activity of the TiO 2 film was evaluated by the oxidative decomposition rate of the CTS monolayer. The relationship between the film thickness and the decomposition rate constant is shown in FIG. This shows that the photocatalytic activity increases as the film thickness increases, reaches the maximum from 50 nm to 100 nm, and then decreases again. That is, the film thickness is 20 nm to
In the range of 200 nm, particularly preferably in the range of 50 to 100 nm, the activity becomes high because the photocatalyst on the surface remarkably increases the light absorption amount. On the other hand, in the range of 200 nm or more, the photocarriers generated in the film are less likely to reach the surface, and thus the activity is considered to be decreased.
【００３０】（２）ストッカによる評価・試験 ストッカ内にウェハを設置し、接触角の増加防止につい
て調べた。 ストッカの大きさ ； ５０リットル 光触媒担持体 ； 石英ガラス上にＴｉＯ2 を担持。 膜厚：２０ｎｍ、５０ｎｍ、８０ｎｍ、１００ｎｍ、 １４０ｎｍ、２２０ｎｍ 光源 ； 低圧水銀灯、１０Ｗ 接触角の測定 ； 水滴式接触角計 結果 図７に、各種膜厚の光触媒担持体及び、比較として光触
媒を担持しないもの（−●−）の接触角を示す。時間
は、ストッカにおけるウェハの経過時間である。２０ｎ
ｍ：△、５０ｎｍ：〇、８０ｎｍ：◎、１００ｎｍ：
▲、１４０ｎｍ：□、２２０ｎｍ：■を示す。(2) Evaluation / Test by Stocker A wafer was placed in the stocker to investigate prevention of increase in contact angle. Stocker size: 50 liters Photocatalyst carrier: TiO 2 is supported on quartz glass. Film thickness: 20 nm, 50 nm, 80 nm, 100 nm, 140 nm, 220 nm Light source; Low-pressure mercury lamp, 10 W contact angle measurement; Water-drop type contact angle meter result FIG. The contact angle of the product (-●-) is shown. Time is the elapsed time of the wafer in the stocker. 20n
m: Δ, 50 nm: ○, 80 nm: ◎, 100 nm:
▲, 140 nm: □, 220 nm: □.
【００３１】[0031]
【発明の効果】本発明によれば、次のような効果を奏す
ることができる。 １）光透過性支持体の表面に光触媒を担持し、該裏面よ
り光照射を行う。光触媒担持体において、光触媒の被覆
の厚さを２０〜２００ｎｍとすることにより、 膜の裏面から光照射する場合には、膜厚が薄いと光
を十分に吸収できないので、また膜厚が厚すぎると、表
面までフォトキャリヤーが到達しないので光触媒の作用
は不十分（活性が低い）だが、２０〜２００ｎｍでは適
正膜厚となり、光触媒の光吸収が効果的になるために、
光触媒の活性が高くなった。 特に、膜厚が５０〜１００ｎｍの範囲で、顕著な作
用が得られた。According to the present invention, the following effects can be obtained. 1) A photocatalyst is carried on the surface of the light transmissive support, and light is irradiated from the back surface. In the photocatalyst carrier, by setting the thickness of the photocatalyst coating to 20 to 200 nm, when the light is irradiated from the back surface of the film, the light cannot be sufficiently absorbed if the film is thin, and thus the film is too thick. Then, since the photocarrier does not reach the surface, the action of the photocatalyst is insufficient (low activity), but at 20 to 200 nm, an appropriate film thickness is obtained and the photocatalyst absorbs light effectively.
The photocatalyst activity became higher. In particular, a remarkable effect was obtained in the film thickness range of 50 to 100 nm.
【００３２】２）支持体がガラス材であるので、光触媒
への紫外光及び／又は可視光の光照射を処理物を介さず
に、光触媒の裏面より直接できるので、処理装置の構造
を利用分野によってより効果的に自由度大に選択するこ
とができる。例えば、利用分野によって、光触媒を外
部、光源を内部、あるいは、光触媒を内部、光源を外
部、また両方を同時に組合せて実施することもできる。
また、これにより太陽光も適宜に利用できる。すなわ
ち、従来の表面のみからの照射だと、時間経過により光
触媒表面に固体状物質などが付着した場合、その部分は
全くデッドスペースとなり性能劣化した。また、従来法
は処理物を介して照射されるので、処理物により性能が
影響を受け、また処理物によっては処理物が光を吸収し
てしまい光が有効に利用できなかった。本発明では、前
記したように、性能が処理物によらず、長時間安定に維
持できた。2) Since the support is a glass material, it is possible to directly irradiate the photocatalyst with ultraviolet light and / or visible light from the back surface of the photocatalyst without passing through the object to be treated. Can be selected more effectively and with a large degree of freedom. For example, depending on the field of use, the photocatalyst can be external, the light source can be internal, or the photocatalyst can be internal, the light source can be external, or both can be implemented simultaneously.
In addition, sunlight can also be used accordingly. That is, when irradiation is performed only from the conventional surface, when a solid substance or the like adheres to the photocatalyst surface over time, that portion becomes a dead space and the performance deteriorates. Further, in the conventional method, since the irradiation is performed through the treated product, the performance is affected by the treated product, and depending on the treated product, the treated product absorbs light, so that the light cannot be effectively used. In the present invention, as described above, the performance can be stably maintained for a long time regardless of the processed material.
【図１】（ａ）は病院における空気清浄に用いた本発明
の有害ガス除去装置の基本構成図で、（ｂ）は（ａ）の
Ａ−Ａ′断面図。1A is a basic configuration diagram of a harmful gas removing apparatus of the present invention used for air cleaning in a hospital, and FIG. 1B is a sectional view taken along the line AA ′ of FIG.
【図２】（ａ）は半導体工場のクリーンルームに用いた
本発明の除去装置の概略構成図で、（ｂ）は（ａ）のＢ
−Ｂ′断面図。FIG. 2 (a) is a schematic configuration diagram of a removing apparatus of the present invention used in a clean room of a semiconductor factory, and FIG. 2 (b) is B of (a).
-B 'sectional view.
【図３】半導体工場のクリーンルームに設置されたスト
ッカの概略構成図。FIG. 3 is a schematic configuration diagram of a stocker installed in a clean room of a semiconductor factory.
【図４】ホテルのロビーの照明に本発明を適用した概略
図。FIG. 4 is a schematic diagram in which the present invention is applied to lighting in a hotel lobby.
【図５】高速道路の壁面に本発明を適用した概略図。FIG. 5 is a schematic view in which the present invention is applied to a wall surface of an expressway.
【図６】膜厚と分解速度定数の関係を示すグラフ。FIG. 6 is a graph showing the relationship between film thickness and decomposition rate constant.
【図７】各種膜厚の接触角と時間の関係を示すグラフ。FIG. 7 is a graph showing the relationship between the contact angle of various film thicknesses and time.
１：病院の待合室、２：タバコ、３：有害ガス、４：前
処理フィルタ、５：静電フィルタ、５-1、５-2：ＵＬＰ
Ａフィルタ、６：活性炭、７：イオン交換フィルタ、
８：光触媒担持体、９：紫外線ランプ、１０：ファン、
１１：空気清浄器、１２：汚染空気、１３：清浄空気、
１４：遮光材、１５：反射面、１６：気流の流れ、１
７：電源コード、１８：自動車、１９：道路壁面、２
０：太陽光、２１：ピット、２２：架台、３０：クリー
ンルーム、３１：作業、３２：微粒子、３３：ストッカ1: Hospital waiting room, 2: Cigarette, 3: Harmful gas, 4: Pretreatment filter, 5: Electrostatic filter, 5 -1 , 5 -2 : ULP
A filter, 6: activated carbon, 7: ion exchange filter,
8: photocatalyst carrier, 9: ultraviolet lamp, 10: fan,
11: Air purifier, 12: Contaminated air, 13: Clean air,
14: light-shielding material, 15: reflective surface, 16: air flow, 1
7: power cord, 18: automobile, 19: road wall surface, 2
0: Sunlight, 21: Pit, 22: Stand, 30: Clean room, 31: Work, 32: Fine particles, 33: Stocker
Claims (3)
て、該気体を、表面に２０〜２００ｎｍの厚さの光触媒
を担持させた光透過性支持体の表面に、裏面から光を照
射させながら接触させることを特徴とする有害ガスの除
去方法。1. A method for removing harmful gas in a gas, which comprises irradiating the surface of a light-transmissive support having a photocatalyst having a thickness of 20 to 200 nm on its surface with light from the back surface. A method for removing harmful gases, which is characterized by bringing them into contact with each other.
て、表面に２０〜２００ｎｍの厚さの光触媒を担持させ
た光透過性支持体と、該支持体の裏面から光を照射する
光源とを有することを特徴とする有害ガスの除去装置。2. An apparatus for removing harmful gas in a gas, comprising: a light-transmissive support having a photocatalyst having a thickness of 20 to 200 nm carried on the surface thereof, and a light source for irradiating light from the back surface of the support. A device for removing harmful gas, which is characterized by having.
は、厚さが５０〜１００ｎｍであることを特徴とする請
求項２記載の有害ガスの除去装置。3. The harmful gas removing apparatus according to claim 2, wherein the photocatalyst supported on the light transmissive support has a thickness of 50 to 100 nm.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04688796A JP3476302B2 (en) | 1996-02-09 | 1996-02-09 | Method and apparatus for removing harmful gas |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04688796A JP3476302B2 (en) | 1996-02-09 | 1996-02-09 | Method and apparatus for removing harmful gas |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH09215910A true JPH09215910A (en) | 1997-08-19 |
| JP3476302B2 JP3476302B2 (en) | 2003-12-10 |
Family
ID=12759884
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP04688796A Expired - Fee Related JP3476302B2 (en) | 1996-02-09 | 1996-02-09 | Method and apparatus for removing harmful gas |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3476302B2 (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH1190236A (en) * | 1997-09-22 | 1999-04-06 | Ebara Corp | Photocatalyst and reaction device using photocatalyst |
| JP2006158994A (en) * | 2004-12-02 | 2006-06-22 | Keio Gijuku | Air cleaner |
| JP2010063979A (en) * | 2008-09-09 | 2010-03-25 | Totoku Electric Co Ltd | Method for manufacturing photocatalyst fiber |
-
1996
- 1996-02-09 JP JP04688796A patent/JP3476302B2/en not_active Expired - Fee Related
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH1190236A (en) * | 1997-09-22 | 1999-04-06 | Ebara Corp | Photocatalyst and reaction device using photocatalyst |
| JP2006158994A (en) * | 2004-12-02 | 2006-06-22 | Keio Gijuku | Air cleaner |
| JP2010063979A (en) * | 2008-09-09 | 2010-03-25 | Totoku Electric Co Ltd | Method for manufacturing photocatalyst fiber |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3476302B2 (en) | 2003-12-10 |
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