JP7429020B2 - Method for decomposing organic matter using photocatalyst and composition used for the same - Google Patents
Method for decomposing organic matter using photocatalyst and composition used for the same Download PDFInfo
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- JP7429020B2 JP7429020B2 JP2019096647A JP2019096647A JP7429020B2 JP 7429020 B2 JP7429020 B2 JP 7429020B2 JP 2019096647 A JP2019096647 A JP 2019096647A JP 2019096647 A JP2019096647 A JP 2019096647A JP 7429020 B2 JP7429020 B2 JP 7429020B2
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- 239000011941 photocatalyst Substances 0.000 title claims description 116
- 238000000034 method Methods 0.000 title claims description 37
- 239000005416 organic matter Substances 0.000 title claims description 19
- 239000000203 mixture Substances 0.000 title description 27
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 236
- 239000013566 allergen Substances 0.000 claims description 55
- 239000000126 substance Substances 0.000 claims description 45
- 230000001699 photocatalysis Effects 0.000 claims description 26
- 238000000354 decomposition reaction Methods 0.000 claims description 20
- 239000000428 dust Substances 0.000 claims description 13
- 244000052769 pathogen Species 0.000 claims description 7
- 241000700605 Viruses Species 0.000 claims description 5
- 244000005700 microbiome Species 0.000 claims description 5
- 229920006317 cationic polymer Polymers 0.000 claims 2
- 238000012986 modification Methods 0.000 claims 2
- 230000004048 modification Effects 0.000 claims 2
- 230000001717 pathogenic effect Effects 0.000 claims 2
- 239000000243 solution Substances 0.000 description 26
- 239000008351 acetate buffer Substances 0.000 description 19
- 241000218645 Cedrus Species 0.000 description 15
- 229960004784 allergens Drugs 0.000 description 14
- 239000013573 pollen allergen Substances 0.000 description 12
- 230000009467 reduction Effects 0.000 description 12
- 239000002953 phosphate buffered saline Substances 0.000 description 11
- 108010055622 Dermatophagoides farinae antigen f 1 Proteins 0.000 description 9
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 9
- LOKCTEFSRHRXRJ-UHFFFAOYSA-I dipotassium trisodium dihydrogen phosphate hydrogen phosphate dichloride Chemical compound P(=O)(O)(O)[O-].[K+].P(=O)(O)([O-])[O-].[Na+].[Na+].[Cl-].[K+].[Cl-].[Na+] LOKCTEFSRHRXRJ-UHFFFAOYSA-I 0.000 description 8
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 8
- 239000007864 aqueous solution Substances 0.000 description 7
- 238000006243 chemical reaction Methods 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- SCVFZCLFOSHCOH-UHFFFAOYSA-M potassium acetate Chemical compound [K+].CC([O-])=O SCVFZCLFOSHCOH-UHFFFAOYSA-M 0.000 description 6
- 206010020751 Hypersensitivity Diseases 0.000 description 5
- 239000000872 buffer Substances 0.000 description 5
- 241000238876 Acari Species 0.000 description 4
- 241001091433 Itea Species 0.000 description 4
- 230000003213 activating effect Effects 0.000 description 4
- -1 biomolecules Substances 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 4
- 230000001419 dependent effect Effects 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- 241000894006 Bacteria Species 0.000 description 3
- 241000233866 Fungi Species 0.000 description 3
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 230000004913 activation Effects 0.000 description 3
- 229910052783 alkali metal Inorganic materials 0.000 description 3
- 230000003139 buffering effect Effects 0.000 description 3
- 230000015556 catabolic process Effects 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 229940079593 drug Drugs 0.000 description 3
- 239000003814 drug Substances 0.000 description 3
- 230000006872 improvement Effects 0.000 description 3
- 230000001678 irradiating effect Effects 0.000 description 3
- 235000011056 potassium acetate Nutrition 0.000 description 3
- 239000001632 sodium acetate Substances 0.000 description 3
- 235000017281 sodium acetate Nutrition 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 239000004094 surface-active agent Substances 0.000 description 3
- 239000012085 test solution Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 238000002965 ELISA Methods 0.000 description 2
- 238000008157 ELISA kit Methods 0.000 description 2
- 229920001213 Polysorbate 20 Polymers 0.000 description 2
- 229940074608 allergen extract Drugs 0.000 description 2
- 239000000427 antigen Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 238000005119 centrifugation Methods 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000004744 fabric Substances 0.000 description 2
- 239000000835 fiber Substances 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 239000003973 paint Substances 0.000 description 2
- 239000000256 polyoxyethylene sorbitan monolaurate Substances 0.000 description 2
- 235000010486 polyoxyethylene sorbitan monolaurate Nutrition 0.000 description 2
- 239000003755 preservative agent Substances 0.000 description 2
- 230000002335 preservative effect Effects 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 239000006228 supernatant Substances 0.000 description 2
- 230000036962 time dependent Effects 0.000 description 2
- SRPWOOOHEPICQU-UHFFFAOYSA-N trimellitic anhydride Chemical compound OC(=O)C1=CC=C2C(=O)OC(=O)C2=C1 SRPWOOOHEPICQU-UHFFFAOYSA-N 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910005540 GaP Inorganic materials 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 241001465754 Metazoa Species 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229930182555 Penicillin Natural products 0.000 description 1
- JGSARLDLIJGVTE-MBNYWOFBSA-N Penicillin G Chemical compound N([C@H]1[C@H]2SC([C@@H](N2C1=O)C(O)=O)(C)C)C(=O)CC1=CC=CC=C1 JGSARLDLIJGVTE-MBNYWOFBSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 235000010724 Wisteria floribunda Nutrition 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- 150000001242 acetic acid derivatives Chemical class 0.000 description 1
- 208000026935 allergic disease Diseases 0.000 description 1
- 230000007815 allergy Effects 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- 208000006673 asthma Diseases 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- UQLDLKMNUJERMK-UHFFFAOYSA-L di(octadecanoyloxy)lead Chemical compound [Pb+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O UQLDLKMNUJERMK-UHFFFAOYSA-L 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- HZXMRANICFIONG-UHFFFAOYSA-N gallium phosphide Chemical compound [Ga]#P HZXMRANICFIONG-UHFFFAOYSA-N 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000003301 hydrolyzing effect Effects 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 210000000987 immune system Anatomy 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 208000030603 inherited susceptibility to asthma Diseases 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 150000002736 metal compounds Chemical class 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 239000002736 nonionic surfactant Substances 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 150000007524 organic acids Chemical class 0.000 description 1
- 235000005985 organic acids Nutrition 0.000 description 1
- 229940049954 penicillin Drugs 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 108090000623 proteins and genes Proteins 0.000 description 1
- 102000004169 proteins and genes Human genes 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 239000007974 sodium acetate buffer Substances 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten 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
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
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Description
本発明は、酢酸と光触媒とを接触させる方法、光触媒を用いて有機物を分解する方法、およびそのために用いる組成物に関する。 The present invention relates to a method of bringing acetic acid into contact with a photocatalyst, a method of decomposing organic matter using a photocatalyst, and a composition used for the same.
光触媒は光を当てることによって有機物（例えば、有害物質の分解や殺菌）および水の加水分解による水素製造などに利用できることからその実用化のための開発が活発に進められている（特許文献１）。光触媒の触媒活性を向上させることによって、光触媒の利用や、光触媒の改良を効率的に進めることができると期待される。 Photocatalysts can be used to produce hydrogen by hydrolyzing organic substances (e.g., decomposition and sterilization of harmful substances) and water by irradiating them with light, so development for their practical use is actively underway (Patent Document 1). . By improving the catalytic activity of photocatalysts, it is expected that the use of photocatalysts and the improvement of photocatalysts can be promoted efficiently.
本発明は、酢酸と光触媒とを接触させる方法、光触媒を用いて有機物を分解する方法、およびそのために用いる組成物を提供する。 The present invention provides a method of bringing acetic acid into contact with a photocatalyst, a method of decomposing organic matter using a photocatalyst, and a composition used for the same.
本発明者は、酢酸存在下では、光触媒の触媒活性が向上すること、および有機物（例えば、病原体やアレルゲン）の光触媒による分解が促進されることを見出した。本発明はこれらの知見に基づくものである。 The present inventors have found that in the presence of acetic acid, the catalytic activity of the photocatalyst is improved and the decomposition of organic substances (eg, pathogens and allergens) by the photocatalyst is promoted. The present invention is based on these findings.
本発明によれば、例えば、以下の産業上利用可能な発明が提供される。
（１）酢酸と光触媒の組合せ。
（２）有機物を更に含む、上記（１）に記載の組合せ。
（３）光触媒によって有機物を分解することに用いるための、上記（１）または（２）に記載の組合せ。
（４）酢酸存在下で、有機物を分解することに用いるための、光触媒を含む組成物。
（５）有機物を分解する方法であって、
酢酸存在下で、光触媒を用いて有機物を分解することを含む、方法。
（６）上記（５）に記載の方法であって、分解中または分解後に有機物を検出することをさらに含む、方法。
（７）光触媒の光触媒活性を増加させる方法であって、
酢酸と光触媒とを接触させることを含む、方法。
（８）光触媒の光触媒活性の評価方法であって、
酢酸存在下で、光触媒の光触媒活性を評価することを含む、方法。
（９）光触媒によるアレルゲンの低減方法であって、
酢酸存在下で、アレルゲンと接触した光触媒の光触媒活性を光照射によって活性化することを含む、方法。
（１０）酢酸と光触媒とを接触させることを含む、方法。
According to the present invention, for example, the following industrially applicable inventions are provided.
(1) Combination of acetic acid and photocatalyst.
(2) The combination according to (1) above, further containing an organic substance.
(3) The combination described in (1) or (2) above for use in decomposing organic substances with a photocatalyst.
(4) A composition containing a photocatalyst for use in decomposing organic substances in the presence of acetic acid.
(5) A method of decomposing organic matter,
A method comprising decomposing organic matter using a photocatalyst in the presence of acetic acid.
(6) The method according to (5) above, further comprising detecting the organic substance during or after decomposition.
(7) A method for increasing the photocatalytic activity of a photocatalyst, comprising:
A method comprising contacting acetic acid with a photocatalyst.
(8) A method for evaluating photocatalytic activity of a photocatalyst, comprising:
A method comprising evaluating photocatalytic activity of a photocatalyst in the presence of acetic acid.
(9) A method for reducing allergens using a photocatalyst, the method comprising:
A method comprising activating the photocatalytic activity of a photocatalyst in contact with an allergen by light irradiation in the presence of acetic acid.
(10) A method comprising contacting acetic acid with a photocatalyst.
本明細書では、光触媒は、特定の光（例えば、紫外線、可視光および赤外線など）を照射すると活性化する性質（このような性質を光触媒活性という）を有する。光触媒としては、酸化チタン、タングステン、インジウム、銀、モリブデン、亜鉛、ガリウムリン、ガリウム、およびヒ素などの金属化合物が挙げられる。酸化チタンは、光照射により活性酸素を発生させる。この活性酸素は、有機物（微生物含む）の分解に有用である。 In this specification, a photocatalyst has a property of being activated when irradiated with specific light (for example, ultraviolet light, visible light, infrared light, etc.) (such property is referred to as photocatalytic activity). Photocatalysts include metal compounds such as titanium oxide, tungsten, indium, silver, molybdenum, zinc, gallium phosphide, gallium, and arsenic. Titanium oxide generates active oxygen when irradiated with light. This active oxygen is useful for decomposing organic matter (including microorganisms).
本明細書では、可視光は、人間の目で視認可能な波長を有する光である。可視光の下限波長は、３６０ｎｍ～４００ｎｍであり、上限波長は、７６０～８３０ｎｍである。紫外線は、下限より短い波長を有し、赤外線は上限よりも長い波長を有する。４２０ｎｍ～７００ｎｍの可視光は視認性が高い可視光である。可視光は、太陽光；ＬＥＤライト、蛍光灯、および白熱灯などの照明により発される光；キセノンランプ、ハロゲンランプ、およびナトリウムランプなどの光源により発される光などが挙げられる。 As used herein, visible light is light having a wavelength that is visible to the human eye. The lower limit wavelength of visible light is 360 nm to 400 nm, and the upper limit wavelength is 760 to 830 nm. Ultraviolet light has a wavelength shorter than the lower limit, and infrared light has a wavelength longer than the upper limit. Visible light of 420 nm to 700 nm is highly visible light. Examples of visible light include sunlight; light emitted by illumination such as LED lights, fluorescent lamps, and incandescent lamps; and light emitted by light sources such as xenon lamps, halogen lamps, and sodium lamps.
本明細書では、有機物は、有機物質を意味する。有機物は炭素を主な成分として含有し、有機物には、有機体（例えば、生物）を構成する物質、揮発性有機化合物、不揮発性有機化合物、生体分子、アレルゲン、有機汚染物質、薬物、汚物、ほこり、チリ、ウイルス、細菌などの微生物、病原体、および臭い成分が挙げられる。 As used herein, organic matter refers to organic substances. Organic substances contain carbon as a main component, and organic substances include substances constituting organisms (e.g. living organisms), volatile organic compounds, non-volatile organic compounds, biomolecules, allergens, organic pollutants, drugs, filth, These include dust, dirt, microorganisms such as viruses and bacteria, pathogens, and odor components.
本明細書では、アレルゲンは、免疫系を有する動物にアレルギーを引き起こす物質をいう。アレルゲンには、Ｉ型アレルギー反応の原因となる、ハウスダスト、ダニ、花粉、真菌、トルエンジシソシアネート（ＴＤＩ）、トリメリティックアンヒドリド（ＴＭＡ）、薬剤；II型アレルギー反応の原因となる、ペニシリンなどの薬剤、および細胞膜や基底膜抗原などの自己抗原；III型アレルギー反応の原因となる、細菌、薬剤、異種タンパク質、および変性IgGやDNAなどの自己抗原；IV型アレルギー反応の原因となる、細菌および真菌が挙げられる。アレルゲンとしては、気管支喘息の原因となる真菌、スギ花粉などの花粉、およびダニなどの室内塵（ハウスダスト）が代表例である。 As used herein, allergen refers to a substance that causes an allergy in animals with an immune system. Allergens include house dust, dust mites, pollen, fungi, toluene disocyanate (TDI), trimellitic anhydride (TMA), which cause type I allergic reactions, and drugs; penicillin, which causes type II allergic reactions. Bacteria, drugs, foreign proteins, and self-antigens such as denatured IgG and DNA, which cause type III allergic reactions; and self-antigens, such as denatured IgG and DNA, which cause type IV allergic reactions. Includes bacteria and fungi. Typical allergens include fungi that cause bronchial asthma, pollen such as cedar pollen, and house dust such as dust mites.
本発明者は、有機酸（特に、酢酸）が光触媒の触媒活性を向上させることを見出した。したがって、本発明によれば、光触媒の触媒活性を向上させる方法であって、酢酸と光触媒とを提供すること、および、酢酸と光触媒とを接触させることのいずれかまたは両方を含む方法が提供される。酢酸と光触媒は、水溶液中で接触させることができる。例えば、酢酸と光触媒は、酢酸を含む水溶液に光触媒を添加することによって接触させることができる。酢酸を含む溶液は、緩衝液であり得る。例えば、酢酸と、酢酸ナトリウムまたは酢酸カリウムなどの酢酸のアルカリ金属塩とを含む溶液は、ｐHの緩衝作用を発揮し、酢酸緩衝液とよばれる。 The present inventors have discovered that organic acids (particularly acetic acid) improve the catalytic activity of photocatalysts. Therefore, according to the present invention, there is provided a method for improving the catalytic activity of a photocatalyst, which includes either or both of providing acetic acid and a photocatalyst, and contacting acetic acid and a photocatalyst. Ru. Acetic acid and a photocatalyst can be brought into contact in an aqueous solution. For example, acetic acid and a photocatalyst can be brought into contact by adding the photocatalyst to an aqueous solution containing acetic acid. The solution containing acetic acid can be a buffer. For example, a solution containing acetic acid and an alkali metal salt of acetic acid, such as sodium acetate or potassium acetate, exerts a pH buffering effect and is called an acetate buffer.
本発明によれば、酢酸と光触媒との組合せが提供される。組合せにおいては、酢酸と光触媒とは、別々に含まれていても、混合された混合物（組成物）の形態で含まれていてもよい。当該組合せが、酢酸と光触媒が混合物の形態で含む場合には、酢酸と光触媒との組合せは、混合して組成物とすることができる。 According to the present invention, a combination of acetic acid and a photocatalyst is provided. In combination, acetic acid and a photocatalyst may be contained separately or in the form of a mixed mixture (composition). When the combination includes acetic acid and a photocatalyst in the form of a mixture, the combination of acetic acid and photocatalyst can be mixed to form a composition.
本発明によればまた、酢酸と光触媒を含む組成物が提供される。本発明の組成物は、水溶液であり得る。本発明の組成物は緩衝液であってもよい。緩衝液である場合には、ｐHは、４～７であってよく、５～６であってよい。本発明の組成物は、界面活性剤（例えば、非イオン性界面活性剤）をさらに含んでいてもよい。光触媒としては、特に限定されないが例えば、酸化チタンを用いることができる。 The invention also provides a composition comprising acetic acid and a photocatalyst. Compositions of the invention may be aqueous solutions. The composition of the invention may be a buffer. If it is a buffer, the pH may be between 4 and 7, and between 5 and 6. The composition of the invention may further include a surfactant (eg, a nonionic surfactant). As the photocatalyst, for example, titanium oxide can be used, although it is not particularly limited.
ある態様では、本発明の組合せにおいて光触媒は、当該組成物を含むフィルター（例えば、エアフィルター、および濾過フィルターなど）などの光触媒担持フィルターの形態；当該組成物を含む繊維、布、および衣類の形態；並びに、当該組成物を含む、塗料またはコーティング剤の形態で提供され得る。
ある態様では、本発明の酢酸と光触媒を含む組成物は、当該組成物を含むフィルター（例えば、エアフィルター、および濾過フィルターなど）などの光触媒担持フィルターの形態；当該組成物を含む繊維、布、および衣類の形態；並びに、当該組成物を含む、塗料またはコーティング剤の形態で提供され得る。
In some embodiments, in the combinations of the present invention, the photocatalyst is in the form of photocatalyst-supported filters, such as filters (e.g., air filters, filtration filters, etc.) comprising the composition; in the form of fibers, fabrics, and clothing comprising the composition. ; and may be provided in the form of a paint or coating containing the composition.
In some embodiments, the composition comprising acetic acid and a photocatalyst of the present invention is in the form of a photocatalyst-supported filter, such as a filter (e.g., an air filter, a filtration filter, etc.) comprising the composition; a fiber, cloth comprising the composition; and clothing; and in the form of a paint or coating containing the composition.
本発明によれば、酢酸と光触媒との組合せ、および酢酸と光触媒を含む組成物は、有機物を分解すること、特に微生物やアレルゲンを分解することに用いることができる。本発明によればまた、酢酸と光触媒との組合せ、および酢酸と光触媒を含む組成物は、光触媒の活性（光触媒活性）を評価することに用いることができる。本発明によればまた、酢酸と光触媒との組合せ、および酢酸と光触媒を含む組成物は、光触媒活性を増加させることに用いることができる。本発明によれば、酢酸と光触媒との組合せは、酢酸と光触媒とを接触させることに用いることができる。 According to the invention, the combination of acetic acid and a photocatalyst, and the composition comprising acetic acid and a photocatalyst, can be used to decompose organic matter, in particular to decompose microorganisms and allergens. According to the present invention, the combination of acetic acid and a photocatalyst, and the composition containing acetic acid and a photocatalyst, can also be used to evaluate the activity of a photocatalyst (photocatalytic activity). Also according to the invention, combinations of acetic acid and photocatalysts and compositions comprising acetic acid and photocatalysts can be used to increase photocatalytic activity. According to the present invention, a combination of acetic acid and a photocatalyst can be used to contact acetic acid and a photocatalyst.
例えば、酢酸と光触媒は、酢酸を含む水溶液に光触媒を添加することによって接触させることができる。酢酸を含む溶液は、緩衝液であり得る。例えば、酢酸と、酢酸ナトリウムまたは酢酸カリウムなどの酢酸のアルカリ金属塩とを含む溶液は、ｐHの緩衝作用を発揮し、このような溶液は酢酸緩衝液とよばれる。したがって、酢酸は、酢酸を含む溶液（例えば、酢酸緩衝液）の形態で、本発明の組合せおよび組成物に含まれていてもよい。酢酸と光触媒を含む組成物に対して特定の光（例えば、紫外線、可視光および赤外線など）を照射すると光触媒の光触媒活性が観察されることとなる。したがって、酢酸と光触媒との組合せ（および酢酸と光触媒を含む組成物）は、光触媒活性の活性化のために用いることができ、光触媒の光触媒活性の評価に用いることができ、有機物（例えば、病原体やアレルゲン）の分解に用いることができる。
本発明のある態様では、光触媒は、酸化チタンであり得る。この態様においては、特定の光は、紫外線であり得る。
For example, acetic acid and a photocatalyst can be brought into contact by adding the photocatalyst to an aqueous solution containing acetic acid. The solution containing acetic acid can be a buffer. For example, a solution containing acetic acid and an alkali metal salt of acetic acid, such as sodium acetate or potassium acetate, exerts a pH buffering effect, and such a solution is called an acetate buffer. Acetic acid may therefore be included in the combinations and compositions of the invention in the form of an acetic acid-containing solution (eg, an acetate buffer). When a composition containing acetic acid and a photocatalyst is irradiated with specific light (eg, ultraviolet light, visible light, infrared light, etc.), the photocatalytic activity of the photocatalyst will be observed. Therefore, combinations of acetic acid and photocatalysts (and compositions containing acetic acid and photocatalysts) can be used for the activation of photocatalytic activity, can be used to evaluate the photocatalytic activity of photocatalysts, and can be used to treat organic substances (e.g. pathogens). and allergens).
In some embodiments of the invention, the photocatalyst can be titanium oxide. In this embodiment, the particular light may be ultraviolet light.
本発明によればまた、光触媒の光触媒活性の評価方法であって、酢酸を含む溶液中で、光触媒の光触媒活性を評価することを含む、方法が提供される。本発明のこの態様では、酢酸と光触媒は、水溶液中で接触させることができる。例えば、酢酸と光触媒は、酢酸を含む水溶液に光触媒を添加することによって接触させることができる。酢酸を含む溶液は、緩衝液であり得る。例えば、酢酸と、酢酸ナトリウムまたは酢酸カリウムなどの酢酸のアルカリ金属塩とを含む溶液は、ｐHの緩衝作用を発揮し、酢酸緩衝液とよばれる。したがって、酢酸は、酢酸を含む溶液（例えば、酢酸緩衝液）であってもよい。光触媒の光触媒活性の評価は、例えば、光触媒に対して、活性化に適した波長の光を照射して行うことができる。光触媒の光触媒活性の評価はまた、光触媒により引き起こされる触媒反応を検証することにより行うことができる。触媒反応としては、水の加水分解や標準物質（例えば、アレルゲン、例えば、スギ花粉アレルゲンやダニアレルゲン）の分解が挙げられ、光触媒活性の評価に用いることができる。
したがって、本発明によれば、光触媒の光触媒活性の評価方法であって、酢酸を含む溶液中で、光触媒の光触媒活性を評価することを含む、方法は、以下(i)～(iii)のいずれか１以上またはすべてをさらに含んでいてもよい：
(i) 酢酸と光触媒は、酢酸を含む水溶液に光触媒を添加することによって接触させること；
(ii) 光触媒に対して、活性化に適した波長の光を照射して行うこと；
(iii) 標準的な光触媒（例えば、改良前の光触媒）と改良した光触媒の光触媒活性を検出し、標準的な光触媒（例えば、改良前の光触媒）と改良した光触媒の光触媒活性を比較すること。
The present invention also provides a method for evaluating the photocatalytic activity of a photocatalyst, which comprises evaluating the photocatalytic activity of the photocatalyst in a solution containing acetic acid. In this aspect of the invention, the acetic acid and photocatalyst can be contacted in an aqueous solution. For example, acetic acid and a photocatalyst can be brought into contact by adding the photocatalyst to an aqueous solution containing acetic acid. The solution containing acetic acid can be a buffer. For example, a solution containing acetic acid and an alkali metal salt of acetic acid, such as sodium acetate or potassium acetate, exerts a pH buffering effect and is called an acetate buffer. Therefore, acetic acid may be a solution containing acetic acid (eg, an acetate buffer). The photocatalytic activity of a photocatalyst can be evaluated, for example, by irradiating the photocatalyst with light of a wavelength suitable for activation. Evaluation of the photocatalytic activity of a photocatalyst can also be performed by verifying the catalytic reaction caused by the photocatalyst. Examples of catalytic reactions include water hydrolysis and decomposition of standard substances (for example, allergens, such as cedar pollen allergen and mite allergen), which can be used to evaluate photocatalytic activity.
Therefore, according to the present invention, there is provided a method for evaluating the photocatalytic activity of a photocatalyst, which method includes evaluating the photocatalytic activity of the photocatalyst in a solution containing acetic acid. It may further include one or more or all of:
(i) The acetic acid and the photocatalyst are brought into contact by adding the photocatalyst to an aqueous solution containing acetic acid;
(ii) Irradiating the photocatalyst with light of a wavelength suitable for activation;
(iii) Detecting the photocatalytic activity of the standard photocatalyst (e.g., the photocatalyst before the improvement) and the improved photocatalyst, and comparing the photocatalytic activity of the standard photocatalyst (e.g., the photocatalyst before the improvement) and the improved photocatalyst.
本発明によれば、有機物を分解する方法であって、酢酸存在下で光触媒を用いて有機物を分解することを含む、方法が提供される。この態様は、有機物と酢酸の存在下で、上記のように光触媒の光触媒活性を活性化させることによって、有機物の分解を誘発することができる。この態様では、本発明の方法は、有機物の分解中または分解後（分解処理中または分解処理後）に有機物を検出することをさらに含んでいてもよい。この態様においては、酢酸は、酢酸を含む溶液の形態で存在していてもよいし、酢酸緩衝液の形態で存在していてもよい。 According to the present invention, there is provided a method of decomposing organic matter, which method includes decomposing the organic matter using a photocatalyst in the presence of acetic acid. In this embodiment, the decomposition of the organic substance can be induced by activating the photocatalytic activity of the photocatalyst as described above in the presence of the organic substance and acetic acid. In this aspect, the method of the invention may further include detecting the organic substance during or after the decomposition of the organic substance (during or after the decomposition treatment). In this embodiment, acetic acid may be present in the form of a solution containing acetic acid or in the form of an acetate buffer.
本発明によれば、光触媒の光触媒活性を増加させる方法であって、酢酸を含む溶液と光触媒とを接触させることを含む、方法が提供される。この態様において、上記のように光触媒の光触媒活性を活性化することができる。光触媒活性は、有機物の分解および水の電気分解を含む様々な応用に用いることができる。 According to the present invention, there is provided a method for increasing the photocatalytic activity of a photocatalyst, which method includes contacting a solution containing acetic acid with the photocatalyst. In this embodiment, the photocatalytic activity of the photocatalyst can be activated as described above. Photocatalytic activity can be used in a variety of applications including the decomposition of organic matter and the electrolysis of water.
本発明によれば、酢酸と光触媒とを接触させることを含む方法が提供される。光触媒は、例えば、溶媒中で酢酸と接触させることができる。本発明の方法は、光触媒を光照射により活性化することをさら含んでいてもよい。本発明の方法はまた、光照射により活性化した光触媒により有機物を分解することをさらに含んでいてもよい。 According to the present invention, a method is provided that includes contacting acetic acid and a photocatalyst. The photocatalyst can be contacted with acetic acid in a solvent, for example. The method of the present invention may further include activating the photocatalyst by light irradiation. The method of the present invention may further include decomposing the organic substance using a photocatalyst activated by light irradiation.
本発明のすべての態様において、光触媒としては、例えば、酸化チタンが好ましく用いられ得る。本発明のすべての態様において、有機物としては、病原体およびアレルゲンが好ましく用いられ得、例えば、スギ花粉およびダニ、特にスギ花粉アレルゲンおよびダニアレルゲンが好ましく用いられ得る。本発明のすべての態様において、酢酸は、酢酸を含む溶液として、または酢酸緩衝液として提供され得る（すなわち、本明細書において、ある態様では「酢酸存在下」は、「酢酸を含む溶液中で」、または「酢酸緩衝液中で」と読み替えてもよい）。
本発明のすべての態様において、触媒は酸化チタンであり得、有機物は、病原体およびアレルゲン（特にスギ花粉およびダニ、特にスギ花粉アレルゲンおよびニアレルゲン）であり得、酢酸は、酢酸を含む溶液（特に、酢酸緩衝液）であり得る。
In all aspects of the present invention, titanium oxide, for example, can be preferably used as the photocatalyst. In all embodiments of the present invention, pathogens and allergens may be preferably used as the organic matter, for example, cedar pollen and mites, particularly cedar pollen allergen and mite allergen. In all embodiments of the invention, acetic acid may be provided as a solution containing acetic acid or as an acetate buffer (i.e., herein, in some embodiments "in the presence of acetic acid" refers to "in a solution containing acetic acid"). ” or “in acetate buffer”).
In all embodiments of the invention, the catalyst may be titanium oxide, the organic matter may be pathogens and allergens (especially cedar pollen and mites, especially cedar pollen allergens and near allergens), and the acetic acid is a solution containing acetic acid (especially , acetate buffer).
実施例１：有機物の分解試験Example 1: Decomposition test of organic matter
［材料］
有機物としては、スギ花粉アレルゲン抽出物（ITEA社、＃10103）、ダニアレルゲン抽出物（ITEA社、＃10102）を用いた。アレルゲンの分解試験溶液中の各アレルゲンの最終濃度はそれぞれ1 μg/mlであった。
光触媒としては、白色粉末状の酸化チタン（TiO2）（富士フィルム和光純薬、205-01715）を用いた。アレルゲンの分解試験溶液中の光触媒の最終濃度：0.005%（w/v)
有機物の分解試験溶液は、以下の溶媒中で行った。
酢酸溶媒（酢酸T）としては、50mM酢酸ナトリウム緩衝液（pH5.0）+0.05％Tween 20（界面活性剤）+0.05％ proclin950(防腐剤）を用いた。
リン酸緩衝生理食塩水（PBST）としては、PBS(pH7.4)+ 0.05％Tween 20 （界面活性剤） +0.05％ proclin950(防腐剤）を用いた。
有機物の分解は、それぞれの有機物用のELASA測定キットを用いて検出した。具体的には、スギ花粉アレルゲンはCry j 1 ELISAキット（ITEA社、#10204）を用いて検出し、ダニアレルゲンはDer f 1 ELISAキット（ITEA社、#10205）を用いて検出した。
[material]
As the organic substances, cedar pollen allergen extract (ITEA, #10103) and mite allergen extract (ITEA, #10102) were used. The final concentration of each allergen in the allergen degradation test solution was 1 μg/ml, respectively.
As a photocatalyst, white powdered titanium oxide (TiO 2 ) (Fuji Film Wako Pure Chemical Industries, Ltd., 205-01715) was used. Final concentration of photocatalyst in allergen degradation test solution: 0.005% (w/v)
The organic substance decomposition test solution was conducted in the following solvent.
As the acetic acid solvent (acetic acid T), 50 mM sodium acetate buffer (pH 5.0) + 0.05% Tween 20 (surfactant) + 0.05% proclin 950 (preservative) was used.
As the phosphate buffered saline (PBST), PBS (pH 7.4) + 0.05% Tween 20 (surfactant) + 0.05% proclin 950 (preservative) was used.
Decomposition of organic substances was detected using an ELASA measurement kit for each organic substance. Specifically, cedar pollen allergen was detected using the Cry j 1 ELISA kit (ITEA, #10204), and mite allergen was detected using the Der f 1 ELISA kit (ITEA, #10205).
［方法の概要］
有機物と光触媒溶液の混合液を蛍光灯照射下および遮光下で3時間、24時間、または48時間反応させた。反応後、遠心分離により回収した上清中のアレルゲン濃度をELISAによって測定した。対照として、光触媒未添加（他の操作は同様）をおいた。反応前アレルゲン溶液のアレルゲン量を100％として、照射および遮光条件下で反応させた後のそれぞれのアレルゲン量から残存率を算出した。また、各反応時間毎の遮光条件下のアレルゲン量を100％として、照射条件下のアレルゲン量の比率、すなわちアレルゲン低減率を算出した。なお、各条件はn=1で実施した。
[Overview of method]
A mixture of an organic substance and a photocatalyst solution was reacted for 3 hours, 24 hours, or 48 hours under fluorescent lamp irradiation and light shielding. After the reaction, the allergen concentration in the supernatant collected by centrifugation was measured by ELISA. As a control, no photocatalyst was added (other operations were the same). The residual rate was calculated from the respective allergen amounts after the reaction under irradiation and light shielding conditions, assuming that the allergen amount in the allergen solution before reaction was 100%. Furthermore, the ratio of the allergen amount under the irradiation condition, that is, the allergen reduction rate, was calculated by setting the allergen amount under the light-shielding condition as 100% for each reaction time. Note that each condition was performed with n=1.
酢酸緩衝液中におけるスギ花粉アレルゲン（Cry j 1）の分解試験の結果は、図１Aに示される通りである。図１Aに示されるように、スギ花粉アレルゲンは、光触媒を光照射によって活性化することによって、光照射依存的に光触媒によって分解を受けた。これに対して、リン酸緩衝食塩水中では、図１Bに示されるように、光照射によるスギ花粉アレルゲンの分解が確認された。図３には、遮光条件下でのCry j 1濃度を100％としたときの照射条件でのCry j 1の比率（低減率）を示している。スギ花粉アレルゲン(Cry j 1)は照射条件下で時間依存的に低減していることが示されており、酢酸緩衝液において顕著に効果的に低減されていることが明らかとなった。酢酸緩衝液においては24時間で顕著に低減（93％）を認めたが、PBSにおいては低減率は6％と低い。 The results of the degradation test of cedar pollen allergen (Cry j 1) in acetate buffer are shown in Figure 1A. As shown in Figure 1A, the cedar pollen allergen was decomposed by the photocatalyst in a light irradiation-dependent manner by activating the photocatalyst with light irradiation. In contrast, in phosphate buffered saline, decomposition of the cedar pollen allergen by light irradiation was confirmed, as shown in Figure 1B. FIG. 3 shows the ratio (reduction rate) of Cry j 1 under irradiation conditions when the Cry j 1 concentration under light shielding conditions is 100%. It was shown that the cedar pollen allergen (Cry j 1) was reduced in a time-dependent manner under irradiation conditions, and it was revealed that it was significantly and effectively reduced in the acetate buffer. In acetate buffer, a remarkable reduction (93%) was observed in 24 hours, but in PBS, the reduction rate was as low as 6%.
次に、ダニアレルゲンについても同様に分析した。結果は図２Aおよび２Bに示されるように図２Aに示されるように、酢酸緩衝液中においては、ダニアレルゲン（Der f 1）は、光触媒により光照射依存的に分解を受けた。これに対して、ダニアレルゲン（Der f 1）は、リン酸緩衝食塩水中では、ほとんど分解を生じなかった。図４には、遮光条件下でのDer f 1量を100％としたときの照射条件でのDer f 1量の比率（低減率）を示している。ダニアレルゲンにおいても照射条件下で時間依存的に低減していることが示されており、酢酸緩衝液において24時間で50％、48時間で76％と効果的に低減されていることが明らかとなった。一方、PBSにおいてはほとんど低減（1～2％）が認められない。 Next, mite allergen was analyzed in the same way. The results are shown in FIGS. 2A and 2B. As shown in FIG. 2A, in the acetate buffer, the mite allergen (Der f 1) was decomposed by a photocatalyst in a light irradiation-dependent manner. In contrast, the mite allergen (Der f 1) was hardly degraded in phosphate buffered saline. FIG. 4 shows the ratio (reduction rate) of the amount of Der f 1 under the irradiation conditions when the amount of Der f 1 under the light shielding condition is taken as 100%. It has been shown that mite allergen is also reduced in a time-dependent manner under irradiation conditions, and it is clear that it is effectively reduced by 50% in 24 hours and 76% in 48 hours in acetate buffer. became. On the other hand, almost no reduction (1-2%) is observed in PBS.
光触媒は光の照射によって有機物の分解を可能とするが、上記の結果により、光触媒による有機物の分解は、酢酸存在下において顕著に増大されることが明らかとなり、その分解の増大の効果は有機物の種類によらないことが明らかとなった。このことから、光触媒活性は、酢酸存在下で増強されることが示唆された。 Photocatalysts enable the decomposition of organic substances by irradiation with light, but the above results reveal that the decomposition of organic substances by photocatalysts is significantly increased in the presence of acetic acid, and the effect of increased decomposition is greater than that of organic substances. It turns out that it doesn't depend on the type. This suggested that the photocatalytic activity was enhanced in the presence of acetic acid.
実施例２：光触媒含有フィルターを用いた有機物の分解
本実施例では、表面に光触媒を含有するエアフィルターを用いて有機物の分解試験を行った。
Example 2: Decomposition of organic substances using a photocatalyst-containing filter In this example, an organic substance decomposition test was conducted using an air filter whose surface contained a photocatalyst.
本実施例では、光触媒として酸化チタン加工フィルター（１ｃｍ×１ｃｍ）を用いた以外は、実施例１と同様に有機物の分解試験を行った。酸化チタン加工フィルターは、信州セラミックス製アースプラスマスクの光触媒加工不織布層を１ｃｍ×１ｃｍサイズに切断して得た。 In this example, an organic substance decomposition test was conducted in the same manner as in Example 1, except that a titanium oxide processed filter (1 cm x 1 cm) was used as a photocatalyst. The titanium oxide processed filter was obtained by cutting the photocatalyst processed nonwoven fabric layer of an Earth Plus mask manufactured by Shinshu Ceramics into a size of 1 cm x 1 cm.
有機物と光触媒溶液の混合液を蛍光灯照射下および遮光下で24時間反応させた。反応後、遠心分離により回収した上清中のアレルゲン濃度をELISAによって測定した。対照として、光触媒未添加（他の操作は同様）をおいた。反応前アレルゲン溶液のアレルゲン量を100％として、照射および遮光条件下で反応させた後のそれぞれのアレルゲン量から残存率を算出した。なお、各条件はn=1で実施した。 A mixture of an organic substance and a photocatalyst solution was reacted for 24 hours under fluorescent lamp irradiation and light shielding. After the reaction, the allergen concentration in the supernatant collected by centrifugation was measured by ELISA. As a control, no photocatalyst was added (other operations were the same). The residual rate was calculated from the respective allergen amounts after the reaction under irradiation and light shielding conditions, assuming that the allergen amount in the allergen solution before reaction was 100%. Note that each condition was performed with n=1.
結果は、図５（Cry j 1の結果）および図６（Der f 1の結果）に示される通りであった。図５および６に示されるように、リン酸緩衝食塩水中では、いずれのアレルゲンも光依存的な低減作用は弱かったが、これに対して、酢酸緩衝液中では、光依存的なアレルゲンの低減作用は顕著に高かった。酢酸緩衝液中ではまた、アレルゲンのフィルターへの吸着も促進されていることが明らかとなった。
以上のことから、酢酸緩衝液中では、光触媒によるアレルゲンの低減作用が増強されることが明らかとなった。また、光触媒による上記アレルゲンの低減作用の増強は、アレルゲンの光触媒への吸着の増加により部分的に説明され得る。
The results were as shown in FIG. 5 (Cry j 1 results) and FIG. 6 (Der f 1 results). As shown in Figures 5 and 6, in phosphate buffered saline, the light-dependent reduction effect of all allergens was weak, whereas in acetate buffer, the light-dependent reduction of allergens was weak. The effect was significantly higher. It was also revealed that adsorption of allergens to the filter was promoted in the acetate buffer.
From the above, it has become clear that the allergen reduction effect of the photocatalyst is enhanced in the acetate buffer. Furthermore, the enhancement of the allergen reduction effect by the photocatalyst can be partially explained by the increased adsorption of the allergen to the photocatalyst.
Claims (6)
酢酸存在下かつ光照射条件下で、光触媒と酢酸以外の有機物を接触させて前記有機物を分解することと｛但し、光触媒は、表面に親水性カチオンポリマー修飾を有するものではない。｝、
分解中または分解後に前記有機物を検出することと、
を含む、方法。 A method for decomposing organic substances other than acetic acid,
In the presence of acetic acid and under light irradiation conditions, a photocatalyst and an organic substance other than acetic acid are brought into contact to decompose the organic substance {However, the photocatalyst does not have a hydrophilic cationic polymer modification on its surface. } ,
detecting the organic substance during or after decomposition;
including methods.
酢酸存在下かつ光照射条件下で、光触媒と酢酸以外の有機物を接触させて前記有機物を分解することと、
分解中または分解後に前記有機物を検出することと、
検出された前記有機物の量に基づいて光触媒の光触媒活性を評価することと｛但し、光触媒は、表面に親水性カチオンポリマー修飾を有するものではない。｝、
を含む、方法。 A method for evaluating photocatalytic activity of a photocatalyst, comprising:
decomposing the organic substance by contacting the photocatalyst with an organic substance other than acetic acid in the presence of acetic acid and under light irradiation conditions;
detecting the organic substance during or after decomposition;
Evaluating the photocatalytic activity of the photocatalyst based on the amount of the detected organic matter {However, the photocatalyst does not have a hydrophilic cationic polymer modification on its surface. } ,
including methods.
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