JPH11347420A - Member having photocatalytic function - Google Patents
Member having photocatalytic functionInfo
- Publication number
- JPH11347420A JPH11347420A JP11014879A JP1487999A JPH11347420A JP H11347420 A JPH11347420 A JP H11347420A JP 11014879 A JP11014879 A JP 11014879A JP 1487999 A JP1487999 A JP 1487999A JP H11347420 A JPH11347420 A JP H11347420A
- Authority
- JP
- Japan
- Prior art keywords
- particles
- layer
- photocatalyst
- tio
- glaze layer
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 18
- 239000002245 particle Substances 0.000 claims abstract description 49
- 239000011941 photocatalyst Substances 0.000 claims abstract description 22
- 239000011230 binding agent Substances 0.000 claims abstract description 12
- 239000000463 material Substances 0.000 claims abstract description 8
- 239000010419 fine particle Substances 0.000 claims abstract description 5
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 24
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 abstract description 21
- 239000000758 substrate Substances 0.000 abstract description 3
- 238000005507 spraying Methods 0.000 abstract description 2
- 238000010438 heat treatment Methods 0.000 description 6
- 230000001877 deodorizing effect Effects 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- LSDPWZHWYPCBBB-UHFFFAOYSA-N Methanethiol Chemical compound SC LSDPWZHWYPCBBB-UHFFFAOYSA-N 0.000 description 2
- 230000000844 anti-bacterial effect Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 238000004332 deodorization Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000003232 water-soluble binding agent Substances 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000003373 anti-fouling effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- TUJKJAMUKRIRHC-UHFFFAOYSA-N hydroxyl Chemical compound [OH] TUJKJAMUKRIRHC-UHFFFAOYSA-N 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- -1 pottery Substances 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Landscapes
- Finishing Walls (AREA)
- Panels For Use In Building Construction (AREA)
- Building Environments (AREA)
- Disinfection, Sterilisation Or Deodorisation Of Air (AREA)
- Application Of Or Painting With Fluid Materials (AREA)
- Laminated Bodies (AREA)
- Catalysts (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、脱臭、抗菌、防汚
等の光触媒機能を有する部材に関する。The present invention relates to a member having a photocatalytic function such as deodorization, antibacterial and antifouling.
【０００２】[0002]
【従来の技術】紫外線の照射を受けて脱臭反応を進行さ
せる光触媒としてアナターゼ型のＴiＯ2が知られてい
る。そして、光触媒粒子をバインダに混練した原料を居
住空間の壁面を構成する部材の表面に塗布した後に焼成
することで、居住空間の壁面に脱臭壁機能をもたせるよ
うにした提案を本出願人は先に行なっている。2. Description of the Related Art Anatase-type TiO 2 is known as a photocatalyst for promoting a deodorizing reaction upon irradiation with ultraviolet rays. The applicant of the present invention has proposed a proposal in which the raw material obtained by kneading the photocatalyst particles into a binder is applied to the surface of a member constituting the wall surface of the living space and then fired so that the wall surface of the living space has a deodorizing wall function. I have done it.
【０００３】[0003]
【発明が解決しようとする課題】図１０は脱臭壁の一部
部分拡大断面図であり、壁材１００の表面にはバインダ
層１０１が形成され、このバインダ層１０１内に光触媒
粒子１０２が保持されている。FIG. 10 is a partially enlarged cross-sectional view of a deodorizing wall. A binder layer 101 is formed on the surface of a wall material 100, and photocatalyst particles 102 are held in the binder layer 101. ing.
【０００４】従来にあってはバインダ層１０１内に光触
媒粒子１０２が完全に埋まっているため、脱臭壁全体と
しては、全ての光触媒粒子１０２に直接紫外線が照射さ
れず、また、光触媒粒子１０２の平均粒径も比較的大き
く、十分な触媒作用を発揮することができない。In the prior art, since the photocatalyst particles 102 are completely buried in the binder layer 101, the entire deodorizing wall does not directly irradiate all the photocatalyst particles 102 with ultraviolet rays. The particle size is relatively large, and a sufficient catalytic action cannot be exhibited.
【０００５】[0005]
【課題を解決するための手段】上記課題を解決すべく本
発明に係る光触媒機能を有する部材は、基材表面にバイ
ンダ層を介して光触媒粒子の層を設けるとともに、光触
媒粒子としては平均粒径が１００Å以上５００Å未満の
ＴiＯ2微粒子を用いるようにした。Means for Solving the Problems To solve the above problems, a member having a photocatalytic function according to the present invention is provided with a layer of photocatalyst particles on a surface of a base material via a binder layer, and the photocatalyst particles have an average particle diameter. TiO 2 fine particles having a thickness of 100 ° or more and less than 500 ° are used.
【０００６】このように、バインダ層を介して光触媒粒
子の層を保持することで、光触媒粒子に十分に紫外線を
照射することができ、更に光触媒粒子としてＴiＯ2微粒
子を用い、且つその平均粒径を１００Å以上５００Å未
満とすることで、光触媒作用が更に向上する。As described above, by holding the layer of the photocatalyst particles through the binder layer, the photocatalyst particles can be sufficiently irradiated with ultraviolet rays. Further, TiO 2 fine particles are used as the photocatalyst particles, and the average particle size thereof is used. Is set to 100 ° or more and less than 500 °, the photocatalytic action is further improved.
【０００７】[0007]
【発明の実施の形態】以下に本発明の実施の形態を添付
図面に基づいて説明する。ここで、図１は本発明に係る
セラミック、陶器、ガラス、金属等の基材表面に光触媒
層を形成した光触媒機能を有する部材の製造方法を工程
順に示した図である。Embodiments of the present invention will be described below with reference to the accompanying drawings. Here, FIG. 1 is a diagram showing a method of manufacturing a member having a photocatalytic function in which a photocatalytic layer is formed on the surface of a base material such as ceramic, pottery, glass, and metal according to the present invention in the order of steps.
【０００８】本発明方法にあっては先ず図１（ａ）に示
すように、壁面、床面或いは天井面を構成する板状部材
としてのタイル素地１の表面に光触媒粒子による光触媒
機能によって分解されにくい材料である釉薬層２を塗布
し、次いで図１（ｂ）に示すように釉薬層２の表面にス
プレー等を用いて光触媒粒子としてのアナターゼ型Ｔi
Ｏ2粒子３をゾル状にして吹き付け、次いで図１（ｃ）
に示すように釉薬層２を加熱溶融せしめた後、冷却して
固化せしめる。尚、ＴiＯ2ゾルにはＣuやＡg等を添加し
て殺菌効果をもたせるようにしてもよい。添加の方法と
しては例えばＣuＳＯ4をＮＨ3溶液でｐＨ１１程度に調
整したＴiＯ2ゾルに添加する。In the method of the present invention, first, as shown in FIG. 1 (a), the surface of a tile substrate 1 as a plate-like member constituting a wall surface, a floor surface or a ceiling surface is decomposed by a photocatalytic function of photocatalytic particles. A glaze layer 2, which is a difficult material, is applied, and then, as shown in FIG. 1B, the surface of the glaze layer 2 is sprayed or the like to form anatase Ti as photocatalyst particles.
The O2 particles 3 are sprayed in the form of a sol, and then FIG.
After the glaze layer 2 is heated and melted as shown in FIG. 3, it is cooled and solidified. Incidentally, Cu, Ag or the like may be added to the TiO 2 sol to have a bactericidal effect. As an addition method, for example, CuSO 4 is added to a TiO 2 sol adjusted to about pH 11 with an NH 3 solution.
【０００９】そして、ＴiＯ2ゾルを前記したように釉薬
層２の表面に吹き付けた後に、３００〜９００℃の範囲
で加熱することで、釉薬層２上にアナターゼ型ＴiＯ2粒
子３からなる光触媒層が形成される。After the TiO 2 sol is sprayed on the surface of the glaze layer 2 as described above, the sol is heated at a temperature in the range of 300 to 900 ° C. so that the photocatalytic layer composed of the anatase type TiO 2 particles 3 is formed on the glaze layer 2. Is formed.
【００１０】また、紫外線がＴiＯ2粒子３に照射される
と、吸着水と光触媒の正孔とが反応して水酸基ラジカル
（ＯＨ*）を生成し、この水酸基ラジカルとアンモニア
とが下式（１）のように反応し、また水酸基ラジカルと
メチルメルカプタンとが下式（２）のように反応して脱
臭すると考えられる。When the TiO 2 particles 3 are irradiated with ultraviolet rays, the adsorbed water reacts with the holes of the photocatalyst to generate hydroxyl radicals (OH * ), and the hydroxyl radicals and ammonia are converted into the following formula (1). ), And the hydroxyl radical and methyl mercaptan react as shown in the following formula (2) to deodorize.
【００１１】 ＮＨ3＋３ＯＨ*→1/2Ｎ2＋３Ｈ2Ｏ・・・・・・・・・・・（１） ＣＨ3ＳＨ＋ＯＨ*→ＣＨ3Ｓ＋Ｈ2Ｏ ２ＣＨ3Ｓ＋２ＯＨ*＋５Ｏ2→２ＣＯ2＋４Ｈ2Ｏ＋２ＳＯ2 ・・（２）NH 3 + 3OH * → 1 / 2N 2 + 3H 2 O (1) CH 3 SH + OH * → CH 3 S + H 2 O 2 CH 3 S + 2OH * + 5O 2 → 2CO 2 + 4H 2 O + 2SO 2・ ・ (2)
【００１２】図２乃至図６は別実施例を示す図であり、
図２に示す実施例にあっては、釉薬層２の表面に印刷に
よってインク層４を形成し、このインク層４の表面にＴ
iＯ2粒子３をその一部が露出するように吹き付け、その
後は前記と同様に加熱し冷却する。FIGS. 2 to 6 show another embodiment.
In the embodiment shown in FIG. 2, an ink layer 4 is formed on the surface of the glaze layer 2 by printing, and T
The TiO 2 particles 3 are sprayed so that a part thereof is exposed, and then heated and cooled in the same manner as described above.
【００１３】図３に示す実施例は、離型紙５の表面に水
溶性バインダ６を介して釉薬層２を形成し、この釉薬層
２の表面にバインダ層７を形成し、このバインダ層７の
表面にＴiＯ2粒子３を吹き付けてシートＳを得る。そし
て、離型紙５を剥離してシートＳをタイル素地１表面に
貼着し、この後前記と同様にして加熱し冷却する。この
ように光触媒機能を有するシートＳを別体として用意し
ておけば、既存のタイル等にも脱臭等の光触媒機能を簡
単に付与することができる。In the embodiment shown in FIG. 3, a glaze layer 2 is formed on the surface of a release paper 5 via a water-soluble binder 6, and a binder layer 7 is formed on the surface of the glaze layer 2. The sheet S is obtained by spraying TiO2 particles 3 on the surface. Then, the release paper 5 is peeled off, the sheet S is adhered to the surface of the tile substrate 1, and then heated and cooled in the same manner as described above. If the sheet S having the photocatalytic function is prepared separately as described above, a photocatalytic function such as deodorization can be easily imparted to existing tiles and the like.
【００１４】図４に示す実施例は、インク層４の表面に
部分的にＴiＯ2粒子３を付着せしめて絵柄とし、装飾効
果を高めるようにしたものであり、ＴiＯ2粒子３を釉薬
層２の表面に形成してもよい。[0014] embodiment shown in FIG. 4, the pattern partially by adhering the TiO 2 particles 3 on the surface of the ink layer 4, which was set to increase the decorative effect, the glaze layer 2 of TiO 2 particles 3 May be formed on the surface.
【００１５】図５（ａ）、（ｂ）に示す実施例は、タイ
ル素地１に滑り止め等の目的で形成した凹部に釉薬層２
を介してＴiＯ2粒子３を保持したものである。このよう
に凹部を形成した場合には凹部に汚れが入り込み汚れが
落ちにくいが、ＴiＯ2粒子３を保持することで、凹部内
の汚れが分解されるので汚れを簡単に除去できる。In the embodiment shown in FIGS. 5A and 5B, a glaze layer 2 is formed in a recess formed in a tile base 1 for the purpose of preventing slippage.
And the TiO 2 particles 3 are held through the intermediary. When the concave portion is formed in this way, the dirt enters the concave portion and the dirt is difficult to remove. However, the dirt in the concave portion is decomposed by holding the TiO 2 particles 3, so that the dirt can be easily removed.
【００１６】図６に示す実施例は、釉薬層２とＴiＯ2粒
子３との間に蒸着アルミニウム粉末やマグネシア等から
なる紫外線反射層８を介在させたものであり、このよう
な構成とすることで、一旦ＴiＯ2粒子３の層を透過した
紫外線を再びＴiＯ2粒子３に照射することができ、触媒
作用が向上する。In the embodiment shown in FIG. 6, an ultraviolet reflecting layer 8 made of vapor-deposited aluminum powder or magnesia is interposed between the glaze layer 2 and the TiO 2 particles 3. in, once the ultraviolet rays transmitted through a layer of TiO 2 particles 3 again can be irradiated to the TiO 2 particles 3, catalysis can be improved.
【００１７】図７はＣＨ3ＳＨ濃度と経過時間との関係
を熱処理（焼成）温度毎に試験した結果を示すグラフで
あり、グラフ中τ1/10は濃度が１／１０になるまでの時
間を示し、点線は紫外線を照射しない場合を示す。また
アナターゼ型ＴiＯ2粒子は平均粒径１００Åのものを用
いた。FIG. 7 is a graph showing the test results of the relationship between the CH 3 SH concentration and the elapsed time for each heat treatment (firing) temperature. In the graph, τ 1/10 represents the time until the concentration becomes 1/10. The dotted line shows the case where no ultraviolet light is irradiated. The anatase type TiO 2 particles having an average particle diameter of 100 ° were used.
【００１８】また、図８は熱処理温度と３０分後の臭気
除去率との関係を実験した結果を示すグラフであり、図
９は平均粒径５００Åのアナターゼ型ＴiＯ2を用いた場
合のＣＨ3ＳＨ濃度と経過時間との関係（熱処理温度；
７００℃）を示すグラフである。FIG. 8 is a graph showing the results of an experiment on the relationship between the heat treatment temperature and the odor removal rate after 30 minutes. FIG. 9 shows CH 3 when anatase type TiO 2 having an average particle size of 500 ° was used. Relationship between SH concentration and elapsed time (heat treatment temperature;
700 ° C.).
【００１９】これら図７、図８及び図９から以下のこと
が言える。第１に紫外線の存在下においてアナターゼ型
ＴiＯ2は触媒作用を発揮する。第２に触媒作用は７００
℃付近で最大値を示し、３０分後の臭気除去率を５０％
以上とするには３００℃以上で９００℃未満とする必要
がある。これは熱処理温度が３００℃未満では活性が生
じにくく９００℃を超えるとＴiＯ2の構造がアナターゼ
からルチルに変化するからと考えられる。第３に触媒作
用は、粒径のある程度小さな、具体的には平均粒径１０
０Å〜５００Åのアナターゼがよいことが分る。The following can be said from FIG. 7, FIG. 8 and FIG. First, in the presence of ultraviolet light, anatase-type TiO 2 exerts a catalytic action. Second, the catalysis is 700
The maximum value is shown around ℃, and the odor removal rate after 30 minutes is 50%.
In order to achieve the above, it is necessary to set the temperature to 300 ° C. or higher and lower than 900 ° C. This is presumably because the activity is unlikely to occur when the heat treatment temperature is lower than 300 ° C, and the structure of TiO 2 changes from anatase to rutile when the heat treatment temperature exceeds 900 ° C. Third, the catalytic action is that the particle size is somewhat small, specifically, the average particle size is 10%.
It can be seen that 0 to 500 degrees anatase is good.
【００２０】[0020]
【発明の効果】以上に説明した如く本発明によれば、基
材表面にバインダ層を介して光触媒粒子の層を設けると
ともに、光触媒粒子としては平均粒径が１００Å以上５
００Å未満のＴiＯ2微粒子を用いるようにしたので、光
触媒作用が向上する。As described above, according to the present invention, a layer of photocatalyst particles is provided on the surface of a base material via a binder layer, and the average particle size of the photocatalyst particles is 100 ° or more.
Since the TiO2 fine particles of less than 00 ° are used, the photocatalytic action is improved.
【図１】本発明に係る光触媒機能を有する部材の製造方
法を工程順に示した図。FIG. 1 is a view showing a method of manufacturing a member having a photocatalytic function according to the present invention in the order of steps.
【図２】別実施例を示す部材の断面図。FIG. 2 is a sectional view of a member showing another embodiment.
【図３】別実施例を示す部材の断面図。FIG. 3 is a sectional view of a member showing another embodiment.
【図４】別実施例を示す部材の断面図。FIG. 4 is a sectional view of a member showing another embodiment.
【図５】別実施例を示す部材の断面図。FIG. 5 is a sectional view of a member showing another embodiment.
【図６】別実施例を示す部材の断面図。FIG. 6 is a sectional view of a member showing another embodiment.
【図７】平均粒径１００Åのアナターゼ型ＴiＯ2を用い
た場合の経過時間とＣＨ3ＳＨ濃度との関係を示すグラ
フ。FIG. 7 is a graph showing the relationship between elapsed time and CH 3 SH concentration when anatase type TiO 2 having an average particle size of 100 ° is used.
【図８】熱処理温度と３０分後の臭気除去率との関係を
示すグラフ。FIG. 8 is a graph showing the relationship between the heat treatment temperature and the odor removal rate after 30 minutes.
【図９】平均粒径５００Åのアナターゼ型ＴiＯ2を用い
た場合の経過時間とＣＨ3ＳＨ濃度との関係を示すグラ
フ。FIG. 9 is a graph showing the relationship between elapsed time and CH 3 SH concentration when anatase type TiO 2 having an average particle size of 500 ° is used.
【図１０】従来の製造方法によって得られた光触媒機能
を有する部材の断面図。FIG. 10 is a cross-sectional view of a member having a photocatalytic function obtained by a conventional manufacturing method.
１…タイル素地、２…釉薬層、３…ＴiＯ2粒子、４…イ
ンク層、５…離型紙、６…水溶性バインダ、７…バイン
ダ層、８…紫外線反射層、Ｓ…シート、１００…壁材、
１０１…バインダ層、１０２…光触媒粒子。1 ... tile base material, 2 ... glaze layer, 3 ... TiO 2 particles, 4 ... ink layer, 5 ... release paper 6 ... water-soluble binder, 7 ... binder layer, 8 ... UV-reflecting layer, S ... sheet, 100 ... wall Timber,
101: binder layer, 102: photocatalyst particles.
───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.6 識別記号 ＦＩ Ｂ３２Ｂ 9/00 Ｂ３２Ｂ 9/00 Ａ Ｅ０４Ｂ 1/92 Ｅ０４Ｂ 1/92 Ｅ０４Ｃ 2/04 Ｅ０４Ｃ 2/04 Ｃ Ｅ０４Ｆ 13/08 Ｅ０４Ｆ 13/08 Ａ (72)発明者 小島 栄一 福岡県北九州市小倉北区中島２丁目１番１ 号 東陶機器株式会社内 (72)発明者 佐伯 義光 福岡県北九州市小倉北区中島２丁目１番１ 号 東陶機器株式会社内──────────────────────────────────────────────────の Continued on the front page (51) Int.Cl. 6 Identification code FI B32B 9/00 B32B 9/00 A E04B 1/92 E04B 1/92 E04C 2/04 E04C 2/04 C E04F 13/08 E04F 13 / 08 A (72) Inventor Eiichi Kojima 2-1-1 Nakajima, Kokurakita-ku, Kitakyushu-city, Fukuoka Prefecture Inside Totoki Equipment Co., Ltd. (72) Yoshimitsu Saeki 2-1-1 Nakajima, Kokurakita-ku, Kitakyushu-shi, Fukuoka Prefecture No. Totoki Co., Ltd.
Claims (1)
子の層を保持した光触媒機能を有する部材であって、前
記光触媒粒子は平均粒径が１００オングストローム以上
５００オングストローム未満のＴiＯ2微粒子であること
を特徴とする光触媒機能を有する部材。1. A member having a photocatalytic function in which a layer of photocatalyst particles is held on a surface of a base material via a binder layer, wherein the photocatalyst particles are TiO 2 fine particles having an average particle diameter of 100 Å to less than 500 Å. A member having a photocatalytic function.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP11014879A JPH11347420A (en) | 1999-01-22 | 1999-01-22 | Member having photocatalytic function |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP11014879A JPH11347420A (en) | 1999-01-22 | 1999-01-22 | Member having photocatalytic function |
Related Parent Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP10159671A Division JPH1120068A (en) | 1998-06-08 | 1998-06-08 | Material having photocatalytic function and manufacture thereof |
Related Child Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP11062579A Division JPH11322524A (en) | 1999-03-10 | 1999-03-10 | Material having antibacterial activity |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH11347420A true JPH11347420A (en) | 1999-12-21 |
Family
ID=11873312
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP11014879A Pending JPH11347420A (en) | 1999-01-22 | 1999-01-22 | Member having photocatalytic function |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH11347420A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001199001A (en) * | 2000-01-20 | 2001-07-24 | Akira Fujishima | Laminated structure having photocatalyst layer |
-
1999
- 1999-01-22 JP JP11014879A patent/JPH11347420A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001199001A (en) * | 2000-01-20 | 2001-07-24 | Akira Fujishima | Laminated structure having photocatalyst layer |
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