JP2991573B2 - Antimicrobial composition - Google Patents

Antimicrobial composition

Info

Publication number
JP2991573B2
JP2991573B2 JP4239857A JP23985792A JP2991573B2 JP 2991573 B2 JP2991573 B2 JP 2991573B2 JP 4239857 A JP4239857 A JP 4239857A JP 23985792 A JP23985792 A JP 23985792A JP 2991573 B2 JP2991573 B2 JP 2991573B2
Authority
JP
Japan
Prior art keywords
silver
antibacterial
antibacterial composition
silica gel
water
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.)
Expired - Lifetime
Application number
JP4239857A
Other languages
Japanese (ja)
Other versions
JPH0687711A (en
Inventor
冨岡  敏一
冨田  勝己
西野  敦
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Panasonic Holdings Corp
Original Assignee
Matsushita Electric Industrial Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Matsushita Electric Industrial Co Ltd filed Critical Matsushita Electric Industrial Co Ltd
Priority to JP4239857A priority Critical patent/JP2991573B2/en
Publication of JPH0687711A publication Critical patent/JPH0687711A/en
Application granted granted Critical
Publication of JP2991573B2 publication Critical patent/JP2991573B2/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Landscapes

  • Agricultural Chemicals And Associated Chemicals (AREA)

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【0001】[0001]

【産業上の利用分野】本発明は抗菌性組成物に関するも
のである。
FIELD OF THE INVENTION The present invention relates to an antibacterial composition.

【0002】[0002]

【従来の技術】近年、合成樹脂製品が多用されるにいた
り、例えば、台所用品などのように衛生面で注意を払う
必要がある分野に用いられる場合に、合成樹脂製品表面
の菌による汚染が問題となってきている。また、建築用
資材として使用されているコーキング材表面に菌がは
え、衛生面は勿論のこと外観的にも悪くなるなどの問題
が生じている。その対策として合成樹脂中に抗菌性組成
物を混入し、合成樹脂製品表面にこの組成物を溶出させ
て製品表面の殺菌を行なう方法が用いられている。
2. Description of the Related Art In recent years, when synthetic resin products are used extensively, or when used in fields where hygiene needs to be paid attention, such as kitchenware, contamination of bacteria on the surface of the synthetic resin products is caused by bacteria. Is becoming a problem. In addition, there is a problem that bacteria grow on the surface of the caulking material used as a building material, which deteriorates not only hygiene but also appearance. As a countermeasure, a method has been used in which an antibacterial composition is mixed into a synthetic resin and the composition is eluted on the surface of the synthetic resin product to sterilize the product surface.

【0003】[0003]

【発明が解決しようとする課題】合成樹脂製品表面に抗
菌性能を付与させる材料として、有機系の抗菌剤と無機
系の抗菌剤がある。これらの抗菌剤の内、有機系抗菌剤
は揮発性を有するため、これを合成樹脂に含有させる
と、合成樹脂製品の周囲環境が汚染され、またこの合成
樹脂製品の表面と接触した排液中には、抗菌剤が含有さ
れており、これが排水環境汚染の原因となり、さらに、
下水処理中の活性汚泥に影響を及ぼすなどの問題があ
る。
There are an organic antibacterial agent and an inorganic antibacterial agent as materials for imparting antibacterial performance to the surface of a synthetic resin product. Of these antibacterial agents, organic antibacterial agents have volatility, so if they are contained in synthetic resin, the surrounding environment of the synthetic resin product will be polluted, and the wastewater in contact with the surface of this synthetic resin product Contains antimicrobial agents, which cause wastewater pollution,
There are problems such as affecting activated sludge during sewage treatment.

【0004】一方、無機系抗菌剤で抗菌性能を付与させ
るために最も抗菌効果の高いものとして銀系抗菌剤が用
いられるが、加熱により呈色し、樹脂に混練して用いる
場合200℃以上の成型温度で着色してしまうという問
題点があった。
On the other hand, a silver-based antibacterial agent is used as the inorganic antibacterial agent having the highest antibacterial effect in order to impart antibacterial performance. There was a problem of coloring at the molding temperature.

【0005】本発明はこのような課題を解決するもの
で、樹脂製品表面上で安定した抗菌効果を示し、また樹
脂中より溶出しても環境汚染の原因となりにくい抗菌性
組成物を提供することを目的とする。
The present invention has been made to solve the above problems, and provides an antibacterial composition which exhibits a stable antibacterial effect on the surface of a resin product and which does not easily cause environmental pollution even if it is eluted from the resin. With the goal.

【0006】[0006]

【課題を解決するための手段】この課題を解決するため
に本発明は、水溶性銀塩、銀錯塩または銀化合物をシリ
カゲルに担持吸着させ、480℃以上600℃以下の温
度で焼成してなるものである。また本発明は、水溶性銀
塩、銀錯塩または銀化合物をシリカゲルに担持吸着さ
せ、480℃以上600℃以下の温度で焼成した抗菌性
組成物の表面の少なくとも1部を反応性有機珪素化合物
の加水分解物でコーティングしてなるものである。さら
に本発明は、水溶性銀塩、銀錯塩または銀化合物をシリ
カゲルに担持吸着して乾燥粉砕させ、その表面の少なく
とも1部を反応性有機珪素化合物の加水分解物でコーテ
ィングし、480℃以上600℃以下の温度で焼成して
なるものである。
According to the present invention, a water-soluble silver salt, a silver complex salt or a silver compound is supported and adsorbed on silica gel, and calcined at a temperature of 480 ° C to 600 ° C. Things. Further, the present invention provides a method in which a water-soluble silver salt, a silver complex salt or a silver compound is carried and adsorbed on silica gel, and at least a part of the surface of the antibacterial composition baked at a temperature of 480 ° C. or more and 600 ° C. or less has a reactive organic silicon compound. It is formed by coating with a hydrolyzate. Further, in the present invention, a water-soluble silver salt, a silver complex salt or a silver compound is supported on silica gel, adsorbed and dried and pulverized, and at least a part of its surface is coated with a hydrolyzate of a reactive organic silicon compound. It is obtained by firing at a temperature of not more than ℃.

【0007】上記水溶性銀塩、銀錯塩または銀化合物は
そのまま用いても良く、例えば水溶性銀塩として酢酸銀
を用い、これを水溶媒に溶解させた後、亜硫酸アンモニ
ウム塩およびチオ硫酸アンモニウム塩を反応させた液中
にシリカゲルを入れ吸着させるようにしても良い。ま
た、上記亜硫酸アンモニウム塩およびチオ硫酸アンモニ
ウム塩は亜硫酸アンモニウムおよびチオ硫酸アンモニウ
ム・ナトリウムが用いられる。さらに上記有機珪素化合
物はテトラエトキシシランが用いられる。
The above water-soluble silver salt, silver complex salt or silver compound may be used as it is. For example, silver acetate is used as a water-soluble silver salt, and after dissolving it in an aqueous solvent, ammonium sulfite and ammonium thiosulfate are used. Silica gel may be placed in the reacted liquid and adsorbed. As the above-mentioned ammonium sulfite and ammonium thiosulfate, ammonium sulfite and ammonium sodium thiosulfate are used. Further, tetraethoxysilane is used as the organic silicon compound.

【0008】[0008]

【作用】以上のように構成された本発明の抗菌性組成物
は、樹脂製品表面上で安定した抗菌効果を示し、樹脂中
より溶出しても環境汚染の原因となりにくいものとな
る。また、成型した樹脂片の呈色も少なくなる。
The antibacterial composition of the present invention thus constituted exhibits a stable antibacterial effect on the surface of a resin product, and hardly causes environmental pollution even if it is eluted from the resin. Also, the coloration of the molded resin piece is reduced.

【0009】[0009]

【実施例】以下、本発明の実施例について説明する。 実施例1 酢酸銀などの水溶性銀塩100重量部、亜硫酸アンモニ
ウム230重量部、およびチオ硫酸アンモニウム・ナト
リウム180重量部を塩素を含まない水に加えて溶解さ
せ、充分攪拌しながら混合しチオスルファト銀錯塩水溶
液を得た。
Embodiments of the present invention will be described below. Example 1 100 parts by weight of a water-soluble silver salt such as silver acetate, 230 parts by weight of ammonium sulfite, and 180 parts by weight of sodium ammonium thiosulfate were added to and dissolved in water containing no chlorine, and mixed with sufficient stirring to obtain a silver thiosulfato complex. An aqueous solution was obtained.

【0010】本実施例に用いる担体は、「JIS Z
0701包装用シリカゲル乾燥剤」に記載のB型のシリ
カゲル粉末である。このB型シリカゲル粉末は低湿度で
は吸湿率が低く、高湿度では吸湿率が高く、かつ高湿度
における総吸湿量の高いシリカゲル粉末であり、その平
均粒径は8μm程度である。
The carrier used in this embodiment is "JIS Z".
0701 silica gel desiccant for packaging ". The B-type silica gel powder has a low moisture absorption rate at low humidity, a high moisture absorption rate at high humidity, and a high total moisture absorption at high humidity, and has an average particle size of about 8 μm.

【0011】このシリカゲル粉末を180℃で2時間以
上乾燥させた。上記シリカゲル100重量部に対し、銀
成分として2重量部になるように前記チオスルファト銀
錯塩水溶液を混合した。その後、速やかに溶媒および担
体中に吸収された水分を除去した。次いで、これを所定
の粒径に粉砕して、抗菌性材料が担持されたシリカゲル
を得た。
The silica gel powder was dried at 180 ° C. for 2 hours or more. The silver thiosulfato complex solution was mixed with 100 parts by weight of the silica gel so that the silver component was 2 parts by weight. Thereafter, the solvent and the water absorbed in the carrier were promptly removed. Next, this was pulverized to a predetermined particle size to obtain silica gel carrying an antibacterial material.

【0012】このシリカゲルを昇温速度約10℃/分で
500℃まで加熱し、抗菌性組成物を得た。上記熱処理
温度が480℃未満では抗菌性組成物は暗褐色に呈色
し、600℃を超えるとシリカゲルがガラス化し、粒子
生長もするため、樹脂への混練に適さない。
The silica gel was heated to 500 ° C. at a rate of about 10 ° C./min to obtain an antibacterial composition. If the heat treatment temperature is lower than 480 ° C., the antibacterial composition turns dark brown, and if it exceeds 600 ° C., the silica gel is vitrified and the particles grow, so that the composition is not suitable for kneading to a resin.

【0013】表1に本実施例1で得られた抗菌性組成物
の抗菌性能を示し、表1からも本実施例1の抗菌性組成
物は実用的な抗菌性能を有することがわかる。なお、抗
菌試験において大腸菌(Escherichia coli)、黄色ブド
ウ状球菌(Staphylococcus aureus )、バチルス属菌
(Bacillus subtillis)を用い、滴下法に準じた。評価
は24時間後に行なった。
Table 1 shows the antibacterial performance of the antibacterial composition obtained in Example 1, and Table 1 shows that the antibacterial composition of Example 1 has practical antibacterial performance. In the antibacterial test, Escherichia coli, Staphylococcus aureus, and Bacillus subtillis were used and the dropping method was followed. The evaluation was performed after 24 hours.

【0014】また、実施例1の抗菌性組成物1%を、ポ
リプロピレン樹脂中に分散混練し、成型した樹脂片の呈
色状態をも表1に示す。
Table 1 also shows the coloration of the resin pieces formed by dispersing and kneading 1% of the antibacterial composition of Example 1 in a polypropylene resin.

【0015】実施例2 実施例1と同様の方法で抗菌性組成物を得、さらに反応
性有機珪素化合物としてテトラエトキシシラン100重
量部をエチルアルコールに希釈混合させた溶液に、上記
シリカゲル100重量部を分散させた後、これに純水を
加えてテトラエトキシシランを加水分解させ、上記実施
例1で得られた抗菌性組成物の表面の少なくとも1部を
コーティングした。次いでこれを乾燥させて実施例2の
抗菌性組成物を得た。
Example 2 An antibacterial composition was obtained in the same manner as in Example 1, and 100 parts by weight of the above silica gel was added to a solution obtained by diluting 100 parts by weight of tetraethoxysilane as a reactive organosilicon compound in ethyl alcohol. Was dispersed therein, and pure water was added thereto to hydrolyze tetraethoxysilane. At least a part of the surface of the antibacterial composition obtained in Example 1 was coated. Next, this was dried to obtain the antibacterial composition of Example 2.

【0016】表1に本実施例2で得られた抗菌性組成物
の抗菌性能を示し、表1からも本実施例2の抗菌性組成
物は実用的な抗菌性能を有することがわかる。なお、抗
菌試験において大腸菌(Escherichia coli)、黄色ブド
ウ状球菌(Staphylococcus aureus )、バチルス属菌
(Bacillus subtillis) を用い、滴下法に準じた。評価
は24時間後に行なった。
Table 1 shows the antibacterial performance of the antibacterial composition obtained in Example 2, and Table 1 shows that the antibacterial composition of Example 2 has practical antibacterial performance. In the antibacterial test, Escherichia coli, Staphylococcus aureus, and Bacillus subtillis were used, and the dropping method was followed. The evaluation was performed after 24 hours.

【0017】また、実施例2の抗菌性組成物1%を、ポ
リプロピレン樹脂中に分散混練し、成型した樹脂片の呈
色状態をも表1に示す。
Table 1 also shows the coloration of the resin pieces obtained by dispersing and kneading 1% of the antibacterial composition of Example 2 in a polypropylene resin and molding.

【0018】実施例3 実施例1と同様の方法で抗菌性材料が担持されたシリカ
ゲルを得た。反応性有機珪素化合物としてテトラエトキ
シシラン100重量部をエチルアルコールに希釈混合さ
せた溶液に、上記抗菌性材料が担持されたシリカゲル1
00重量部を分散させた後、これに純水を加えてテトラ
エトキシシランを加水分解させ、上記シリカゲルの表面
の少なくとも1部をコーティングした。次いでこれを乾
燥させた。上記コーティング処理済みのシリカゲルを昇
温速度約10℃/分で500℃まで加熱し、実施例3の
抗菌性組成物を得た。
Example 3 In the same manner as in Example 1, a silica gel carrying an antibacterial material was obtained. Silica gel 1 carrying the above antibacterial material in a solution obtained by diluting and mixing 100 parts by weight of tetraethoxysilane as a reactive organic silicon compound in ethyl alcohol.
After dispersing 00 parts by weight, pure water was added thereto to hydrolyze tetraethoxysilane, and at least a part of the surface of the silica gel was coated. It was then dried. The coated silica gel was heated to 500 ° C. at a heating rate of about 10 ° C./min to obtain the antibacterial composition of Example 3.

【0019】表1に本実施例3で得られた抗菌性組成物
の抗菌性能を示し、表1からも本実施例3の抗菌性組成
物は実用的な抗菌性能を有することがわかる。なお、抗
菌試験において大腸菌(Escherichia coli)、黄色ブド
ウ状球菌(Staphylococcus aureus )、バチルス属菌
(Bacillus subtillis)を用い、滴下法に準じた。評価
は24時間後に行なった。
Table 1 shows the antibacterial performance of the antibacterial composition obtained in Example 3, and Table 1 shows that the antibacterial composition of Example 3 has practical antibacterial performance. In the antibacterial test, Escherichia coli, Staphylococcus aureus, and Bacillus subtillis were used and the dropping method was followed. The evaluation was performed after 24 hours.

【0020】また、実施例3の抗菌性組成物1%を、ポ
リプロピレン樹脂中に分散混練し、成型した樹脂片の呈
色状態をも表1に示す。
Table 1 also shows the coloration of the resin pieces obtained by dispersing and kneading 1% of the antibacterial composition of Example 3 in a polypropylene resin and molding.

【0021】比較例1 実施例1と同様の方法で抗菌性材料が担持されたシリカ
ゲルを得て、これを加熱せずに用いた。
Comparative Example 1 A silica gel carrying an antibacterial material was obtained in the same manner as in Example 1 and used without heating.

【0022】この比較例1のシリカゲルを用いて実施例
1〜実施例3と同様の方法で抗菌性能および樹脂片の呈
色状態を試験した結果を表1に示しているが、表1から
も樹脂呈色する点で実施例1〜実施例3に比べて劣るこ
とが分かる。
Using the silica gel of Comparative Example 1 and testing the antibacterial performance and the coloration of the resin pieces in the same manner as in Examples 1 to 3, the results are shown in Table 1. It can be seen that the resin coloration is inferior to Examples 1 to 3 in coloration.

【0023】[0023]

【表1】 [Table 1]

【0024】[0024]

【発明の効果】以上のように本発明によれば、水溶性銀
塩、銀錯塩または銀化合物を吸着担持させたシリカゲル
を480℃以上600℃以下の温度でで熱処理すること
により、成型した樹脂片の呈色も少なく、かつ良好な抗
菌性能を発揮することができる。
As described above, according to the present invention, a resin molded by heat-treating silica gel adsorbing and supporting a water-soluble silver salt, silver complex salt or silver compound at a temperature of 480 ° C. to 600 ° C. The coloration of the piece is small and good antibacterial performance can be exhibited.

フロントページの続き (56)参考文献 特開 平5−43414(JP,A) 特開 平5−306207(JP,A) 特開 平6−125970(JP,A) 特開 平5−58829(JP,A) 特開 平6−87710(JP,A) 特開 平5−155725(JP,A) (58)調査した分野(Int.Cl.6,DB名) A01N 59/16 A01N 25/26 Continuation of the front page (56) References JP-A-5-43414 (JP, A) JP-A-5-306207 (JP, A) JP-A-6-125970 (JP, A) JP-A-5-58829 (JP) JP-A-6-87710 (JP, A) JP-A-5-155725 (JP, A) (58) Fields investigated (Int. Cl. 6 , DB name) A01N 59/16 A01N 25/26

Claims (7)

(57)【特許請求の範囲】(57) [Claims] 【請求項1】 水溶性銀塩、銀錯塩または銀化合物をシ
リカゲルに担持吸着させ、480℃以上600℃以下の
温度で焼成してなることを特徴とする抗菌性組成物。
1. An antibacterial composition comprising a water-soluble silver salt, a silver complex salt or a silver compound carried and adsorbed on silica gel and calcined at a temperature of 480 ° C. or more and 600 ° C. or less.
【請求項2】 水溶性銀塩、銀錯塩または銀化合物をシ
リカゲルに担持吸着させ、480℃以上600℃以下の
温度で焼成した抗菌性組成物の表面の少なくとも1部を
反応性有機珪素化合物の加水分解物でコーティングして
なることを特徴とする抗菌性組成物。
2. An antibacterial composition, wherein a water-soluble silver salt, a silver complex salt or a silver compound is carried and adsorbed on silica gel and calcined at a temperature of 480 ° C. or more and 600 ° C. or less, at least a part of the surface of the reactive organic silicon compound An antibacterial composition characterized by being coated with a hydrolyzate.
【請求項3】 水溶性銀塩、銀錯塩または銀化合物をシ
リカゲルに担持吸着して乾燥粉砕させ、その表面の少な
くとも1部を反応性有機珪素化合物の加水分解物でコー
ティングし、480℃以上600℃以下の温度で焼成し
てなることを特徴とする抗菌性組成物。
3. A water-soluble silver salt, silver complex salt or silver compound is supported on silica gel, adsorbed and dried and pulverized, and at least a part of its surface is coated with a hydrolyzate of a reactive organic silicon compound. An antibacterial composition characterized by being calcined at a temperature of not more than ℃.
【請求項4】 水溶性銀塩を水溶媒に溶解させた後、亜
硫酸アンモニウム塩およびチオ硫酸アンモニウム塩を反
応させた液中にシリカゲルを入れ吸着させることを特徴
とする請求項1または2または3記載の抗菌性組成物。
4. The method according to claim 1, wherein after dissolving the water-soluble silver salt in the aqueous solvent, silica gel is adsorbed in a liquid obtained by reacting ammonium sulfite and ammonium thiosulfate. Antimicrobial composition.
【請求項5】 亜硫酸アンモニウム塩およびチオ硫酸ア
ンモニウム塩は亜硫酸アンモニウムおよびチオ硫酸アン
モニウム・ナトリウムであることを特徴とする請求項4
記載の抗菌性組成物。
5. The method according to claim 4, wherein the ammonium sulfite and the ammonium thiosulfate are ammonium sulfite and ammonium sodium thiosulfate.
The antibacterial composition according to any one of the preceding claims.
【請求項6】 水溶性銀塩は酢酸銀であることを特徴と
する請求項4記載の抗菌性組成物。
6. The antibacterial composition according to claim 4, wherein the water-soluble silver salt is silver acetate.
【請求項7】 有機珪素化合物はテトラエトキシシラン
であることを特徴とする請求項2または3記載の抗菌性
組成物。
7. The antibacterial composition according to claim 2, wherein the organosilicon compound is tetraethoxysilane.
JP4239857A 1992-09-09 1992-09-09 Antimicrobial composition Expired - Lifetime JP2991573B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP4239857A JP2991573B2 (en) 1992-09-09 1992-09-09 Antimicrobial composition

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP4239857A JP2991573B2 (en) 1992-09-09 1992-09-09 Antimicrobial composition

Publications (2)

Publication Number Publication Date
JPH0687711A JPH0687711A (en) 1994-03-29
JP2991573B2 true JP2991573B2 (en) 1999-12-20

Family

ID=17050917

Family Applications (1)

Application Number Title Priority Date Filing Date
JP4239857A Expired - Lifetime JP2991573B2 (en) 1992-09-09 1992-09-09 Antimicrobial composition

Country Status (1)

Country Link
JP (1) JP2991573B2 (en)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP4804669B2 (en) * 2001-08-20 2011-11-02 興亜硝子株式会社 Antibacterial material and antibacterial resin composition

Also Published As

Publication number Publication date
JPH0687711A (en) 1994-03-29

Similar Documents

Publication Publication Date Title
US5510109A (en) Antibacterial and antifungal composition
JPS627748A (en) Moistureproof antifungal zeolite composition and its production
JP2991573B2 (en) Antimicrobial composition
JPH1179921A (en) Antimicrobial and antifungal composition and its production
JP3347875B2 (en) Antibacterial antiviral antifungal agent and its complex
JP3166277B2 (en) Antimicrobial composition
JP3154374B2 (en) Manufacturing method of antibacterial material
JP2988012B2 (en) Antimicrobial composition
JP3107450B2 (en) Antibacterial material and method for producing the same
JPH054816A (en) Antibacterial titania
JPS63221175A (en) Coating wall and spraying material having mildewproofing and antibacterial performance
JP3585059B2 (en) Antimicrobial composition and method for producing antimicrobial resin composition
JP3049906B2 (en) Antibacterial resin
JPH08113729A (en) Antimicrobial composition and production thereof
JPH07247205A (en) Antimicrobial agent
JP3067905B2 (en) Antibacterial antifungal composition, antibacterial antifungal resin and antibacterial antifungal caulking material
JP3127745B2 (en) Granules for microbial control
JP2001010850A (en) Inorganic filling admixture
JP2965834B2 (en) Antibacterial particles
JP3154371B2 (en) Manufacturing method of antibacterial material
JPH0543414A (en) Production of antibacterial mildew-proofing composition
JPH07238001A (en) Antimicrobial additive for resin and molding of antimicrobial resin
JP3350212B2 (en) Antimicrobial composition
JP2965459B2 (en) Antimicrobial composite and method for producing the same
JPH04231063A (en) Antimicrobial composition

Legal Events

Date Code Title Description
FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20081015

Year of fee payment: 9

FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20091015

Year of fee payment: 10

FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20091015

Year of fee payment: 10

FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20101015

Year of fee payment: 11

FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20111015

Year of fee payment: 12

FPAY Renewal fee payment (event date is renewal date of database)

Free format text: PAYMENT UNTIL: 20121015

Year of fee payment: 13

EXPY Cancellation because of completion of term