JP2584559B2 - One-component aqueous quick-drying adhesive - Google Patents

One-component aqueous quick-drying adhesive

Info

Publication number
JP2584559B2
JP2584559B2 JP3339455A JP33945591A JP2584559B2 JP 2584559 B2 JP2584559 B2 JP 2584559B2 JP 3339455 A JP3339455 A JP 3339455A JP 33945591 A JP33945591 A JP 33945591A JP 2584559 B2 JP2584559 B2 JP 2584559B2
Authority
JP
Japan
Prior art keywords
adhesive
component
resin
solid content
aqueous
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 - Fee Related
Application number
JP3339455A
Other languages
Japanese (ja)
Other versions
JPH05156224A (en
Inventor
春樹 西池
文俊 築山
保雄 中嶋
一彦 三井
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.)
Daikin Industries Ltd
Resonac Holdings Corp
Original Assignee
Daikin Industries Ltd
Showa Highpolymer 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 Daikin Industries Ltd, Showa Highpolymer Co Ltd filed Critical Daikin Industries Ltd
Priority to JP3339455A priority Critical patent/JP2584559B2/en
Publication of JPH05156224A publication Critical patent/JPH05156224A/en
Application granted granted Critical
Publication of JP2584559B2 publication Critical patent/JP2584559B2/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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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、各種紙器、製袋、包
装、紙管等の紙工用や木工用、天井板(ロックウール化
粧板、インシュレーションボード、パーチクルボード、
石膏ボード、ケイカル板、アクリル板、グラスウー
ル)、自動車内装材、タイル等のごとき、主として多孔
質基材の接着を対象とした、安定で初期接着力の発現が
極めて速い、一液水性即乾型接着剤に関する。
BACKGROUND OF THE INVENTION The present invention relates to a paperboard and a woodwork for various paper containers, bag making, packaging, paper tubes, etc., ceiling boards (rock wool decorative boards, insulation boards, particle boards,
Gypsum board, calcical board, acrylic board, glass wool), automotive interior materials, tiles, etc. For adhesives.

【0002】[0002]

【従来の技術】近年、各種の塗料や接着剤においては、
消防法の改正や各種公害規制の強化の状況下で、有機溶
剤を多量に含む系はますます敬遠され、水性化の要望
が、以前にもまして増大しつつある。水性エマルジョン
系塗料や接着剤は、水性、無公害で、火災等の危険がな
く安全であるばかりでなく、スプレーやロール等各種塗
布設備による作業性が優れ、特に既存設備そのままで、
溶剤系からの切替えが可能である所にメリットがある。
2. Description of the Related Art In recent years, in various paints and adhesives,
Under the circumstances of the revision of the Fire Service Law and the strengthening of various pollution regulations, systems containing a large amount of organic solvents have been further shunned, and the demand for water-based systems has been increasing more than before. Aqueous emulsion paints and adhesives are water-based, non-polluting, safe not only without the danger of fire, etc., but also excellent in workability with various coating equipment such as sprays and rolls.
There is an advantage in that switching from a solvent system is possible.

【0003】水性エマルジョン系接着剤は、火災の危険
もなく、安全、無公害であるため、特に昨今の消防法改
正とも関連して、各業界において盛んに検討されてい
る。しかしながら、水性エマルジョン系接着剤は、本来
水系であるため、蒸発および浸透速度が小さく、乾燥が
遅いため初期接着力の発現が極めて遅く、圧締時間を長
くとらなければ接着しないという難点がある。そのため
に、これら水性エマルジョン系接着剤を用いた各種加工
品の生産性が悪く、不合理であるばかりでなく、接着作
業性が極めて劣るという不都合があった。従って、例え
ば、短時間で接着力の発現が要求されるビルや住宅の天
井板接着、自動車内装材の接着、タイル等における接着
剤としては、極めて不適当であった。
[0003] Aqueous emulsion adhesives are safe and non-polluting without danger of fire, and have been actively studied in various industries, particularly in connection with recent revisions to the Fire Service Law. However, since the aqueous emulsion-based adhesive is originally water-based, it has a low evaporation and permeation rate, and is slow in drying, so that the initial adhesive strength is extremely slow, and there is a problem that the adhesive is not adhered unless the pressing time is long. For this reason, the productivity of various processed products using these aqueous emulsion-based adhesives is poor and not only irrational, but also extremely inferior in bonding workability. Therefore, for example, it is extremely unsuitable as an adhesive for ceilings of buildings and houses, an adhesive for interior materials of automobiles, an adhesive for tiles and the like, which are required to exhibit an adhesive force in a short time.

【0004】これらの諸問題を解決するため、有機溶剤
を添加する方法、被着体を加熱する方法、水性の二液型
接着剤を用いる方法等が提案された。しかし、これらの
方法は、いまだ充分に満足するものではない。例えば有
機溶剤を添加する方法は、環境汚染、火災の危険性等の
問題があり、被着体を加熱する方法は、設備やエネルギ
ーを必要とし、効果も期待できず、被着体の場所によっ
て加熱できない場合もあり、充分とは言えない。また、
水性の二液型接着剤を用いる方法は、主剤と硬化剤とか
らなっており、主剤と硬化剤を2頭ガンで被着体に同時
スプレーするか、主剤と硬化剤を別々の被着体に塗布し
た後貼合するという不便さがある。
In order to solve these problems, a method of adding an organic solvent, a method of heating an adherend, a method of using an aqueous two-component adhesive, and the like have been proposed. However, these methods are not yet fully satisfactory. For example, the method of adding an organic solvent has problems such as environmental pollution and the danger of fire.The method of heating the adherend requires equipment and energy, cannot be expected to be effective, and depends on the place of the adherend. In some cases, heating cannot be performed, which is not sufficient. Also,
The method using an aqueous two-component adhesive comprises a main agent and a curing agent. The main agent and the curing agent are simultaneously sprayed onto the adherend with a two-head gun, or the main agent and the curing agent are separately applied to the adherend. There is an inconvenience of pasting after applying to the surface.

【0005】[0005]

【発明が解決しようとする課題】本発明は、前記従来の
接着剤の欠点を克服し、安定で初期接着力の発現が極め
て速い、一液水性即乾型接着剤を提供することを目的と
する。
SUMMARY OF THE INVENTION An object of the present invention is to provide a one-pack aqueous quick-drying adhesive which overcomes the above-mentioned drawbacks of the conventional adhesive, and which is stable and exhibits an extremely fast initial adhesive strength. I do.

【0006】[0006]

【課題を解決するための手段】本発明者らは、前記従来
の接着剤が有する欠点を解決すべく、鋭意研究の結果、
固形分40〜85%の合成樹脂および天然樹脂から選ば
れた樹脂の水性エマルジョンと、ある種の芳香族系オリ
ゴマーを含む混合物が、一液安定で初期接着力の発現が
極めて速く、即乾型接着剤として有用であることを見出
して、本発明を完成するに到った。
Means for Solving the Problems The present inventors have conducted intensive studies to solve the disadvantages of the conventional adhesives,
Select from synthetic resin and natural resin with solid content of 40-85%
It has been found that a mixture containing the obtained aqueous emulsion of a resin and a certain aromatic oligomer is one-pack stable, has an extremely fast initial adhesive strength, and is useful as a quick-drying adhesive. It was completed.

【0007】即ち、本発明は、(A)固形分40〜85
%の合成樹脂および天然樹脂から選ばれた樹脂の水性エ
マルジョンと(B)下記の一般式(I)で表される芳香
族系オリゴマーとを含む一液水性即乾型接着剤であっ
て、かつ成分(B)の配合量が成分(A)の固形分10
0重量部に対して0.5〜50重量部であることを特徴
とする一液水性即乾型接着剤に関する。 一般式(I)
That is, the present invention relates to (A) a solid content of 40 to 85.
Met% of synthetic resin and the natural resin from the chosen resin aqueous emulsion (B) one-component aqueous immediate drying adhesive containing an aromatic oligomer represented by the following general formula (I)
And the amount of the component (B) is 10% of the solid content of the component (A).
0.5 to 50 parts by weight with respect to 0 parts by weight
And a one-pack aqueous quick-drying adhesive. General formula (I)

【0008】[0008]

【化2】 (但し、nは2〜10の整数であり、RはCm
2m+1で、mが1〜4の整数である。)
Embedded image (Where n is an integer of 2 to 10, and R is C m H
In 2m + 1 , m is an integer of 1 to 4. )

【0009】本発明において用いられる成分(A)の水
性エマルジョンは、通常用いられる合成樹脂および天然
樹脂エマルジョンから適宜選択される。具体的には、例
えば、ポリ酢酸ビニル、アクリル酸エステルやビニルバ
ーサテートと酢酸ビニルの共重合体、アクリル酸エステ
ル、メタクリル酸エステルおよびスチレン各種単独また
は共重合体、エチレン−酢酸ビニル共重合体、エチレン
−酢酸ビニル−アクリル酸エステルやビニルバーサテー
ト等多元共重合体、ポリオレフィン、スチレン−ブタジ
エン共重合体、アクリロニトニル−ブタジエン共重合
体、ポリクロロプレン、ポリイソプレン、ポリウレタ
ン、ポリエポキシアスファルト、スチレン−イソプレン
共重合体、マレイン酸−イソプレン共重合体、ポリ塩化
ビニル、塩化ビニリデン共重合体、ポリビニルアルキル
エーテル、フェノール−ホルマリン反応性混合液、なら
びに天然ゴム等の樹脂等を主成分とする水性エマルジョ
ンであり、所望によりロジン、変性フェノール樹脂、テ
ルペン、石油樹脂、クマロン−インデン樹脂のようなタ
ツキファイヤー、炭酸カルシウム、クレー、シリカ、ア
スベストのような充填材、高級アルコール、各種グリコ
ール類、各種フタル酸エステル、セロソルブ類やテキサ
ノール等の可塑剤、造膜助剤、チタン白、その他の染顔
料のような着色剤、酸化防止剤、紫外線吸収剤、酸素吸
収剤、各種増粘剤のような老化防止剤等を添加した固形
分40〜85%、好ましくは50〜75%のものが挙げ
られる。
The aqueous emulsion of the component (A) used in the present invention is appropriately selected from commonly used synthetic resin and natural resin emulsions. Specifically, for example, polyvinyl acetate, acrylic acid ester or vinyl versate and vinyl acetate copolymer, acrylic acid ester, methacrylic acid ester and styrene various homopolymers or copolymers, ethylene-vinyl acetate copolymer, Multi-component copolymers such as ethylene-vinyl acetate-acrylate and vinyl versatate, polyolefin, styrene-butadiene copolymer, acrylonitonyl-butadiene copolymer, polychloroprene, polyisoprene, polyurethane, polyepoxy asphalt, styrene-isoprene copolymer An aqueous emulsion mainly containing a polymer, a maleic acid-isoprene copolymer, a polyvinyl chloride, a vinylidene chloride copolymer, a polyvinyl alkyl ether, a phenol-formalin reactive mixture, and a resin such as a natural rubber. , If desired, rosin, modified phenolic resin, terpene, petroleum resin, tackifiers such as cumarone-indene resin, calcium carbonate, clay, silica, fillers such as asbestos, higher alcohols, various glycols, various phthalates, Plasticizers such as cellosolves and texanol, film-forming aids, coloring agents such as titanium white and other dyes and pigments, antioxidants, ultraviolet absorbers, oxygen absorbers, antioxidants such as various thickeners, etc. And a solid content of 40 to 85%, preferably 50 to 75%.

【0010】水性エマルジョンの固形分が40%未満の
場合、芳香族系オリゴマーを加えても接着剤の固形分が
低すぎ、即乾性に劣る。また、水性エマルジョンの固形
分が85%より多い場合、芳香族系オリゴマーを加えた
場合高粘度となり作業性に劣る。
When the solid content of the aqueous emulsion is less than 40%, the solid content of the adhesive is too low even if an aromatic oligomer is added, and the quick drying property is poor. When the solid content of the aqueous emulsion is more than 85%, the viscosity becomes high when an aromatic oligomer is added, resulting in poor workability.

【0011】また、本発明において用いられる成分
(B)の芳香族系オリゴマーは、前記一般式(I)で表
されるものである。一般式(I)中のnは2〜10、好
ましくは2〜3のものである。
The aromatic oligomer of the component (B) used in the present invention is represented by the general formula (I). N in the general formula (I) is 2 to 10, preferably 2 to 3.

【0012】一般式(I)で表される芳香族系オリゴマ
ーは、石油精製工程で得られるある種の芳香族留分とホ
ルムアルデヒドを原料とし、酸触媒の存在下に付加縮合
反応して得られるノボラック型樹脂であり、市販品とし
ては、三菱石油(株)社製のオリゴテック1000、オ
リゴテック1020、オリゴテック1030、オリゴテ
ック1040、オリゴテック1100等の液状樹脂が挙
げられる。
The aromatic oligomer represented by the general formula (I) is obtained by subjecting a certain aromatic fraction obtained in a petroleum refining process and formaldehyde as raw materials to an addition condensation reaction in the presence of an acid catalyst. It is a novolak type resin, and commercially available products include liquid resins such as Oligotech 1000, Oligotech 1020, Oligotech 1030, Oligotech 1040, and Oligotech 1100 manufactured by Mitsubishi Petroleum Corporation.

【0013】オリゴテックには、固形樹脂、液状樹脂お
よび樹脂をエマルジョン化した乳化樹脂があるが、水性
エマルジョンの樹脂成分との相溶性の点からは上記のご
とき液状のオリゴテックの使用が好ましい。
Oligotech includes solid resin, liquid resin and emulsified resin obtained by emulsifying the resin. From the viewpoint of compatibility with the resin component of the aqueous emulsion, use of the above-mentioned liquid oligotech is preferred.

【0014】一般式(I)で表される成分(B)の芳香
族系オリゴマーの配合量は、成分(A)の水性エマルジ
ョンの固形分100重量部に対し0.5〜50重量部が
好ましく、とりわけ2〜30重量部が好適である。成分
(B)の芳香族系オリゴマーの配合量が0.5重量部未
満の場合は、前記諸効果の発現が不充分である。また、
成分(B)の芳香族系オリゴマーの配合量が50重量部
より多い場合は、可塑化効果が強すぎるため、樹脂の凝
集力を低下させ、好ましくない。
The amount of the aromatic oligomer of the component (B) represented by the general formula (I) is preferably 0.5 to 50 parts by weight based on 100 parts by weight of the solid content of the aqueous emulsion of the component (A). In particular, 2 to 30 parts by weight is suitable. When the blending amount of the aromatic oligomer of the component (B) is less than 0.5 part by weight, the effects described above are insufficiently exhibited. Also,
If the blending amount of the aromatic oligomer of the component (B) is more than 50 parts by weight, the plasticizing effect is too strong, and the cohesive strength of the resin is reduced, which is not preferable.

【0015】[0015]

【作用】成分(B)の芳香族系オリゴマーの役割は、成
分(A)の水性エマルジョンにおける樹脂成分を可塑化
し、より柔軟性を付与し、樹脂皮膜のタックを向上させ
ると同時に、被着体に対するぬれ性を改善し、樹脂の浸
透を助ける。また、特に液状で水性エマルジョンに添加
した場合、エマルジョンの粘性を改良し、接着剤として
ウェットな状態で被着体同士があたかも接着したかのよ
うな状態となり、お互いに剥離しにくくなるため、圧締
に要する時間を大幅に短縮せしめることが可能となる。
さらに、芳香族系オリゴマーの性状がオリゴマーである
ため、蒸発し難く、水性エマルジョンの固形分の増大に
寄与し、このために乾燥速度を大幅に増大させることが
でき、接着剤としての初期接着力の発現を著しく速める
ことができる。
The role of the aromatic oligomer of the component (B) is to plasticize the resin component in the aqueous emulsion of the component (A), to provide more flexibility and to improve the tack of the resin film, Improves wettability to water and helps resin penetration. In particular, when added to an aqueous emulsion in the form of a liquid, the viscosity of the emulsion is improved, and the adherends are in a wet state as an adhesive, as if they were adhered to each other, making it difficult for the adherends to peel off from each other. The time required for fastening can be greatly reduced.
Further, since the aromatic oligomer is a property of an oligomer, it hardly evaporates and contributes to an increase in the solid content of the aqueous emulsion. Therefore, the drying speed can be greatly increased. Can be remarkably accelerated.

【0016】本発明方法一液水性即乾型接着剤は、特
に被着体の少なくとも一方が多孔質で吸水性の場合に有
効である。また、本発明の一液水性即乾型接着剤は、水
性塗料にも適用でき、前記したような同様な作用、効果
により、塗料の粘性を改良し、被着体へのぬれ性を高
め、接着力を改善すると同時に乾燥性を大幅に改善する
ことが可能である。また、さらにコーキング材やシーリ
ング材への応用も、同様な作用を想定して期待できる。
The one-component aqueous quick-drying adhesive of the present invention is particularly effective when at least one of the adherends is porous and water-absorbing. Further, the one-pack aqueous quick-drying adhesive of the present invention can be applied to water-based paints, and by the same action and effect as described above, improves the viscosity of the paints and enhances the wettability to adherends. It is possible to improve the adhesive force and at the same time significantly improve the drying property. Further, application to a caulking material or a sealing material can be expected assuming a similar effect.

【0017】[0017]

【実施例】以下、実施例および比較例を挙げて本発明を
さらに詳細に説明する。
The present invention will be described below in more detail with reference to examples and comparative examples.

【0018】実施例1 固形分60%のエチレン−酢酸ビニル共重合体エマルジ
ョンの固形分100重量部に対して、芳香族系オリゴマ
ーとしてオリゴテック1030(三菱石油(株)社製)
20重量部とポリエーテル型増粘剤3重量部を加え、デ
ィスパーにて1時間撹拌し、固形分66%、粘度10万
cps の接着剤を作製した。
Example 1 Oligotec 1030 (manufactured by Mitsubishi Petroleum Co., Ltd.) as an aromatic oligomer per 100 parts by weight of a solid content of an ethylene-vinyl acetate copolymer emulsion having a solid content of 60%.
20 parts by weight and 3 parts by weight of a polyether-type thickener were added, and the mixture was stirred for 1 hour with a disper.
An adhesive of cps was made.

【0019】実施例2〜8および比較例1〜4 水性エマルジョンの固形分100重量部に対して、芳香
族系オリゴマーとしてオリゴテック1030(三菱石油
(株)社製)、ポリエーテル型増粘剤を表1〜表3に示
す割合で混合し、ディスパーにて1時間撹拌して接着剤
を作製した。得られた接着剤の固形分および粘度を表1
〜表3に示した。
Examples 2 to 8 and Comparative Examples 1 to 4 Oligotec 1030 (manufactured by Mitsubishi Petroleum Co., Ltd.) as an aromatic oligomer and a polyether-type thickener based on 100 parts by weight of the solid content of the aqueous emulsion Were mixed at the ratios shown in Tables 1 to 3 and stirred for 1 hour with a disper to prepare an adhesive. Table 1 shows the solid content and viscosity of the obtained adhesive.
~ Shown in Table 3.

【0020】[0020]

【表1】 [Table 1]

【0021】[0021]

【表2】 [Table 2]

【0022】[0022]

【表3】 [Table 3]

【0023】以上により作製した各種接着剤を縦60c
m、横30cmの大きさのロックウール化粧板にウェット
で7g塗布し、石膏ボードと貼り合せ、接着に要する時
間(初期接着性)を測定した。その結果を表4〜表6に
示した。
The above-prepared adhesives were applied in a length of 60 c.
7 g of a 30-cm-wide rock wool decorative board was wet-coated, bonded to a gypsum board, and the time required for adhesion (initial adhesion) was measured. The results are shown in Tables 4 to 6.

【0024】次に、同じ各種接着剤をライナー紙に50
g/m2 塗布し、ライナー紙同士を貼合し、接着に要す
る時間(初期接着性)を測定した。その結果を表4〜表
6に示した。
Next, the same various adhesives were applied to liner paper for 50 times.
g / m 2 , the liner papers were stuck together, and the time required for adhesion (initial adhesion) was measured. The results are shown in Tables 4 to 6.

【0025】また、上記各種接着剤を4×4cmのまかん
ばの柾目板(容積密度0.5g/cm3 )に100g/m
2 塗布し、ただちにまかんばの柾目板に接着させ、1分
後の引っ張り接着力(初期接着力)と20℃×65%R
Hの恒温室で24時間乾燥後の引っ張り接着力を測定し
た。その結果を表4〜表6に示した。
The above-mentioned various adhesives were applied to a 4 × 4 cm straight-grained straight-grained board (volume density 0.5 g / cm 3 ) at a rate of 100 g / m 2.
2 Coating, immediately adhere to the straight-grained board of makanba, 1 minute after tensile adhesion (initial adhesion) and 20 ℃ × 65% R
The tensile adhesion after drying in a constant temperature chamber of H for 24 hours was measured. The results are shown in Tables 4 to 6.

【0026】[0026]

【表4】 [Table 4]

【0027】[0027]

【表5】 [Table 5]

【0028】[0028]

【表6】 [Table 6]

【0029】表4〜表6から明らかなごとく、本発明の
一液水性即乾型接着剤は、特に多孔質被着体への初期接
着力の発現が極めて速いことが認められる。
As is evident from Tables 4 to 6, it is recognized that the one-pack aqueous quick-drying adhesive of the present invention has an extremely fast initial adhesive strength particularly to a porous adherend.

【0030】[0030]

【発明の効果】本発明の一液水性即乾型接着剤は、一液
安定で初期接着力の発現が極めて短時間であるため、ビ
ルや住宅の天井板接着、自動車内装材の接着、タイル等
における接着剤として有効利用が可能である。
The one-pack water-based quick-drying adhesive of the present invention is stable in one-pack and has a very short initial adhesive strength. And the like can be effectively used as an adhesive.

───────────────────────────────────────────────────── フロントページの続き (72)発明者 三井 一彦 大阪府大阪市北区中之島2丁目3番18号 大建工業株式会社内 ──────────────────────────────────────────────────続 き Continuation of front page (72) Inventor Kazuhiko Mitsui 2-3-18 Nakanoshima, Kita-ku, Osaka City, Osaka Inside Daiken Kogyo Co., Ltd.

Claims (1)

(57)【特許請求の範囲】(57) [Claims] 【請求項1】 (A)固形分40〜85%の合成樹脂お
よび天然樹脂から選ばれた樹脂の水性エマルジョンと
(B)下記の一般式(I)で表される芳香族系オリゴマ
ーとを含む一液水性即乾型接着剤であって、かつ成分
(B)の配合量が成分(A)の固形分100重量部に対
して0.5〜50重量部であることを特徴とする一液水
性即乾型接着剤。 一般式(I) 【化1】 (但し、nは2〜10の整数であり、RはC
2m+1で、mが1〜4の整数である。)
1. A synthetic resin having a solid content of 40 to 85% .
And the aqueous emulsion of selected resins from natural resins (B) A one-component aqueous immediate drying adhesive containing an aromatic oligomer represented by the following general formula (I), and component
The blending amount of (B) is based on 100 parts by weight of the solid content of component (A).
A one-pack aqueous quick-drying adhesive characterized in that the amount is 0.5 to 50 parts by weight . General formula (I) (However, n is an integer of 2 to 10, and R is C m H
In 2m + 1 , m is an integer of 1 to 4. )
JP3339455A 1991-11-29 1991-11-29 One-component aqueous quick-drying adhesive Expired - Fee Related JP2584559B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP3339455A JP2584559B2 (en) 1991-11-29 1991-11-29 One-component aqueous quick-drying adhesive

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP3339455A JP2584559B2 (en) 1991-11-29 1991-11-29 One-component aqueous quick-drying adhesive

Publications (2)

Publication Number Publication Date
JPH05156224A JPH05156224A (en) 1993-06-22
JP2584559B2 true JP2584559B2 (en) 1997-02-26

Family

ID=18327632

Family Applications (1)

Application Number Title Priority Date Filing Date
JP3339455A Expired - Fee Related JP2584559B2 (en) 1991-11-29 1991-11-29 One-component aqueous quick-drying adhesive

Country Status (1)

Country Link
JP (1) JP2584559B2 (en)

Also Published As

Publication number Publication date
JPH05156224A (en) 1993-06-22

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