JP2019217445A - Photocatalyst coating agent, method for manufacturing photocatalyst coating agent and photocatalyst-supported magnetic material - Google Patents
Photocatalyst coating agent, method for manufacturing photocatalyst coating agent and photocatalyst-supported magnetic material Download PDFInfo
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- JP2019217445A JP2019217445A JP2018115922A JP2018115922A JP2019217445A JP 2019217445 A JP2019217445 A JP 2019217445A JP 2018115922 A JP2018115922 A JP 2018115922A JP 2018115922 A JP2018115922 A JP 2018115922A JP 2019217445 A JP2019217445 A JP 2019217445A
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- Prior art keywords
- photocatalyst
- coating agent
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- VEALVRVVWBQVSL-UHFFFAOYSA-N strontium titanate Chemical compound [Sr+2].[O-][Ti]([O-])=O VEALVRVVWBQVSL-UHFFFAOYSA-N 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 229910001936 tantalum oxide Inorganic materials 0.000 description 1
- 239000013077 target material Substances 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
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- 229910052718 tin Inorganic materials 0.000 description 1
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- QORWJWZARLRLPR-UHFFFAOYSA-H tricalcium bis(phosphate) Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O QORWJWZARLRLPR-UHFFFAOYSA-H 0.000 description 1
- NFACJZMKEDPNKN-UHFFFAOYSA-N trichlorfon Chemical compound COP(=O)(OC)C(O)C(Cl)(Cl)Cl NFACJZMKEDPNKN-UHFFFAOYSA-N 0.000 description 1
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Abstract
Description
本発明は、光触媒コート剤、光触媒コート剤の製造方法、及び光触媒担持磁性体に関する。 The present invention relates to a photocatalyst coating agent, a method for producing a photocatalyst coating agent, and a photocatalyst-supporting magnetic material.
光触媒は、光触媒性能を有する。光触媒性能は、例えば、空気中の有害物質の分解、悪臭原因物質の分解、水中に溶解若しくは分散した汚染物質の分解、菌類の分解、菌類の成長抑制、外壁の汚れの抑制、又は窓の汚れの抑制である。光触媒を実用化するためには、光触媒性能を損なうことなく、光触媒を基材上に固定化する必要がある。例えば、特許文献１には、アクリルシリコン塗料に光触媒乾燥粉末を含有させた光触媒性塗料が開示されている。 The photocatalyst has photocatalytic performance. Photocatalytic performance includes, for example, decomposition of harmful substances in the air, decomposition of odor-causing substances, decomposition of contaminants dissolved or dispersed in water, decomposition of fungi, suppression of fungal growth, suppression of dirt on outer walls, or contamination of windows. It is suppression of. In order to put the photocatalyst into practical use, it is necessary to fix the photocatalyst on the substrate without impairing the photocatalytic performance. For example, Patent Document 1 discloses a photocatalytic paint in which a photocatalyst dry powder is contained in an acrylic silicone paint.
しかし、特許文献１に記載の塗料を用いる場合、アクリルシリコンのようなポリマーの内部に光触媒が埋没して、ポリマーから光触媒が露出しないことがある。ポリマーから光触媒が露出しないと、光触媒の光触媒性能が低下する。また、ポリマーから光触媒を露出させるためにバインダーの量を減らすと、バインダーに対する光触媒の付着強度が低下し、バインダーから光触媒が脱離してしまう。 However, when the paint described in Patent Literature 1 is used, the photocatalyst may be buried in a polymer such as acrylic silicon, and the photocatalyst may not be exposed from the polymer. If the photocatalyst is not exposed from the polymer, the photocatalytic performance of the photocatalyst decreases. Also, if the amount of the binder is reduced to expose the photocatalyst from the polymer, the adhesion strength of the photocatalyst to the binder is reduced, and the photocatalyst is detached from the binder.
本発明は上述の課題に鑑みてなされたものであり、その目的は、光触媒の脱離を抑制しつつ、光触媒性能を向上させる光触媒コート剤、光触媒コート剤の製造方法、及び光触媒担持磁性体を提供することである。 The present invention has been made in view of the above-described problems, and an object of the present invention is to provide a photocatalyst coating agent that improves photocatalytic performance while suppressing desorption of a photocatalyst, a method for manufacturing a photocatalyst coating agent, and a photocatalyst-supporting magnetic material. To provide.
本発明の光触媒コート剤は、少なくとも２種の光触媒と、バインダーとを含有する。前記少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有する。前記第１光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が最も小さい。前記第２光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が２番目に小さい。前記第２光触媒の平均一次粒子径は、前記第１光触媒の平均一次粒子径の２．０倍以上である。 The photocatalyst coating agent of the present invention contains at least two types of photocatalysts and a binder. The at least two types of photocatalysts include at least a first photocatalyst and a second photocatalyst. The first photocatalyst has the smallest average primary particle diameter among the at least two types of photocatalysts. The second photocatalyst has the second smallest average primary particle diameter among the at least two types of photocatalysts. The average primary particle diameter of the second photocatalyst is at least 2.0 times the average primary particle diameter of the first photocatalyst.
本発明の光触媒コート剤の製造方法は、前記少なくとも２種の光触媒と、前記バインダーとを混合する工程を含む。製造される前記光触媒コート剤は、上述した光触媒コート剤である。 The method for producing a photocatalyst coating agent of the present invention includes a step of mixing the at least two kinds of photocatalysts and the binder. The manufactured photocatalyst coating agent is the photocatalyst coating agent described above.
本発明の光触媒担持磁性体は、磁性材料を含有するコアと、前記コアを被覆するコート層とを備える。前記コート層は、少なくとも２種の光触媒と、バインダーとを含有する。前記少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有する。前記第１光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が最も小さい。前記第２光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が２番目に小さい。前記第２光触媒の平均一次粒子径は、前記第１光触媒の平均一次粒子径の２．０倍以上である。 The photocatalyst-supporting magnetic body of the present invention includes a core containing a magnetic material, and a coat layer covering the core. The coat layer contains at least two kinds of photocatalysts and a binder. The at least two types of photocatalysts include at least a first photocatalyst and a second photocatalyst. The first photocatalyst has the smallest average primary particle diameter among the at least two types of photocatalysts. The second photocatalyst has the second smallest average primary particle diameter among the at least two types of photocatalysts. The average primary particle diameter of the second photocatalyst is at least 2.0 times the average primary particle diameter of the first photocatalyst.
本発明の光触媒コート剤及び光触媒担持磁性体は、光触媒の脱離を抑制しつつ、光触媒性能を向上させることができる。本発明の製造方法により製造された光触媒コート剤は、光触媒の脱離を抑制しつつ、光触媒性能を向上させることができる。 The photocatalyst coating agent and the photocatalyst-supporting magnetic material of the present invention can improve the photocatalytic performance while suppressing the desorption of the photocatalyst. The photocatalyst coating agent produced by the production method of the present invention can improve photocatalytic performance while suppressing desorption of the photocatalyst.
以下、本発明の実施形態について説明する。なお、本発明は、実施形態に何ら限定されず、本発明の目的の範囲内で適宜変更を加えて実施できる。 Hereinafter, embodiments of the present invention will be described. The present invention is not limited to the embodiments at all, and can be implemented with appropriate modifications within the scope of the present invention.
＜第１実施形態：光触媒コート剤＞
本発明の第１実施形態は、光触媒コート剤に関する。第１実施形態に係る光触媒コート剤は、少なくとも２種の光触媒と、バインダーとを含有する。
<First embodiment: photocatalyst coating agent>
The first embodiment of the present invention relates to a photocatalyst coating agent. The photocatalyst coating agent according to the first embodiment contains at least two types of photocatalysts and a binder.
（光触媒）
光触媒コート剤は、光触媒として、少なくとも２種の光触媒を含有する。少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有する。第１光触媒は、光触媒コート剤に含有される少なくとも２種の光触媒のうちで、平均一次粒子径が最も小さい光触媒である。第２光触媒は、光触媒コート剤に含有される少なくとも２種の光触媒のうちで、平均一次粒子径が２番目に小さい光触媒である。なお、第１光触媒、及び第２光触媒、は、各々、第１光触媒粒子から構成される粉体、及び第２光触媒粒子から構成される粉体である。光触媒コート剤は、光触媒として、２種又は３種の光触媒を含有することが好ましい。
(photocatalyst)
The photocatalyst coating agent contains at least two types of photocatalysts as photocatalysts. At least two types of photocatalysts contain at least a first photocatalyst and a second photocatalyst. The first photocatalyst is a photocatalyst having the smallest average primary particle diameter among at least two types of photocatalysts contained in the photocatalyst coating agent. The second photocatalyst is a photocatalyst having the second smallest average primary particle diameter among at least two types of photocatalysts contained in the photocatalyst coating agent. Note that the first photocatalyst and the second photocatalyst are a powder composed of the first photocatalyst particles and a powder composed of the second photocatalyst particles, respectively. The photocatalyst coating agent preferably contains two or three types of photocatalysts as photocatalysts.
第１実施形態に係る光触媒コート剤が、平均一次粒子径が小さい第１光触媒と、平均一次粒子径が大きい第２光触媒とを含有することで、次の第１から第３の利点が得られる。まず、第１の利点について説明する。光触媒コート剤が基材に塗布され乾燥された場合に、平均一次粒子径が大きい第２光触媒を構成する第２光触媒粒子の表面の一部が、バインダーから露出する。第２光触媒粒子の表面の一部が露出することで、第２光触媒が分解対象物と接触でき、第２光触媒によって分解対象物が好適に分解される。これにより、光触媒性能を向上できる。 Since the photocatalyst coating agent according to the first embodiment contains the first photocatalyst having a small average primary particle diameter and the second photocatalyst having a large average primary particle diameter, the following first to third advantages can be obtained. . First, the first advantage will be described. When the photocatalyst coating agent is applied to the substrate and dried, a part of the surface of the second photocatalyst particles constituting the second photocatalyst having a large average primary particle diameter is exposed from the binder. By exposing a part of the surface of the second photocatalyst particles, the second photocatalyst can come into contact with the decomposition target, and the decomposition target is suitably decomposed by the second photocatalyst. Thereby, the photocatalytic performance can be improved.
次に、第２の利点について説明する。光触媒コート剤が基材に塗布され乾燥された場合に、平均一次粒子径が小さい第１光触媒を構成する第１光触媒粒子が、第２光触媒粒子の表面に付着する。バインダーから露出している第２光触媒粒子の表面に第１光触媒粒子が付着した場合、この第１光触媒粒子の表面積分、バインダーから露出する光触媒粒子（第１光触媒粒子及び第２光触媒粒子）の表面積を拡大できる。これにより、光触媒性能が一層向上する。 Next, a second advantage will be described. When the photocatalyst coating agent is applied to the substrate and dried, the first photocatalyst particles constituting the first photocatalyst having a small average primary particle diameter adhere to the surface of the second photocatalyst particles. When the first photocatalyst particles adhere to the surface of the second photocatalyst particles exposed from the binder, the surface integral of the first photocatalyst particles, the surface area of the photocatalyst particles (first and second photocatalyst particles) exposed from the binder Can be expanded. Thereby, the photocatalytic performance is further improved.
次に、第３の利点について説明する。既に述べたように、光触媒コート剤が基材に塗布され乾燥された場合に、平均一次粒子径が小さい第１光触媒を構成する第１光触媒粒子が、第２光触媒粒子の表面に付着する。バインダーから露出していない第２光触媒粒子の表面に第１光触媒粒子が付着した場合、凝集力によって第１光触媒粒子が第２光触媒粒子に強く引き寄せられているため、バインダー内に位置する第１光触媒粒子によって第２光触媒粒子がバインダーから脱離し難くなる。 Next, a third advantage will be described. As described above, when the photocatalyst coating agent is applied to the base material and dried, the first photocatalyst particles constituting the first photocatalyst having a small average primary particle diameter adhere to the surface of the second photocatalyst particles. When the first photocatalyst particles adhere to the surface of the second photocatalyst particles that are not exposed from the binder, the first photocatalyst particles located in the binder are strongly attracted to the second photocatalyst particles by the cohesive force. The particles make it difficult for the second photocatalyst particles to be detached from the binder.
なお、光触媒により分解される分解対象物としては、例えば、有機リン殺虫剤（より具体的には、ジクロボス（ＤＤＶＰ）、ビニフェート、ランガード、Ｏ−エチル Ｏ−４−ニトロフェニルフェニルフォスホノチオエート（ＥＰＮ）、ジプテレックス、スミチオン、ダイアジノン、エストックス、ダイシストン、マラソン、エカチン、スプラサイド、及びオルトラン等）、有機塩素除草剤及び有機塩素殺虫剤（より具体的には、クロロネブ、ＤＤＶＰ、ヘキサクロロベンゼン、α−ヘキサクロロシクロヘキサン、及びβ−ヘキサクロロシクロヘキサン等）、カーバメイト除草剤（より具体的には、チオベンカルブメフェナセット等）、ジフェニルエーテル除草剤（より具体的には、クロロニトロフェン等）、フェノール類（より具体的には、トリクロロフェノール等）、アルキルフェノール類（より具体的には、４−ｔ−ブチルフェノール、４−ｎ−ペンチルフェノール、４−ｎ−ヘキシルフェノール、４−ヘプチルフェノール、４−ｔ−オクチルフェノール、４−ｎ−オクチルフェノール、及びノニルフェノール等）、並びに揮発性有機化合物（ＶＯＣ、より具体的には、ホルムアルデヒド、アセトアルデヒド、及びアンモニア等）が挙げられる。 In addition, as a decomposition | disassembly target object decomposed | disassembled by a photocatalyst, an organic phosphorus insecticide (more specifically, diclo boss (DDVP), vinylite, languard, O-ethyl O-4-nitrophenyl phenylphosphonothioate ( EPN), dipterex, sumithion, diazinon, estocks, diciston, marathon, ecatin, supraside, and orthotran, etc., organochlorine herbicides and organochlorine pesticides (more specifically, chloroneb, DDVP, hexachlorobenzene, α) -Hexachlorocyclohexane and β-hexachlorocyclohexane, etc.), carbamate herbicides (more specifically, thiobencarb mefenacet etc.), diphenyl ether herbicides (more specifically, chloronitrophen etc.), phenols (more specifically, , Alkylphenols (more specifically, 4-t-butylphenol, 4-n-pentylphenol, 4-n-hexylphenol, 4-heptylphenol, 4-t-octylphenol, 4-n- Octyl phenol, nonyl phenol, etc.), and volatile organic compounds (VOC, more specifically, formaldehyde, acetaldehyde, ammonia, etc.).
第２光触媒の平均一次粒子径は、第１光触媒の平均一次粒子径の２．０倍以上である。即ち、第１光触媒の平均一次粒子径に対する、第２光触媒の平均一次粒子径の比率（第２光触媒の平均一次粒子径／第１光触媒の平均一次粒子径）は、２．０以上である。第２光触媒の平均一次粒子径が第１光触媒の平均一次粒子径の２．０倍以上であることで、第１光触媒の平均一次粒子径と第２光触媒の平均一次粒子径との差が大きくなり、既に述べた第１から第３の利点を好適に得ることができる。 The average primary particle diameter of the second photocatalyst is at least 2.0 times the average primary particle diameter of the first photocatalyst. That is, the ratio of the average primary particle diameter of the second photocatalyst to the average primary particle diameter of the first photocatalyst (the average primary particle diameter of the second photocatalyst / the average primary particle diameter of the first photocatalyst) is 2.0 or more. When the average primary particle diameter of the second photocatalyst is at least 2.0 times the average primary particle diameter of the first photocatalyst, the difference between the average primary particle diameter of the first photocatalyst and the average primary particle diameter of the second photocatalyst is large. Thus, the above-described first to third advantages can be suitably obtained.
光触媒の脱離を抑制しつつ、光触媒性能を向上させるためには、第２光触媒の平均一次粒子径は、第１光触媒の平均一次粒子径の２．０倍以上５．０倍以下であることが好ましく、２．５倍以上５．０倍以下であることがより好ましく、３．０倍以上５．０倍以下であることが一層好ましく、３．５倍以上５．０倍以下であることがより一層好ましく、４．０倍以上５．０倍以下であることが特に好ましい。なお、第２光触媒の平均一次粒子径は、第１光触媒の平均一次粒子径の２．０倍、２．１倍、２．５倍、３．５倍、４．０倍、及び５．０倍から選ばれる２つの値の範囲内であってもよい。 In order to improve the photocatalytic performance while suppressing the desorption of the photocatalyst, the average primary particle diameter of the second photocatalyst should be 2.0 times or more and 5.0 times or less the average primary particle diameter of the first photocatalyst. Is preferably 2.5 times or more and 5.0 times or less, more preferably 3.0 times or more and 5.0 times or less, and even more preferably 3.5 times or more and 5.0 times or less. Is still more preferable, and it is particularly preferable that it is 4.0 times or more and 5.0 times or less. The average primary particle diameter of the second photocatalyst was 2.0 times, 2.1 times, 2.5 times, 3.5 times, 4.0 times, and 5.0 times the average primary particle diameter of the first photocatalyst. It may be in the range of two values selected from the double.
光触媒コート剤は、光触媒として、第１光触媒及び第２光触媒のみを含有していてもよい。また、光触媒コート剤は、光触媒として、第１光触媒及び第２光触媒に加えて、第１光触媒及び第２光触媒以外の光触媒（以下「その他の光触媒」と記載することがある）を更に含有していてもよい。その他の光触媒が含有される場合、光触媒コート剤は、少なくとも３種の光触媒を含有する。その他の光触媒の平均一次粒子径は、第２光触媒の平均一次粒子径よりも大きい。その他の光触媒は、光触媒コート剤に含有される少なくとも３種（例えば、３種）の光触媒のうちで、平均一次粒子径が小さい方から３番目以上（例えば、３番目）である光触媒である。なお、その他の光触媒は、その他の光触媒粒子から構成される粉体である。 The photocatalyst coating agent may contain only the first and second photocatalysts as photocatalysts. In addition, the photocatalyst coating agent further contains, as a photocatalyst, a photocatalyst other than the first and second photocatalysts (hereinafter sometimes referred to as “other photocatalysts”) in addition to the first and second photocatalysts. You may. When other photocatalysts are contained, the photocatalyst coating agent contains at least three types of photocatalysts. The average primary particle diameter of other photocatalysts is larger than the average primary particle diameter of the second photocatalyst. The other photocatalyst is a photocatalyst that is the third or more (for example, the third) photocatalyst among the at least three (for example, three) photocatalysts contained in the photocatalyst coating agent, which has the smaller average primary particle diameter. The other photocatalyst is a powder composed of other photocatalyst particles.
第１光触媒の平均一次粒子径、第２光触媒の平均一次粒子径、及びその他の光触媒の平均一次粒子径は、各々、１ｎｍ以上１００ｎｍ以下であることが好ましく、５ｎｍ以上５０ｎｍ以下であることがより好ましい。第１光触媒の平均一次粒子径、第２光触媒の平均一次粒子径、及びその他の光触媒の平均一次粒子径が５ｎｍ以上であると、各光触媒が凝集し難くなる。一方、第１光触媒の平均一次粒子径、第２光触媒の平均一次粒子径、及びその他の光触媒の平均一次粒子径が５０ｎｍ以下であると、光触媒コート剤中に各光触媒を均一に分散させ易い。また、第１光触媒の平均一次粒子径、第２光触媒の平均一次粒子径、及びその他の光触媒の平均一次粒子径が５０ｎｍ以下であると、バインダーから各光触媒が脱離することを好適に抑制できる。 The average primary particle diameter of the first photocatalyst, the average primary particle diameter of the second photocatalyst, and the average primary particle diameter of other photocatalysts are each preferably 1 nm or more and 100 nm or less, more preferably 5 nm or more and 50 nm or less. preferable. When the average primary particle size of the first photocatalyst, the average primary particle size of the second photocatalyst, and the average primary particle size of the other photocatalysts are 5 nm or more, it becomes difficult for each photocatalyst to aggregate. On the other hand, when the average primary particle diameter of the first photocatalyst, the average primary particle diameter of the second photocatalyst, and the average primary particle diameter of the other photocatalysts are 50 nm or less, it is easy to uniformly disperse each photocatalyst in the photocatalyst coating agent. When the average primary particle diameter of the first photocatalyst, the average primary particle diameter of the second photocatalyst, and the average primary particle diameter of the other photocatalysts are 50 nm or less, the desorption of each photocatalyst from the binder can be suitably suppressed. .
光触媒の脱離を抑制しつつ、光触媒性能を向上させるためには、第１光触媒の平均一次粒子径は、５ｎｍ以上１５ｎｍ以下であることが一層好ましい。また、第１光触媒の平均一次粒子径は、５ｎｍ、１０ｎｍ、及び１５ｎｍから選ばれる２つの値の範囲内であってもよい。例えば、第１光触媒の平均一次粒子径は、５ｎｍ以上１０ｎｍ以下、及び１０ｎｍ以上１５ｎｍ以下の何れかであってもよい。 In order to improve the photocatalytic performance while suppressing the desorption of the photocatalyst, the average primary particle diameter of the first photocatalyst is more preferably from 5 nm to 15 nm. Further, the average primary particle diameter of the first photocatalyst may be in a range of two values selected from 5 nm, 10 nm, and 15 nm. For example, the average primary particle diameter of the first photocatalyst may be any one of 5 nm to 10 nm, and 10 nm to 15 nm.
光触媒の脱離を抑制しつつ、光触媒性能を向上させるためには、第２光触媒の平均一次粒子径は、１５ｎｍ以上３０ｎｍ以下であることが一層好ましく、１５ｎｍより大きく３０ｎｍ以下であることが特に好ましい。また、第２光触媒の平均一次粒子径は、１５ｎｍ、２０ｎｍ、２５ｎｍ、及び３０ｎｍから選ばれる２つの値の範囲内であってもよい。例えば、第２光触媒の平均一次粒子径は、１５ｎｍ以上２０ｎｍ以下、１５ｎｍ以上２５ｎｍ以下、２０ｎｍ以上２５ｎｍ以下、２０ｎｍ以上３０ｎｍ以下、及び２５ｎｍ以上３０ｎｍ以下の何れかであってもよい。 In order to improve the photocatalytic performance while suppressing the desorption of the photocatalyst, the average primary particle diameter of the second photocatalyst is more preferably 15 nm or more and 30 nm or less, and particularly preferably larger than 15 nm and 30 nm or less. . In addition, the average primary particle diameter of the second photocatalyst may be in a range of two values selected from 15 nm, 20 nm, 25 nm, and 30 nm. For example, the average primary particle diameter of the second photocatalyst may be any one of 15 nm to 20 nm, 15 nm to 25 nm, 20 nm to 25 nm, 20 nm to 30 nm, and 25 nm to 30 nm.
その他の光触媒の平均一次粒子径は、第２光触媒の平均一次粒子径よりも大きく且つ３０ｎｍ以上５０ｎｍ以下であることが一層好ましい。 The average primary particle diameter of the other photocatalyst is more preferably larger than the average primary particle diameter of the second photocatalyst and 30 nm or more and 50 nm or less.
光触媒の平均一次粒子径は、後述する実施例に記載の方法、又はその代替法により測定できる。 The average primary particle diameter of the photocatalyst can be measured by the method described in Examples described later or an alternative method thereof.
光触媒の脱離を抑制しつつ、光触媒性能を向上させるためには、第２光触媒の体積Ｖ２に対する、第１光触媒の体積Ｖ１の比率Ｖ１／Ｖ２は、２．０以上５．０以下であることが好ましい。また、比率Ｖ１／Ｖ２は、２．０、２．５、３．０、３．５、４．０、４．５、及び５．０から選ばれる２つの値の範囲内であってもよい。 In order to improve the photocatalytic performance while suppressing the desorption of the photocatalyst, the ratio V1 / V2 of the volume V1 of the first photocatalyst to the volume V2 of the second photocatalyst should be 2.0 or more and 5.0 or less. Is preferred. Further, the ratio V1 / V2 may be within a range of two values selected from 2.0, 2.5, 3.0, 3.5, 4.0, 4.5, and 5.0. .
第１光触媒の体積Ｖ１と第２光触媒の体積Ｖ２との合計含有率は、少なくとも２種の光触媒の総体積ＶＣに対して、９５体積％以上であることが好ましく、９６体積％以上であることがより好ましく、１００体積％であることが特に好ましい。 The total content of the volume V1 of the first photocatalyst and the volume V2 of the second photocatalyst is preferably at least 95% by volume, more preferably at least 96% by volume, based on the total volume VC of at least two types of photocatalysts. Is more preferable, and particularly preferably 100% by volume.
光触媒コート剤に含有される第１光触媒の体積Ｖ１は、式「Ｖ１＝第１光触媒の重量／第１光触媒の密度」から算出される。光触媒コート剤に含有される第２光触媒の体積Ｖ２は、式「Ｖ２＝第２光触媒の重量／第２光触媒の密度」から算出される。光触媒コート剤に含有されるその他の光触媒の体積Ｖ３は、式「Ｖ３＝その他の光触媒の重量／その他の光触媒の密度」から算出される。少なくとも２種の光触媒の総体積ＶＣは、式「ＶＣ＝第１光触媒の体積Ｖ１＋第２光触媒の体積Ｖ２＋その他の光触媒の体積Ｖ３」から算出される。 The volume V1 of the first photocatalyst contained in the photocatalyst coating agent is calculated from the equation “V1 = weight of first photocatalyst / density of first photocatalyst”. The volume V2 of the second photocatalyst contained in the photocatalyst coating agent is calculated from the equation “V2 = weight of second photocatalyst / density of second photocatalyst”. The volume V3 of the other photocatalyst contained in the photocatalyst coating agent is calculated from the equation “V3 = weight of other photocatalyst / density of other photocatalyst”. The total volume VC of at least two types of photocatalysts is calculated from the equation “VC = volume of first photocatalyst V1 + volume of second photocatalyst V2 + volume of other photocatalysts V3”.
第１光触媒、第２光触媒、及びその他の光触媒を構成する材料は、特に限定されず、例えば、酸化チタン、酸化タングステン、チタン酸ストロンチウム（より具体的には、ＳｒＴｉＯ3）、酸化ニオブ（より具体的には、Ｎｂ2Ｏ5）、酸化タンタル（より具体的には、Ｔａ2Ｏ5）、酸化ジルコニウム（より具体的には、ＺｒＯ2）、酸化ビスマス（より具体的には、Ｂｉ2Ｏ3）、及び酸化鉄（より具体的には、Ｆｅ2Ｏ3）が挙げられる。第１光触媒、第２光触媒、及びその他の光触媒を構成する材料としては、酸化チタン、又は酸化タングステンが好ましい。 The materials constituting the first photocatalyst, the second photocatalyst, and other photocatalysts are not particularly limited. For example, titanium oxide, tungsten oxide, strontium titanate (more specifically, SrTiO 3 ), niobium oxide (more specifically, Specifically, Nb 2 O 5 ), tantalum oxide (more specifically, Ta 2 O 5 ), zirconium oxide (more specifically, ZrO 2 ), bismuth oxide (more specifically, Bi 2 O) 3 ) and iron oxide (more specifically, Fe 2 O 3 ). As a material constituting the first photocatalyst, the second photocatalyst, and another photocatalyst, titanium oxide or tungsten oxide is preferable.
酸化チタンは、ＴｉＯ2（二酸化チタン）である。酸化チタンの結晶構造としては、例えば、アナターゼ型、及びルチル型が挙げられる。光触媒性能を向上させるために、酸化チタンの結晶構造としては、アナターゼ型が好ましい。 Titanium oxide is TiO 2 (titanium dioxide). Examples of the crystal structure of titanium oxide include an anatase type and a rutile type. In order to improve the photocatalytic performance, the crystal structure of titanium oxide is preferably an anatase type.
酸化タングステンとしては、例えば、ＷＯ3（三酸化タングステン）、ＷＯ2、ＷＯ、Ｗ2Ｏ3、Ｗ4Ｏ5、Ｗ4Ｏ11、Ｗ25Ｏ73、Ｗ20Ｏ58、及びＷ24Ｏ68、並びにこれらの混合物が挙げられる。光触媒性能を向上させるために、酸化タングステンとしては、ＷＯ3が好ましい。酸化タングステンの結晶構造としては、例えば、単斜晶、三斜晶、斜方晶、及びこれらの少なくとも２種の混晶が挙げられる。 The tungsten oxide, for example, WO 3 (tungsten trioxide), WO 2, WO, W 2 O 3, W 4 O 5, W 4 O 11, W 25 O 73, W 20 O 58, and W 24 O 68 , As well as mixtures thereof. WO 3 is preferably used as tungsten oxide in order to improve the photocatalytic performance. Examples of the crystal structure of tungsten oxide include a monoclinic crystal, a triclinic crystal, an orthorhombic crystal, and a mixed crystal of at least two of these.
光触媒のエネルギーギャップを小さくして可視光領域での光触媒の応答性を向上させるために、光触媒は助触媒を担持していていもよい。助触媒としては、例えば、白金（Ｐｔ）、パラジウム（Ｐｄ）、ロジウム（Ｒｈ）、ルテニウム（Ｒｕ）、オスミウム（Ｏｓ）、イリジウム（Ｉｒ）、金（Ａｕ）、銀（Ａｇ）、銅（Ｃｕ）、亜鉛（Ｚｎ）、鉄、ニッケル、ニオブ、ジルコニウム、及びモリブデンが挙げられる。これらの金属は、例えば、錯体、塩化物、臭化物、沃化物、酸化物、水酸化物、硫酸塩、硝酸塩、炭酸塩、酢酸塩、燐酸塩、又は有機酸塩の形態で、助触媒として含有されていてもよい。助触媒としては、白金、パラジウム、ロジウム、ルテニウム、オスミウム、又はイリジウムが好ましく、白金がより好ましい。光触媒に対する助触媒の含有率（以下、助触媒担持率と記載することがある）は、０．０１重量％以上３重量％以下であることが好ましい。助触媒担持率がこのような範囲内であると、光触媒の光触媒性能を更に向上できる。 In order to reduce the energy gap of the photocatalyst and improve the responsiveness of the photocatalyst in the visible light region, the photocatalyst may carry a promoter. Examples of the promoter include platinum (Pt), palladium (Pd), rhodium (Rh), ruthenium (Ru), osmium (Os), iridium (Ir), gold (Au), silver (Ag), and copper (Cu). ), Zinc (Zn), iron, nickel, niobium, zirconium, and molybdenum. These metals are included as cocatalysts, for example, in the form of complexes, chlorides, bromides, iodides, oxides, hydroxides, sulfates, nitrates, carbonates, acetates, phosphates or organic acid salts. It may be. As the promoter, platinum, palladium, rhodium, ruthenium, osmium, or iridium is preferable, and platinum is more preferable. The content of the cocatalyst with respect to the photocatalyst (hereinafter, sometimes referred to as the cocatalyst carrying rate) is preferably 0.01% by weight or more and 3% by weight or less. When the cocatalyst carrying ratio is within such a range, the photocatalytic performance of the photocatalyst can be further improved.
第１光触媒は、酸化チタン又は酸化タングステンを含有することが好ましく、酸化チタンを含有することがより好ましく、アナターゼ型の酸化チタンを含有することが一層好ましい。第２光触媒は、酸化チタン又は酸化タングステンを含有することが好ましい。第２光触媒が含有する酸化チタンは、アナターゼ型の酸化チタンであることが好ましい。第２光触媒が含有する酸化タングステンは、白金を担持した酸化タングステンであることが好ましく、白金を担持した三酸化タングステンであることがより好ましい。第１光触媒を構成する材料は、第２光触媒を構成する材料と同一であってもよく、異なっていてもよい。その他の光触媒は、酸化チタン又は酸化タングステンを含有することが好ましく、酸化チタンを含有することがより好ましく、アナターゼ型の酸化チタンを含有することが一層好ましい。 The first photocatalyst preferably contains titanium oxide or tungsten oxide, more preferably contains titanium oxide, and even more preferably contains anatase-type titanium oxide. The second photocatalyst preferably contains titanium oxide or tungsten oxide. The titanium oxide contained in the second photocatalyst is preferably an anatase type titanium oxide. The tungsten oxide contained in the second photocatalyst is preferably a tungsten oxide carrying platinum, more preferably a tungsten trioxide carrying platinum. The material forming the first photocatalyst may be the same as or different from the material forming the second photocatalyst. The other photocatalyst preferably contains titanium oxide or tungsten oxide, more preferably contains titanium oxide, and even more preferably contains anatase-type titanium oxide.
（バインダー）
バインダーは、特に限定されない。バインダーの例としては、バインダー樹脂が挙げられる。バインダー樹脂としては、例えば、シリコーン樹脂、エポキシ樹脂、ウレタン樹脂、フェノール樹脂、アクリル樹脂、スチレン樹脂、ポリアミド樹脂、ポリエステル樹脂、アセタール樹脂、ポリカーボネート樹脂、塩化ビニル樹脂、酢酸ビニル樹脂、セルロース樹脂、及びポリオレフィン樹脂が挙げられる。バインダー樹脂は、これらの樹脂を共重合させた共重合体であってもよい。バインダー樹脂は、これらの樹脂の混合物であってもよい。バインダーの別の例としては、ガラスが挙げられる。光及び熱に強く、光触媒によって分解され難いことから、バインダーとしては、シリコーン樹脂又はガラスが好ましい。加工が容易であることから、バインダーとしては、シリコーン樹脂がより好ましい。
(binder)
The binder is not particularly limited. Examples of the binder include a binder resin. Examples of the binder resin include silicone resin, epoxy resin, urethane resin, phenol resin, acrylic resin, styrene resin, polyamide resin, polyester resin, acetal resin, polycarbonate resin, vinyl chloride resin, vinyl acetate resin, cellulose resin, and polyolefin. Resins. The binder resin may be a copolymer obtained by copolymerizing these resins. The binder resin may be a mixture of these resins. Another example of a binder includes glass. Silicone resin or glass is preferred as the binder because it is resistant to light and heat and is not easily decomposed by a photocatalyst. Since the processing is easy, a silicone resin is more preferable as the binder.
シリコーン樹脂として、市販品を使用してもよい。市販のシリコーン樹脂の例としては、東レ・ダウコーニング株式会社製のＢＡ２４００、ＢＡ２４１０、ＢＡ２４１１、ＢＡ２５１０、ＢＡ２４０５、８４０ＲＥＳＩＮ、及び８０４ＲＥＳＩＮが挙げられる。市販のシリコーン樹脂の別の例としては、信越化学工業株式会社製のＫＲ−３５０、ＫＲ−２７１、ＫＲ−２７２、ＫＲ−２７４、ＫＲ−２１６、ＫＲ−２８０、ＫＲ−２８２、ＫＲ−２６１、ＫＲ−２６０、ＫＲ−２５５、ＫＲ−２６６、ＫＲ−２５１、ＫＲ−１５５、ＫＲ−１５２、ＫＲ−２１４、ＫＲ−２２０、ＫＲ−２２０ＬＰ、Ｘ−４０４０−１７１、ＫＲ−２０１、ＫＲ−５２０２、及びＫＲ−３０９３が挙げられる。 A commercially available product may be used as the silicone resin. Examples of commercially available silicone resins include BA2400, BA2410, BA2411, BA2510, BA2405, 840RESIN, and 804RESIN manufactured by Dow Corning Toray Co., Ltd. As another example of a commercially available silicone resin, KR-350, KR-271, KR-272, KR-274, KR-216, KR-280, KR-282, KR-261, manufactured by Shin-Etsu Chemical Co., Ltd. KR-260, KR-255, KR-266, KR-251, KR-155, KR-152, KR-214, KR-220, KR-220LP, X-4040-171, KR-201, KR-5202, And KR-3093.
バインダーの体積ＶＢに対する、少なくとも２種の光触媒の総体積ＶＣの比率ＶＣ／ＶＢは、２．０以上１０．０以下であることが好ましい。比率ＶＣ／ＶＢが２．０以上であると、光触媒の含有量が多くなり、光触媒がバインダーから好適に露出する。これにより、光触媒が分解対象物と接触して、光触媒によって分解対象物が好適に分解され、光触媒性能を向上できる。比率ＶＣ／ＶＢが１０．０以下であると、光触媒の含有量が多くなり過ぎず、バインダーに対する光触媒の付着強度が高まり、バインダーからの光触媒の脱離を好適に抑制できる。比率ＶＣ／ＶＢは、２．０、２．５、３．０、３．５、５．０、６．０、７．０、８．０、９．０、及び１０．０から選ばれる２つの値の範囲内であってもよい。光触媒コート剤に含有されるバインダーの体積ＶＢは、式「ＶＢ＝バインダーの重量／バインダーの密度」から算出される。なお、バインダーが液状又はエマルション状である場合には、バインダーの体積ＶＢは、バインダーの固形分の体積である。 The ratio VC / VB of the total volume VC of at least two types of photocatalysts to the volume VB of the binder is preferably 2.0 or more and 10.0 or less. When the ratio VC / VB is 2.0 or more, the content of the photocatalyst increases, and the photocatalyst is suitably exposed from the binder. Accordingly, the photocatalyst comes into contact with the decomposition target, and the decomposition target is suitably decomposed by the photocatalyst, and the photocatalytic performance can be improved. When the ratio VC / VB is 10.0 or less, the content of the photocatalyst does not become too large, the adhesion strength of the photocatalyst to the binder is increased, and the desorption of the photocatalyst from the binder can be suitably suppressed. The ratio VC / VB is selected from 2.0, 2.5, 3.0, 3.5, 5.0, 6.0, 7.0, 8.0, 9.0, and 10.0. It may be in the range of two values. The volume VB of the binder contained in the photocatalyst coating agent is calculated from the formula “VB = weight of binder / density of binder”. When the binder is in a liquid or emulsion state, the volume VB of the binder is the volume of the solid content of the binder.
（添加剤）
光触媒コート剤は、必要に応じて、添加剤を更に含有してもよい。添加剤としては、例えば、珪素化合物、アルミニウム化合物、アルミノ珪酸塩、アルカリ土類金属、リン酸カルシウム、モレキュラーシーブ、及び活性炭が挙げられる。
(Additive)
The photocatalyst coating agent may further contain an additive, if necessary. Examples of the additive include a silicon compound, an aluminum compound, an aluminosilicate, an alkaline earth metal, calcium phosphate, molecular sieve, and activated carbon.
（溶媒）
光触媒コート剤は、必要に応じて、溶媒を更に含有してもよい。溶媒としては、例えば極性溶媒が挙げられる。極性溶媒としては、例えば、水、メタノール、エタノール、及びプロパノール（より具体的には、２−プロパノール）が挙げられる。以上、第１実施形態に係る光触媒コート剤について説明した。
(solvent)
The photocatalyst coating agent may further contain a solvent, if necessary. Examples of the solvent include a polar solvent. Examples of the polar solvent include water, methanol, ethanol, and propanol (more specifically, 2-propanol). The photocatalyst coating agent according to the first embodiment has been described above.
＜第２実施形態：光触媒コート剤の製造方法＞
本発明の第２実施形態は、光触媒コート剤の製造方法に関する。第２実施形態に係る光触媒コート剤の製造方法は、第１実施形態に係る光触媒コート剤を製造する方法である。第２実施形態に係る光触媒コート剤の製造方法は、少なくとも２種の光触媒と、バインダーとを混合する工程（混合工程）を含む。必要に応じて、混合工程において、その他の光触媒を更に添加してもよい。また、必要に応じて、混合工程において、添加剤及び溶媒の一方又は両方を更に添加してもよい。第２実施形態に係る光触媒コート剤の製造方法で用いられる第１光触媒、第２光触媒、その他の光触媒、バインダー、添加剤、及び溶媒は、各々、第１実施形態で述べた通りである。混合工程で用いられる混合装置としては、例えば、ホモジナイザーが挙げられる。以上、第２実施形態に係る光触媒コート剤の製造方法について説明した。
<Second embodiment: Method for producing photocatalyst coating agent>
The second embodiment of the present invention relates to a method for producing a photocatalyst coating agent. The method for producing a photocatalyst coating agent according to the second embodiment is a method for producing the photocatalyst coating agent according to the first embodiment. The method for producing a photocatalyst coating agent according to the second embodiment includes a step of mixing at least two types of photocatalysts and a binder (mixing step). If necessary, other photocatalysts may be further added in the mixing step. If necessary, one or both of the additive and the solvent may be further added in the mixing step. The first photocatalyst, the second photocatalyst, other photocatalysts, binders, additives, and solvents used in the method for producing a photocatalyst coating agent according to the second embodiment are as described in the first embodiment. Examples of the mixing device used in the mixing step include a homogenizer. The method for producing the photocatalyst coating agent according to the second embodiment has been described above.
＜第３実施形態：光触媒担持磁性体＞
本発明の第３実施形態は、光触媒担持磁性体に関する。第３実施形態に係る光触媒担持磁性体は、コアと、コアを被覆するコート層とを備える。
<Third Embodiment: Photocatalyst-Supported Magnetic Material>
The third embodiment of the present invention relates to a photocatalyst-supporting magnetic body. The photocatalyst-supporting magnetic body according to the third embodiment includes a core and a coat layer that covers the core.
（コート層）
コート層は、少なくとも２種の光触媒と、バインダーとを含有する。少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有する。少なくとも２種の光触媒は、その他の光触媒を更に含有してもよい。また、コート層は、必要に応じて、添加剤を更に含有してもよい。第３実施形態に係る光触媒担持磁性体のコート層に含有される第１光触媒、第２光触媒、その他の光触媒、バインダー、及び添加剤は、各々、第１実施形態で述べた通りである。
(Coat layer)
The coat layer contains at least two types of photocatalysts and a binder. At least two types of photocatalysts contain at least a first photocatalyst and a second photocatalyst. At least two kinds of photocatalysts may further contain other photocatalysts. Further, the coat layer may further contain an additive, if necessary. The first photocatalyst, the second photocatalyst, other photocatalysts, the binder, and the additives contained in the coat layer of the photocatalyst-supporting magnetic material according to the third embodiment are the same as those described in the first embodiment.
コート層の含有量は、１００重量部のコアに対して、１重量部以上２０重量部以下であることが好ましく、３重量部以上１０重量部以下であることがより好ましい。 The content of the coat layer is preferably from 1 to 20 parts by weight, more preferably from 3 to 10 parts by weight, based on 100 parts by weight of the core.
（コア）
コアは、磁性材料を含有する。コアが磁性材料を含有することで、次の利点が得られる。例えば、分解対象物を含有する水の中に光触媒担持磁性体を分散させる。光触媒を活性化する波長の光を照射して、水中の分解対象物を分解する。その際に、磁性材料を含有するコアを備える光触媒担持磁性体を、磁石を用いて移動又は回収することができる。
(core)
The core contains a magnetic material. When the core contains a magnetic material, the following advantages are obtained. For example, the photocatalyst-carrying magnetic material is dispersed in water containing the decomposition target. The object to be decomposed in water is decomposed by irradiating light having a wavelength to activate the photocatalyst. At this time, the photocatalyst-carrying magnetic body including the core containing the magnetic material can be moved or collected using a magnet.
磁性材料は、特に限定されない。磁性材料としては、例えば、酸化鉄（より具体的には、フェライト、及びマグネタイト等）、酸化鉄以外の金属酸化物、金属（より具体的には、鉄、コバルト、及びニッケル等）、及びこれらの合金が挙げられる。酸化鉄は、他の元素を更に含有していてもよい。酸化鉄に更に含有される元素としては、コバルト、ニッケル、アルミニウム、銅、鉛、マグネシウム、スズ、亜鉛、アンチモン、ベリリウム、ビスマス、カルシウム、マンガン、セレン、チタン、タングステン、バナジウム、バリウム、及びストロンチウムが挙げられる。他の元素を更に含有した酸化鉄としては、マンガン−フェライト、マンガン−亜鉛−フェライト、ニッケル−亜鉛−フェライト、銅−亜鉛−フェライト、バリウム−フェライト、及びストロンチウム−フェライトが挙げられる。磁性材料としては、酸化鉄が好ましく、フェライトがより好ましく、マンガン−フェライトが更に好ましい。 The magnetic material is not particularly limited. Examples of the magnetic material include iron oxides (more specifically, ferrite and magnetite, etc.), metal oxides other than iron oxides, metals (more specifically, iron, cobalt, nickel, etc.), and these. Alloys. Iron oxide may further contain other elements. Elements further contained in iron oxide include cobalt, nickel, aluminum, copper, lead, magnesium, tin, zinc, antimony, beryllium, bismuth, calcium, manganese, selenium, titanium, tungsten, vanadium, barium, and strontium. No. Iron oxides further containing other elements include manganese-ferrite, manganese-zinc-ferrite, nickel-zinc-ferrite, copper-zinc-ferrite, barium-ferrite, and strontium-ferrite. As the magnetic material, iron oxide is preferable, ferrite is more preferable, and manganese-ferrite is still more preferable.
コアの数平均粒子径は、５μｍ以上５０００μｍ以下であることが好ましく、５μｍ以上１００μｍ以下であることがより好ましい。コアの数平均粒子径がこのような範囲内であると、光触媒担持磁性体の製造に用いられる液にコアが分散し易くなり、コアの表面に均一なコート層が形成され易い。 The number average particle diameter of the core is preferably 5 μm or more and 5000 μm or less, more preferably 5 μm or more and 100 μm or less. When the number average particle diameter of the core is within such a range, the core is easily dispersed in the liquid used for producing the photocatalyst-supporting magnetic material, and a uniform coat layer is easily formed on the surface of the core.
（光触媒担持磁性体の製造方法）
次に、光触媒担持磁性体の製造方法の一例を説明する。光触媒担持磁性体は、例えば、第１実施形態に係る光触媒コート剤によりコアを被覆して、コート層を形成することにより製造される。コート層は、光触媒コート剤処理層である。
(Method for producing photocatalyst-supporting magnetic material)
Next, an example of a method for producing a photocatalyst-supporting magnetic material will be described. The photocatalyst-supporting magnetic material is manufactured, for example, by coating the core with the photocatalyst coating agent according to the first embodiment and forming a coat layer. The coat layer is a photocatalyst coat agent treatment layer.
光触媒コート剤によりコアを被覆する方法の一例を説明する。まず、液中でコアと光触媒コート剤とを混合した後、乾燥させる。これにより、コアの表面にコート層を形成して、光触媒担持磁性体を得る。得られた光触媒担持磁性体は、必要に応じて、洗浄、及び乾燥されてもよい。コアと光触媒コート剤とを混合するための液としては、例えば、光触媒コート剤に含有される溶媒と同じものを使用できる。コアとコート層との結着性を高めるために、液にバインダーを更に添加してもよい。更に添加されるバインダーとしては、例えば、光触媒コート剤に含有されるバインダーと同じものを使用できる。なお、コア及び光触媒コート剤のみで好適に混合できる場合には、コアと光触媒コート剤とを混合するための液を使用しなくてもよい。 An example of a method of coating a core with a photocatalyst coating agent will be described. First, the core and the photocatalyst coating agent are mixed in a liquid and then dried. Thus, a coat layer is formed on the surface of the core to obtain a photocatalyst-carrying magnetic material. The obtained photocatalyst-supporting magnetic material may be washed and dried as necessary. As a liquid for mixing the core and the photocatalyst coating agent, for example, the same solvent as that contained in the photocatalyst coating agent can be used. In order to enhance the binding between the core and the coat layer, a binder may be further added to the liquid. As the binder to be further added, for example, the same binder as that contained in the photocatalyst coating agent can be used. When the core and the photocatalyst coating agent can be suitably mixed only, it is not necessary to use a liquid for mixing the core and the photocatalyst coating agent.
光触媒コート剤によりコアを被覆する方法の別の例としては、光触媒コート剤にコアを浸漬させる浸漬法、コアに光触媒コート剤を噴霧するスプレー法、コアに光触媒コート剤を滴下する滴下法、流動エアによりコアを浮遊させた状態で光触媒コート剤を噴霧する流動床法、及びニーダーコーター中でコアと光触媒コート剤とを混合し溶媒を除去するニーダーコーター法が挙げられる。以上、第３実施形態に係る光触媒担持磁性体について説明した。 Other examples of the method of coating the core with the photocatalyst coating agent include a dipping method of dipping the core in the photocatalyst coating agent, a spray method of spraying the photocatalyst coating agent on the core, a dropping method of dropping the photocatalyst coating agent on the core, and a flow method. A fluidized bed method in which the photocatalyst coating agent is sprayed while the core is suspended by air, and a kneader coater method in which the core and the photocatalyst coating agent are mixed in a kneader coater and the solvent is removed. The photocatalyst-supporting magnetic body according to the third embodiment has been described above.
以下、実施例を示して本発明をより具体的に説明する。ただし、本発明は、実施例に限定されるものではない。なお、光触媒の平均一次粒子径は、次の方法で測定した。まず、比表面積・細孔分布測定装置（カンタクローム・インスツルメンツ社製「ＮＯＶＡ ４２００ｅ」）を用いて、単位質量あたりの光触媒の比表面積Ｓｍを測定した。次いで、測定した光触媒の比表面積Ｓｍから、下記式（１）に従って、光触媒の平均一次粒子径ｄを算出した。
平均一次粒子径ｄ＝６／（光触媒の比表面積Ｓｍ×光触媒の密度ρ）・・・（１）
Hereinafter, the present invention will be described more specifically with reference to examples. However, the present invention is not limited to the examples. The average primary particle diameter of the photocatalyst was measured by the following method. First, the specific surface area Sm of the photocatalyst per unit mass was measured using a specific surface area / pore distribution measuring device (“NOVA 4200e” manufactured by Kantachrome Instruments). Next, from the measured specific surface area Sm of the photocatalyst, the average primary particle diameter d of the photocatalyst was calculated according to the following equation (1).
Average primary particle diameter d = 6 / (specific surface area Sm of photocatalyst × density ρ of photocatalyst) (1)
［光触媒コート剤の作製］
光触媒コート剤（Ａ−１）〜（Ａ−７）及び（Ｂ−１）〜（Ｂ−３）を、以下の方法で作製した。
[Preparation of photocatalyst coating agent]
Photocatalyst coating agents (A-1) to (A-7) and (B-1) to (B-3) were produced by the following method.
＜光触媒コート剤（Ａ−１）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部にバインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）０．７５重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）２０重量部と、第２光触媒としての酸化チタン（日本アエロジル株式会社製「Ｐ−２５」、アナターゼ型酸化チタン、平均一次粒子径：２１ｎｍ）５重量部とを分散させた。これにより、光触媒コート剤（Ａ−１）を得た。
<Preparation of photocatalyst coating agent (A-1)>
Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, 100 parts by weight of 2-propanol and a binder (silicone resin, “KR-220LP” manufactured by Shin-Etsu Chemical Co., Ltd.) 0.75 Parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 6 nm) and 5 parts by weight of titanium oxide (“P-25” manufactured by Nippon Aerosil Co., Ltd., anatase type titanium oxide, average primary particle diameter: 21 nm) as a second photocatalyst Was dispersed. Thus, a photocatalyst coating agent (A-1) was obtained.
＜光触媒コート剤（Ａ−２）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）１５重量部と、第２光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０２」、アナターゼ型酸化チタン、平均一次粒子径：１５ｎｍ）７重量部とを分散させた。これにより、光触媒コート剤（Ａ−２）を得た。
<Preparation of photocatalyst coating agent (A-2)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 15 parts by weight of titanium oxide (average primary particle diameter: 6 nm) and 7 parts by weight of titanium oxide (“TKP-102” manufactured by Teica Corporation, anatase type titanium oxide, average primary particle diameter: 15 nm) as a second photocatalyst Dispersed. Thus, a photocatalyst coating agent (A-2) was obtained.
＜光触媒コート剤（Ａ−３）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡの条件で５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）２．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）２０重量部と、第２光触媒としての酸化チタン（テイカ株式会社製「ＡＭＴ−３０」、アナターゼ型酸化チタン、平均一次粒子径：３０ｎｍ）４重量部とを分散させた。これにより、光触媒コート剤（Ａ−３）を得た。
<Preparation of photocatalyst coating agent (A-3)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol under the conditions of 50 μA for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 2.00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 6 nm) and 4 parts by weight of titanium oxide (“AMT-30” manufactured by Teica Corporation, anatase type titanium oxide, average primary particle diameter: 30 nm) as a second photocatalyst Dispersed. Thus, a photocatalyst coating agent (A-3) was obtained.
＜光触媒コート剤（Ａ−４）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（日本アエロジル株式会社製「Ｐ−９０」、アナターゼ型酸化チタン、平均一次粒子径：１４ｎｍ）２０重量部と、第２光触媒としての酸化チタン（テイカ株式会社製「ＡＭＴ−３０」、アナターゼ型酸化チタン、平均一次粒子径：３０ｎｍ）５重量部とを分散させた。これにより、光触媒コート剤（Ａ−４）を得た。
<Preparation of photocatalyst coating agent (A-4)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“P-90” manufactured by Nippon Aerosil Co., Ltd., anatase) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 14 nm) and 5 parts by weight of titanium oxide (“AMT-30” manufactured by Teica Corporation, anatase type titanium oxide, average primary particle diameter: 30 nm) as a second photocatalyst Was dispersed. Thus, a photocatalyst coating agent (A-4) was obtained.
＜光触媒コート剤（Ａ−５）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０２」、アナターゼ型酸化チタン、平均一次粒子径：１５ｎｍ）２０重量部と、第２光触媒としての酸化チタン（テイカ株式会社製「ＡＭＴ−３０」、アナターゼ型酸化チタン、平均一次粒子径：３０ｎｍ）５重量部とを分散させた。これにより、光触媒コート剤（Ａ−５）を得た。
<Preparation of photocatalyst coating agent (A-5)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder liquid was added to titanium oxide (TKA-102 manufactured by Teica, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 15 nm) and 5 parts by weight of titanium oxide (“AMT-30” manufactured by Teica Corporation, anatase type titanium oxide, average primary particle diameter: 30 nm) as a second photocatalyst Dispersed. Thus, a photocatalyst coating agent (A-5) was obtained.
＜光触媒コート剤（Ａ−６）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）３．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）２０重量部と、第２光触媒としての酸化タングステンＷ−Ａ（白金担持酸化タングステン、平均一次粒子径：３０ｎｍ）８重量部とを分散させた。これにより、光触媒コート剤（Ａ−６）を得た。
<Preparation of photocatalyst coating agent (A-6)>
2. Using an ultrasonic homogenizer ("ULTRASONICGENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, 100 parts by weight of 2-propanol and a binder (silicone resin, “KR-220LP” manufactured by Shin-Etsu Chemical Co., Ltd.) 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 6 nm) and 8 parts by weight of tungsten oxide WA (platinum-supported tungsten oxide, average primary particle diameter: 30 nm) as a second photocatalyst were dispersed. Thus, a photocatalyst coating agent (A-6) was obtained.
なお、酸化タングステンＷ−Ａは、次の方法で作製した。水５０ｍＬに、酸化タングステン（ＷＯ3、株式会社高純度化学研究所製）５ｇを分散させて、分散液Ｉを得た。ビーズミル（日本コークス工業株式会社製「ＭＳＣ５０−ＺＺ」）に、分散液Ｉを投入した。ビーズミルを用いて、９０分間、分散液Ｉ中の酸化タングステンを粉砕した。次いで、遠心分離機（株式会社コクサン製「Ｈ−２０１Ｆ」）を用いて、３０００ｒｐｍの回転速度で５分間、分散液Ｉを遠心分離し、沈降した酸化タングステン粒子を取り出した。取り出した酸化タングステン粒子５ｇを、水５０ｍＬに分散させて、分散液ＩＩを得た。酸化タングステン粒子１００重量部に対して白金が０．５重量部となるように、分散液ＩＩにヘキサクロロ白金酸水溶液を添加した。添加された分散液ＩＩに、攪拌、濾過、水洗浄、及び乾燥を行うことにより、酸化タングステンＷ−Ａを得た。得られた酸化タングステンＷ−Ａは、白金を担持した酸化タングステンであり、平均一次粒子径は３０ｎｍであった。 The tungsten oxide WA was manufactured by the following method. In 50 mL of water, 5 g of tungsten oxide (WO 3 , manufactured by Kojundo Chemical Laboratory Co., Ltd.) was dispersed to obtain Dispersion I. Dispersion I was charged into a bead mill (“MSC50-ZZ” manufactured by Nippon Coke Industry Co., Ltd.). The tungsten oxide in the dispersion liquid I was ground for 90 minutes using a bead mill. Next, the dispersion liquid I was centrifuged at a rotation speed of 3000 rpm for 5 minutes using a centrifugal separator (“H-201F” manufactured by Kokusan Co., Ltd.), and sedimented tungsten oxide particles were taken out. 5 g of the removed tungsten oxide particles were dispersed in 50 mL of water to obtain Dispersion II. An aqueous solution of hexachloroplatinic acid was added to Dispersion II such that 0.5 parts by weight of platinum was added to 100 parts by weight of the tungsten oxide particles. The added dispersion liquid II was stirred, filtered, washed with water, and dried to obtain tungsten oxide WA. The obtained tungsten oxide WA was tungsten oxide carrying platinum and had an average primary particle diameter of 30 nm.
＜光触媒コート剤（Ａ−７）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）２０重量部と、第２光触媒としての酸化チタン（日本アエロジル株式会社製「Ｐ−２５」、アナターゼ型酸化チタン、平均一次粒子径：２１ｎｍ）５重量部と、その他の光触媒としての酸化チタン（テイカ株式会社製「ＡＭＴ−３０」、アナターゼ型酸化チタン、平均一次粒子径：３０ｎｍ）１重量部とを分散させた。これにより、光触媒コート剤（Ａ−７）を得た。
<Preparation of photocatalyst coating agent (A-7)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 6 nm) and 5 parts by weight of titanium oxide (“P-25” manufactured by Nippon Aerosil Co., Ltd., anatase type titanium oxide, average primary particle diameter: 21 nm) as a second photocatalyst And 1 part by weight of titanium oxide ("AMT-30" manufactured by Teica Corporation, anatase type titanium oxide, average primary particle diameter: 30 nm) as another photocatalyst. Thus, a photocatalyst coating agent (A-7) was obtained.
＜光触媒コート剤（Ｂ−１）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（日本アエロジル株式会社製「Ｐ−２５」、アナターゼ型酸化チタン、平均一次粒子径：２１ｎｍ）５重量部を分散させた。なお、第２光触媒は添加しなかった。これにより、光触媒コート剤（Ｂ−１）を得た。
<Preparation of photocatalyst coating agent (B-1)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added to titanium oxide (“P-25” manufactured by Nippon Aerosil Co., Ltd., anatase) as a first photocatalyst. (Titanium oxide, average primary particle size: 21 nm) in an amount of 5 parts by weight. Note that the second photocatalyst was not added. Thus, a photocatalyst coating agent (B-1) was obtained.
＜光触媒コート剤（Ｂ−２）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０１」、アナターゼ型酸化チタン、平均一次粒子径：６ｎｍ）２０重量部を分散させた。なお、第２光触媒は添加しなかった。これにより、光触媒コート剤（Ｂ−２）を得た。
<Preparation of photocatalyst coating agent (B-2)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder solution was added with titanium oxide (“TKP-101” manufactured by Teica Corporation, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 6 nm) were dispersed. Note that the second photocatalyst was not added. Thus, a photocatalyst coating agent (B-2) was obtained.
＜光触媒コート剤（Ｂ−３）の作製＞
超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１００重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）１．００重量部を分散させた。これにより、バインダー液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られたバインダー液に、第１光触媒としての酸化チタン（テイカ株式会社製「ＴＫＰ−１０２」、アナターゼ型酸化チタン、平均一次粒子径：１５ｎｍ）２０重量部と、第２光触媒としての酸化チタン（日本アエロジル株式会社製「Ｐ−２５」、アナターゼ型酸化チタン、平均一次粒子径：２１ｎｍ）５重量部とを分散させた。これにより、光触媒コート剤（Ｂ−３）を得た。
<Preparation of photocatalyst coating agent (B-3)>
A binder (silicone resin, "KR-220LP" manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 100 parts by weight of 2-propanol at 50 .mu.A for 5 minutes using an ultrasonic homogenizer ("ULTRASONIC GENATOR" manufactured by Nippon Seiki Seisaku-sho, Ltd.). 00 parts by weight were dispersed. Thus, a binder liquid was obtained. Using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.) at 50 μA for 5 minutes, the obtained binder liquid was added to titanium oxide (TKA-102 manufactured by Teica, anatase type) as a first photocatalyst. 20 parts by weight of titanium oxide (average primary particle diameter: 15 nm) and 5 parts by weight of titanium oxide (“P-25” manufactured by Nippon Aerosil Co., Ltd., anatase type titanium oxide, average primary particle diameter: 21 nm) as a second photocatalyst Was dispersed. Thus, a photocatalyst coating agent (B-3) was obtained.
［評価］
（評価用光触媒担持磁性体の作製）
光触媒コート剤（Ａ−１）〜（Ａ−７）及び（Ｂ−１）〜（Ｂ−３）の各々を用いて、評価用光触媒担持磁性体を作製した。詳しくは、超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、２−プロパノール１０重量部に、バインダー（シリコーン樹脂、信越化学工業株式会社製「ＫＲ−２２０ＬＰ」）２重量部を分散させた。これにより、バインダー液を得た。攪拌機（アズワン株式会社販売「オートセルマスターＣＭ−２００」）を用いて、回転数１００００ｒｐｍで１０分間、得られたバインダー液と、磁性材料含有コア（数平均粒子径：３５μｍ、Ｍｎ−フェライトのコア）１００重量部とを混合し、混合物を得た。攪拌機（アズワン株式会社販売「オートセルマスターＣＭ−２００」）を用いて、回転数１００００ｒｐｍで１０分間、得られた混合物と、光触媒コート剤２５重量部とを更に混合した。得られた混合物を４０℃で２４時間乾燥させることにより、２−プロパノールを除去した。これにより、評価用光触媒担持磁性体を得た。光触媒担持磁性体は、磁性材料含有コアと、コアを被覆するコート層とを備えていた。
[Evaluation]
(Production of magnetic material supporting photocatalyst for evaluation)
Using each of the photocatalyst coating agents (A-1) to (A-7) and (B-1) to (B-3), a photocatalyst-supporting magnetic material for evaluation was produced. Specifically, a binder (silicone resin, “KR-220LP” manufactured by Shin-Etsu Chemical Co., Ltd.) was added to 10 parts by weight of 2-propanol at 50 μA for 5 minutes using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.). ) 2 parts by weight were dispersed. Thus, a binder liquid was obtained. Using a stirrer ("Autocell Master CM-200" sold by AS ONE Corporation) at 10,000 rpm for 10 minutes, the obtained binder liquid and a magnetic material-containing core (number average particle diameter: 35 µm, Mn-ferrite core) ) 100 parts by weight to obtain a mixture. The obtained mixture and 25 parts by weight of a photocatalyst coating agent were further mixed for 10 minutes at 10,000 rpm using a stirrer (“Autocell Master CM-200” sold by AS ONE Corporation). The resulting mixture was dried at 40 ° C. for 24 hours to remove 2-propanol. As a result, a photocatalyst-supporting magnetic material for evaluation was obtained. The photocatalyst-supporting magnetic body had a magnetic material-containing core and a coat layer covering the core.
（付着強度の評価）
評価用光触媒担持磁性体に対して、付着強度の評価を行った。まず、蛍光Ｘ線分析装置を用いて、評価用光触媒担持磁性体に含有される光触媒の量（具体的には、チタン元素の量、及びタングステン元素の量）を測定した。測定された光触媒の量を、超音波処理前の含有量とした。次いで、純水に評価用光触媒担持磁性体を分散させて、分散液を得た。超音波ホモジナイザー（株式会社日本精機製作所製「ＵＬＴＲＡＳＯＮＩＣＧＥＮＥＲＡＴＯＲ」）を用いて、５０μＡで５分間、得られた分散液に超音波処理を行った。次いで、分散液を４０℃で２４時間乾燥させて、超音波処理後の光触媒担持磁性体を得た。蛍光Ｘ線分析装置を用いて、超音波処理後の光触媒担持磁性体に含有される光触媒の量（具体的には、チタン元素の量、及びタングステン元素の量）を測定した。測定された光触媒の量を、超音波処理後の含有量とした。式「光触媒残存率＝１００×（超音波処理後の含有量）／（超音波処理前の含有量）」に従って、光触媒残存率（単位：％）を算出した。そして、光触媒残存率から、下記基準に従って、コアに対する光触媒の付着強度を評価した。評価結果を、表１に示す。
評価Ａ：光触媒残存率が８０％以上である。
評価Ｂ：光触媒残存率が７０％以上８０％未満である。
評価Ｃ：光触媒残存率が７０％未満である。
(Evaluation of adhesion strength)
The adhesion strength of the photocatalyst-supporting magnetic material for evaluation was evaluated. First, the amount of the photocatalyst (specifically, the amount of the titanium element and the amount of the tungsten element) contained in the evaluation photocatalyst-supporting magnetic material was measured using an X-ray fluorescence analyzer. The measured amount of the photocatalyst was defined as the content before the ultrasonic treatment. Next, the photocatalyst-supporting magnetic material for evaluation was dispersed in pure water to obtain a dispersion. The obtained dispersion was subjected to ultrasonic treatment at 50 μA for 5 minutes using an ultrasonic homogenizer (“ULTRASONIC GENATOR” manufactured by Nippon Seiki Seisaku-sho, Ltd.). Next, the dispersion was dried at 40 ° C. for 24 hours to obtain a photocatalyst-supporting magnetic material after ultrasonic treatment. Using an X-ray fluorescence spectrometer, the amount of the photocatalyst (specifically, the amount of the titanium element and the amount of the tungsten element) contained in the photocatalyst-supporting magnetic material after the ultrasonic treatment was measured. The measured amount of the photocatalyst was defined as the content after the ultrasonic treatment. The photocatalyst remaining rate (unit:%) was calculated according to the formula “photocatalyst remaining rate = 100 × (content after ultrasonic treatment) / (content before ultrasonic treatment)”. Then, the adhesion strength of the photocatalyst to the core was evaluated from the photocatalyst remaining rate according to the following criteria. Table 1 shows the evaluation results.
Evaluation A: The residual ratio of the photocatalyst is 80% or more.
Evaluation B: The residual ratio of the photocatalyst is 70% or more and less than 80%.
Evaluation C: The residual ratio of the photocatalyst is less than 70%.
（メチレンブルー分解活性の評価）
光触媒性能として、メチレンブルー分解活性を評価した。ガラス製容器に、評価用光触媒担持磁性体１ｇと、メチレンブルー三水和物水溶液（濃度：２０μｍｏｌ／Ｌ）３０ｍＬとを入れて、評価液を作製した。次いで、紫外線ランプ（アズワン株式会社販売「ＬＵＶ−１６」）を、評価液の液面から５０ｍｍ離れた位置に設置した。０．１Ｌ／分の量の空気を評価液に送り込みながら、紫外線ランプを用いて３６５ｎｍの紫外線を、２４時間、評価液に照射した。紫外線照射後の評価液に対して、分光光度計（株式会社島津製作所製「ＵＶ−２４５０」）を用いて、メチレンブルーに由来する波長６６３ｎｍの光の透過率を測定した。測定された波長６６３ｎｍの光の透過率から、下記基準に従って、メチレンブルー分解活性を評価した。評価結果を、表１に示す。なお、波長６６３ｎｍの光の透過率が高い程、メチレンブルーが分解されていることを示す。
評価Ａ：透過率が７０％以上１００％以下である。
評価Ｂ：透過率が２０％超７０％未満である。
評価Ｃ：透過率が０％以上２０％以下である。
(Evaluation of methylene blue decomposition activity)
As photocatalytic performance, methylene blue decomposition activity was evaluated. 1 g of the photocatalyst-supporting magnetic material for evaluation and 30 mL of an aqueous methylene blue trihydrate solution (concentration: 20 μmol / L) were placed in a glass container to prepare an evaluation solution. Next, an ultraviolet lamp ("LUV-16" sold by AS ONE Corporation) was installed at a position 50 mm away from the liquid surface of the evaluation solution. While sending 0.1 L / min of air into the evaluation liquid, the evaluation liquid was irradiated with ultraviolet rays of 365 nm using an ultraviolet lamp for 24 hours. The transmittance of light having a wavelength of 663 nm derived from methylene blue was measured using a spectrophotometer (“UV-2450” manufactured by Shimadzu Corporation) for the evaluation liquid after the ultraviolet irradiation. From the measured transmittance of light having a wavelength of 663 nm, methylene blue decomposition activity was evaluated according to the following criteria. Table 1 shows the evaluation results. The higher the transmittance of light having a wavelength of 663 nm, the more methylene blue is decomposed.
Evaluation A: The transmittance is 70% or more and 100% or less.
Evaluation B: The transmittance is more than 20% and less than 70%.
Evaluation C: transmittance is 0% or more and 20% or less.
なお、表１中の各用語は、次の意味である。「部」は「重量部」を示す。「−」は該当する成分を含有していないことを示す。「径」は「平均一次粒子径」を示す。「径比率」の欄の「第２／第１」は、第１光触媒の平均一次粒子径に対する、第２光触媒の平均一次粒子径の比率を示す。「Ｖ１／Ｖ２」は、第２光触媒の体積Ｖ２に対する、第１光触媒の体積Ｖ１の比率を示す。「ＶＣ／ＶＢ」は、バインダーの体積ＶＢに対する、少なくとも２種の光触媒の総体積ＶＣの比率を示す。 In addition, each term in Table 1 has the following meaning. “Parts” indicates “parts by weight”. "-" Indicates that the corresponding component is not contained. “Diameter” indicates “average primary particle diameter”. “Second / first” in the column of “diameter ratio” indicates the ratio of the average primary particle diameter of the second photocatalyst to the average primary particle diameter of the first photocatalyst. “V1 / V2” indicates the ratio of the volume V1 of the first photocatalyst to the volume V2 of the second photocatalyst. “VC / VB” indicates the ratio of the total volume VC of at least two photocatalysts to the volume VB of the binder.
表１に示す各材料の主成分及び密度を、表２に示す。各材料の主成分とは、対象となる材料において、９９重量％以上を占める成分である。第１光触媒の体積Ｖ１は、式「Ｖ１＝（表１に示す第１光触媒の量）／４．２３」から算出した。第２光触媒の主成分が酸化チタンである場合、第２光触媒の体積Ｖ２は、式「Ｖ２＝（表１に示す第２光触媒の量）／４．２３」から算出した。第２光触媒の主成分が酸化タングステンである場合、第２光触媒の体積Ｖ２は、式「Ｖ２＝（表１に示す第２光触媒の量）／７．１６」から算出した。その他の光触媒の体積Ｖ３は、式「Ｖ３＝（表１に示すその他の光触媒の量）／４．２３」から算出した。その他の光触媒を含有しない場合、少なくとも２種の光触媒の総体積ＶＣは、式「ＶＣ＝Ｖ１＋Ｖ２」から算出した。その他の光触媒を含有する場合、少なくとも２種の光触媒の総体積ＶＣは、式「ＶＣ＝Ｖ１＋Ｖ２＋Ｖ３」から算出した。バインダーの体積ＶＢは、式「ＶＢ＝（表１に示すバインダーの量）／１．２０」から算出した。なお、光触媒コート剤（Ａ−７）において、少なくとも２種の光触媒の総体積ＶＣに対する、第１光触媒の体積Ｖ１と第２光触媒の体積Ｖ２との合計含有率は、９６体積％であった。 Table 2 shows the main components and densities of each material shown in Table 1. The main component of each material is a component that accounts for 99% by weight or more of the target material. The volume V1 of the first photocatalyst was calculated from the equation “V1 = (amount of the first photocatalyst shown in Table 1) /4.23”. When the main component of the second photocatalyst is titanium oxide, the volume V2 of the second photocatalyst was calculated from the equation “V2 = (amount of the second photocatalyst shown in Table 1) /4.23”. When the main component of the second photocatalyst is tungsten oxide, the volume V2 of the second photocatalyst was calculated from the equation “V2 = (amount of the second photocatalyst shown in Table 1) /7.16”. The volume V3 of the other photocatalyst was calculated from the equation “V3 = (amount of other photocatalyst shown in Table 1) /4.23”. When no other photocatalyst was contained, the total volume VC of at least two types of photocatalysts was calculated from the equation “VC = V1 + V2”. When other photocatalysts are contained, the total volume VC of at least two types of photocatalysts was calculated from the equation “VC = V1 + V2 + V3”. The volume VB of the binder was calculated from the equation “VB = (amount of binder shown in Table 1) /1.20”. In the photocatalyst coating agent (A-7), the total content of the volume V1 of the first photocatalyst and the volume V2 of the second photocatalyst with respect to the total volume VC of at least two photocatalysts was 96% by volume.
表１に示すように、光触媒コート剤（Ａ−１）〜（Ａ−７）の各々は、少なくとも２種の光触媒と、バインダーとを含有していた。具体的には、光触媒コート剤（Ａ−１）〜（Ａ−６）の各々は、２種の光触媒（第１光触媒及び第２光触媒）とバインダーとを含有していた。光触媒コート剤（Ａ−７）は、３種の光触媒（第１光触媒、第２光触媒、及びその他の光触媒）とバインダーとを含有していた。第２光触媒の平均一次粒子径は、第１光触媒の平均一次粒子径の２．０倍以上であった。そのため、表１に示すように、光触媒コート剤（Ａ−１）〜（Ａ−７）の各々を用いて作製された光触媒担持磁性体は、付着強度がＡ評価であり、光触媒の脱離を抑制できた。また、光触媒コート剤（Ａ−１）〜（Ａ−７）の各々を用いて作製された光触媒担持磁性体は、メチレンブルー分解活性がＡ評価であり、光触媒性能が良好であった。 As shown in Table 1, each of the photocatalyst coating agents (A-1) to (A-7) contained at least two types of photocatalysts and a binder. Specifically, each of the photocatalyst coating agents (A-1) to (A-6) contained two types of photocatalysts (a first photocatalyst and a second photocatalyst) and a binder. The photocatalyst coating agent (A-7) contained three types of photocatalysts (a first photocatalyst, a second photocatalyst, and another photocatalyst) and a binder. The average primary particle diameter of the second photocatalyst was at least 2.0 times the average primary particle diameter of the first photocatalyst. Therefore, as shown in Table 1, the photocatalyst-carrying magnetic material produced using each of the photocatalyst coating agents (A-1) to (A-7) has an adhesion rating of A, indicating that the photocatalyst is desorbed. Could be suppressed. In addition, the photocatalyst-supporting magnetic material produced using each of the photocatalyst coating agents (A-1) to (A-7) had an A rating of methylene blue decomposition activity and good photocatalytic performance.
一方、表１に示すように、光触媒コート剤（Ｂ−１）〜（Ｂ−２）の各々は、第２触媒を含有していなかった。光触媒コート剤（Ｂ−３）においては、第２光触媒の平均一次粒子径が第１光触媒の平均一次粒子径の２．０倍以上ではなかった。そのため、表１に示すように、光触媒コート剤（Ｂ−１）及び（Ｂ−３）の各々を用いて作製された光触媒担持磁性体は、付着強度がＣ評価であり、光触媒の脱離が抑制できていなかった。また、光触媒コート剤（Ｂ−２）及び（Ｂ−３）の各々を用いて作製された光触媒担持磁性体は、メチレンブルー分解活性がＣ評価であり、光触媒性能が不良であった。 On the other hand, as shown in Table 1, each of the photocatalyst coating agents (B-1) to (B-2) did not contain the second catalyst. In the photocatalyst coating agent (B-3), the average primary particle diameter of the second photocatalyst was not more than 2.0 times the average primary particle diameter of the first photocatalyst. Therefore, as shown in Table 1, the photocatalyst-carrying magnetic material produced using each of the photocatalyst coating agents (B-1) and (B-3) has an adhesion strength of C evaluation, and the desorption of the photocatalyst is low. Could not be suppressed. Further, the photocatalyst-supporting magnetic material produced using each of the photocatalyst coating agents (B-2) and (B-3) had a methylene blue decomposition activity of C evaluation and poor photocatalytic performance.
以上のことから、本発明に包含される光触媒コート剤（Ａ−１）〜（Ａ−７）は、光触媒コート剤（Ｂ−１）〜（Ｂ−３）と比較して、光触媒の脱離を抑制しつつ、光触媒性能を向上できることが示された。また、本発明の製造方法により製造された光触媒コート剤は、光触媒の脱離を抑制しつつ、光触媒性能を向上できることが示された。また、本発明の光触媒コート剤を用いて製造された光触媒担持磁性体は、光触媒の脱離を抑制しつつ、光触媒性能を向上できることが示された。 From the above, the photocatalyst coating agents (A-1) to (A-7) included in the present invention have a higher desorption of photocatalyst than the photocatalyst coating agents (B-1) to (B-3). It was shown that the photocatalytic performance can be improved while suppressing the occurrence of photocatalysis. Moreover, it was shown that the photocatalyst coating agent produced by the production method of the present invention can improve the photocatalytic performance while suppressing the desorption of the photocatalyst. In addition, it was shown that the photocatalyst-supporting magnetic material manufactured using the photocatalyst coating agent of the present invention can improve the photocatalytic performance while suppressing the desorption of the photocatalyst.
本発明の光触媒コート剤、本発明の製造方法により製造された光触媒体コート剤、及び本発明の光触媒担持磁性体は、水を浄化するための光触媒製品に利用できる。 The photocatalyst coating agent of the present invention, the photocatalyst coating agent manufactured by the manufacturing method of the present invention, and the photocatalyst-supporting magnetic material of the present invention can be used for a photocatalyst product for purifying water.
Claims (7)
前記少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有し、
前記第１光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が最も小さく、
前記第２光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が２番目に小さく、
前記第２光触媒の平均一次粒子径は、前記第１光触媒の平均一次粒子径の２．０倍以上である、光触媒コート剤。 Containing at least two kinds of photocatalysts and a binder,
The at least two types of photocatalysts include at least a first photocatalyst and a second photocatalyst,
The first photocatalyst has the smallest average primary particle diameter among the at least two types of photocatalysts,
The second photocatalyst has an average primary particle diameter of the second smallest among the at least two types of photocatalysts,
The photocatalyst coating agent, wherein the average primary particle diameter of the second photocatalyst is 2.0 times or more the average primary particle diameter of the first photocatalyst.
前記第２光触媒の平均一次粒子径は、１５ｎｍ以上３０ｎｍ以下である、請求項１に記載の光触媒コート剤。 The average primary particle diameter of the first photocatalyst is 5 nm or more and 15 nm or less,
The photocatalyst coating agent according to claim 1, wherein the average primary particle diameter of the second photocatalyst is 15 nm or more and 30 nm or less.
前記第２光触媒は、酸化チタン又は酸化タングステンを含有する、請求項１又は２に記載の光触媒コート剤。 The first photocatalyst contains titanium oxide or tungsten oxide,
The photocatalyst coating agent according to claim 1, wherein the second photocatalyst contains titanium oxide or tungsten oxide.
前記コート層は、少なくとも２種の光触媒と、バインダーとを含有し、
前記少なくとも２種の光触媒は、第１光触媒と、第２光触媒とを少なくとも含有し、
前記第１光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が最も小さく、
前記第２光触媒は、前記少なくとも２種の光触媒のうちで平均一次粒子径が２番目に小さく、
前記第２光触媒の平均一次粒子径は、前記第１光触媒の平均一次粒子径の２．０倍以上である、光触媒担持磁性体。 A core containing a magnetic material, comprising a coat layer covering the core,
The coat layer contains at least two kinds of photocatalysts and a binder,
The at least two types of photocatalysts include at least a first photocatalyst and a second photocatalyst,
The first photocatalyst has the smallest average primary particle diameter among the at least two types of photocatalysts,
The second photocatalyst has an average primary particle diameter of the second smallest among the at least two types of photocatalysts,
The photocatalyst-supporting magnetic material, wherein the average primary particle diameter of the second photocatalyst is 2.0 times or more the average primary particle diameter of the first photocatalyst.
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