JPH04130111A - Production of rubber-reinforced styrene resin material - Google Patents

Production of rubber-reinforced styrene resin material

Info

Publication number
JPH04130111A
JPH04130111A JP24878190A JP24878190A JPH04130111A JP H04130111 A JPH04130111 A JP H04130111A JP 24878190 A JP24878190 A JP 24878190A JP 24878190 A JP24878190 A JP 24878190A JP H04130111 A JPH04130111 A JP H04130111A
Authority
JP
Japan
Prior art keywords
rubber
reinforcing rubber
monomer liquid
monomer
producing
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.)
Granted
Application number
JP24878190A
Other languages
Japanese (ja)
Other versions
JPH0794510B2 (en
Inventor
Kouji Yasutake
保武 晃二
Osamu Wada
修 和田
Masanori Kususe
楠瀬 正憲
Hidekazu Mukai
向井 秀和
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.)
Nippon Steel Chemical and Materials Co Ltd
Original Assignee
Nippon Steel Chemical 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 Nippon Steel Chemical Co Ltd filed Critical Nippon Steel Chemical Co Ltd
Priority to JP24878190A priority Critical patent/JPH0794510B2/en
Publication of JPH04130111A publication Critical patent/JPH04130111A/en
Publication of JPH0794510B2 publication Critical patent/JPH0794510B2/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Abstract

PURPOSE:To dissolve a reinforcing rubber at good efficiency and to obtain continuously the title material of stable properties by dissolving said rubber by a specified means in producing the title material by dissolving said rubber in a monomer solution containing a styrene monomer. CONSTITUTION:A process for producing the title material by dissolving a reinforcing rubber (e.g. polybutadiene rubber) in a monomer solution containing a styrene monomer (e.g. styrene/ethylbenzene mixture), which comprises a precut reinforcing rubber adding to a monomer solution in the first agitation tank, agitating the resulting mixture, discharging a monomer solution containing undissolved reinforcing rubber from the bottom of the first agitation tank, wet grinding the undissolved reinforcing rubber contained in the monomer solution, sending the ground rubber to the second agitation tank, and dissolving it under agitation.

Description

【発明の詳細な説明】 〔産業上の利用分野〕 本発明は、ゴム補強スチレン系樹脂原料の製造方法に係
り、特に補強用ゴムとして高粘度のゴムを用いる場合に
好適なゴム補強スチレン系樹脂原料の製造方法に関する
DETAILED DESCRIPTION OF THE INVENTION [Industrial Application Field] The present invention relates to a method for producing a rubber-reinforced styrenic resin raw material, and particularly a rubber-reinforced styrenic resin suitable for using high-viscosity rubber as the reinforcing rubber. It relates to a method for producing raw materials.

〔従来の技術〕[Conventional technology]

ゴム補強スチレン系樹脂を製造する方法としてスチレン
系単量体を含む単量体液に補強用ゴムを溶解した原料を
塊状重合法や溶液重合法により重合する方法がある(特
開昭63−162.713号公報、特開平1−252.
648号公報)。この場合、補強用ゴムの溶解が不十分
であると、原料を重合工程に搬送する配管や、原料から
不純物を除くための濾過装置か目詰まりを起こしたり、
原料をタンクに貯蔵している間に未溶解の補強用ゴムが
タンク内に沈澱したり、得られるコム補強スチレン系樹
脂の品質か不安定になり目標とする物性のものか得られ
なくなる等の問題かおこる。特に、補強用ゴムとして高
粘度のゴムを用いる場合に、ゴムの溶解が不十分になり
やすい。
As a method for manufacturing rubber-reinforced styrenic resin, there is a method in which a raw material obtained by dissolving reinforcing rubber in a monomer liquid containing a styrene monomer is polymerized by bulk polymerization or solution polymerization (Japanese Patent Application Laid-open No. 63-162). Publication No. 713, JP-A-1-252.
Publication No. 648). In this case, if the reinforcing rubber is not sufficiently dissolved, the piping that transports the raw material to the polymerization process and the filtration device that removes impurities from the raw material may become clogged.
While the raw materials are stored in the tank, undissolved reinforcing rubber may settle in the tank, or the quality of the resulting comb-reinforced styrene resin may become unstable, making it impossible to obtain the desired physical properties. A problem will occur. In particular, when a high viscosity rubber is used as the reinforcing rubber, the rubber tends to be insufficiently dissolved.

単量体液に補強用ゴムを溶解する方法として、従来は、
数mm程度の大きさに切断した補強用ゴムを単量体液に
添加して攪拌槽で攪拌することにより溶解していた。と
ころが、攪拌槽での溶解では溶解速度か余り大きくなく
、攪拌を強めても限界があった。そのため、三種以上の
攪拌槽を直列に連結することが行われているが、装置が
大規模になる、攪拌工程での滞留時間が長くなる等の問
題かある。
Conventionally, the method of dissolving reinforcing rubber in monomer liquid was as follows:
Reinforcing rubber cut into pieces about several mm in size was added to the monomer liquid and dissolved by stirring in a stirring tank. However, when dissolving in a stirring tank, the dissolution rate was not very high, and there was a limit even if the stirring was strengthened. For this reason, three or more types of stirring tanks are connected in series, but there are problems such as the equipment becomes large-scale and the residence time in the stirring process becomes long.

〔発明が解決しようとする課題〕[Problem to be solved by the invention]

本発明の目的は、単量体液に補強用ゴムを溶解してゴム
補強スチレン系樹脂原料を製造するために効率のよい方
法を提供することにある。
An object of the present invention is to provide an efficient method for producing a rubber-reinforced styrenic resin raw material by dissolving reinforcing rubber in a monomer liquid.

〔課題を解決するための手段〕[Means to solve the problem]

本発明者は、上記のような課題を解決するため研究を行
い、スチレン系単量体を含む単量体液に補強用ゴムを溶
解するに当り、未溶解の補強用ゴムを湿式粉砕すること
により、ゴムの溶解が効率よく行えることを見出し本発
明を完成した。
The present inventor conducted research to solve the above problems, and when dissolving reinforcing rubber in a monomer liquid containing a styrene monomer, the undissolved reinforcing rubber was wet-pulverized. discovered that rubber can be dissolved efficiently and completed the present invention.

すなわち、本発明は、スチレン系単量体を含む単量体液
に補強用ゴムを溶解してゴム補強スチレン系樹脂原料を
製造する方法であって、予め切断した補強用ゴムを第一
の攪拌槽内の単量体液に添加して攪拌し、該第一の攪拌
槽の底部から未溶解の補強用ゴムを含む単量体液を流出
し、該単量体液に含まれている未溶解の補強用ゴムを湿
式粉砕してから第二の攪拌槽に流入して攪拌・溶解する
ことを特徴とするゴム補強スチレン系樹脂原料の製造方
法である。
That is, the present invention is a method for producing a rubber-reinforced styrenic resin raw material by dissolving a reinforcing rubber in a monomer liquid containing a styrene monomer, in which the reinforcing rubber cut in advance is placed in a first stirring tank. The monomer liquid containing undissolved reinforcing rubber is added to the monomer liquid in the tank and stirred, and the undissolved reinforcing rubber contained in the monomer liquid flows out from the bottom of the first stirring tank. This is a method for producing a rubber-reinforced styrenic resin raw material, which is characterized in that rubber is wet-pulverized and then flows into a second stirring tank where it is stirred and dissolved.

以下、本発明の詳細な説明する。The present invention will be explained in detail below.

本発明で用いるスチレン系単量体としては、スチレンの
他に、α−メチルスチレン、p−メチルスチレン、クロ
ルスチレン等の置換スチレンかあり、本発明でいう単量
体液は、スチレン系単量体から選択される1種又は2種
以上の混合物を含むか、好ましくはスチレンを含み、そ
の他、アクリロニトリル、無水マレイン酸、メタクリル
酸メチル等のメタクリル酸誘導体等のスチレン系単量体
と共重合可能な単量体を含んでもよい。また、溶液重合
用の原料の場合、トルエン、キシレン、エチルベンセン
等の溶剤を含む。この場合のスチレン系単量体と溶剤と
の重量比は通常70/30〜9515好ましくは75 
/ 25〜85 / 15である。
In addition to styrene, the styrenic monomer used in the present invention includes substituted styrenes such as α-methylstyrene, p-methylstyrene, and chlorostyrene. It preferably contains styrene and is copolymerizable with styrene monomers such as acrylonitrile, maleic anhydride, and methacrylic acid derivatives such as methyl methacrylate. It may also contain a monomer. In addition, in the case of raw materials for solution polymerization, solvents such as toluene, xylene, and ethylbenzene are included. In this case, the weight ratio of the styrene monomer to the solvent is usually 70/30 to 9515, preferably 75.
/25 to 85/15.

本発明で用いる補強用ゴムとしては、ポリブタジェン、
SBR等があり、その使用量は、通常、補強用ゴムとス
チレン系単量体との重量比が2/98〜15/85とな
る量である。本発明は、高粘度のゴムを補強用ゴムとし
て用いる場合に好適であり、特に25℃で測定した5%
スチレン溶液の粘度が300〜1300センチポイズの
範囲内にあり、ムーニー粘度が80〜l 50 (ML
 1−4゜。。・)の範囲内にあるゴムを用いる場合に
有効である。
The reinforcing rubber used in the present invention includes polybutadiene,
There are SBR and the like, and the amount used is usually such that the weight ratio of reinforcing rubber to styrene monomer is 2/98 to 15/85. The present invention is suitable when a high viscosity rubber is used as a reinforcing rubber, and in particular, 5%
The viscosity of the styrene solution is within the range of 300-1300 centipoise, and the Mooney viscosity is 80-150 (ML
1-4°. . It is effective when using rubber within the range of ・).

本発明では、単量体液に補強用ゴムを効率よく溶解する
ために、攪拌と湿式粉砕とを採用する。
In the present invention, stirring and wet pulverization are employed in order to efficiently dissolve the reinforcing rubber in the monomer liquid.

すなわち、補強用ゴムの溶解を促進するために単量体液
を攪拌する他に、未溶解の補強用ゴムが残存する間に、
未溶解の補強用ゴムを湿式粉砕して溶解し易くする。
That is, in addition to stirring the monomer liquid to promote dissolution of the reinforcing rubber, while the undissolved reinforcing rubber remains,
Wet-pulverize undissolved reinforcing rubber to make it easier to dissolve.

単量体液の攪拌は攪拌翼を備えた攪拌槽で行うことがで
きる。また、補強用ゴムの湿式粉砕は通常の湿式粉砕に
用いている粉砕機を用いることができ、中でも連続的に
湿式粉砕できるものが好ましい。このような粉砕機とし
てトリゴナルタイプの粉砕機、アトリションミル、コロ
イドミル、ピン型ミル等がある。特に、トリゴナルタイ
プの粉砕機はポンプとしての作用も有しており、単量体
液を搬送するために用いるポンプとしてトリゴナルタイ
プの粉砕機を用いることにより、本発明の効果を奏する
ことができるので好ましい粉砕機といえる。本発明にお
いて補強用ゴムの湿式粉砕をトリゴナルポンプを用いて
行う場合、ギャップを0.6mm以下、好ましくは0.
3〜0.5mm程度に調整するのがよい。
The monomer liquid can be stirred in a stirring tank equipped with stirring blades. Further, for wet pulverization of the reinforcing rubber, a pulverizer used for normal wet pulverization can be used, and among them, a pulverizer that can be wet pulverized continuously is preferable. Such crushers include trigonal type crushers, attrition mills, colloid mills, pin type mills, and the like. In particular, a trigonal type crusher also has the function of a pump, and by using a trigonal type crusher as a pump used to convey the monomer liquid, the effects of the present invention can be achieved, so this is a preferable crusher. It can be said. In the present invention, when the reinforcing rubber is wet-pulverized using a trigonal pump, the gap is 0.6 mm or less, preferably 0.6 mm or less.
It is best to adjust it to about 3 to 0.5 mm.

本発明では、粉砕工程の前後に攪拌工程を設けて補強用
ゴムの溶解を行う。具体的には、補強用ゴムを添加した
単量体液の攪拌を二種の攪拌槽で行い、第一の攪拌槽か
ら流出した未溶解の補強用ゴムを含む単量体液を湿式粉
砕してから第二の攪拌槽に流入する。
In the present invention, a stirring process is provided before and after the crushing process to dissolve the reinforcing rubber. Specifically, the monomer liquid containing the reinforcing rubber is stirred in two types of stirring tanks, and the monomer liquid containing the undissolved reinforcing rubber flowing out from the first stirring tank is wet-pulverized. It flows into the second stirring tank.

以下、第1ifflに基づいて本発明を具体的に説明す
る。
Hereinafter, the present invention will be specifically explained based on the first iffl.

第1図は、本発明の実施例の工程を示すフローシートで
ある。攪拌翼(1)を備えた攪拌槽(2)に、攪拌槽(
2)の上部に連通ずる配管(3)を通して単量体液を連
続的に供給するとともに切断機4で5〜10耶程度に切
断した補強用ゴムを攪拌槽(2)の上部から供給する。
FIG. 1 is a flow sheet showing the steps of an embodiment of the present invention. A stirring tank (2) equipped with a stirring blade (1) is provided with a stirring tank (
A monomer liquid is continuously supplied through a pipe (3) communicating with the upper part of the stirring tank (2), and reinforcing rubber cut into approximately 5 to 10 pieces by a cutting machine 4 is supplied from the upper part of the stirring tank (2).

そして、攪拌槽(2)の底部に設けた配管(5)から未
溶解の補強用ゴムを含む単量体液を連続的に流出し、ギ
ャップを0.1〜]、 Itemの範囲で調節できるト
リゴナルポンプ(6)を通すことにより未溶解の補強用
ゴムを湿式粉砕してから攪拌翼(7)を備えた第二の攪
拌槽(8)に攪拌槽(8)の上部に連通する配管(9)
から連続的に流入する。さらに、攪拌槽(8)の底部に
設けた配管(9)から補強用ゴムが完全に溶解した単量
体液を連続的に流出してタンクQO)に流入し貯蔵する
。なお、タンク(10)に貯蔵した単量体液をゴム補強
スチレン系樹脂原料として用いる際には、濾過装置(1
1)を通して不純物を取り除いてから重合工程(12)
に供給する。また、第二の攪拌槽(8)とタンク(10
)との間及びこのタンク(10)と濾過装置(11)と
の間のポンプ(13)はギアポンプである。
Then, the monomer liquid containing undissolved reinforcing rubber is continuously flowed out from the piping (5) provided at the bottom of the stirring tank (2), and a trigonal pump that can adjust the gap in the range of 0.1 to [Item] (6) to wet-pulverize the undissolved reinforcing rubber and then connect the upper part of the stirring tank (8) to the second stirring tank (8) equipped with stirring blades (7) (9)
Continuous inflow from Furthermore, the monomer liquid in which the reinforcing rubber is completely dissolved is continuously flowed out from the pipe (9) provided at the bottom of the stirring tank (8), and flows into the tank QO) for storage. In addition, when using the monomer liquid stored in the tank (10) as a rubber-reinforced styrene resin raw material, the filtration device (10) is used.
After removing impurities through step 1), polymerization step (12)
supply to. In addition, a second stirring tank (8) and a tank (10
) and between this tank (10) and the filtration device (11) are gear pumps.

〔作 用〕[For production]

本発明は、単量体液に補強用ゴムを溶解するに当り、未
溶解の補強用ゴムを湿式粉砕する工程を含むものであり
、未溶解の補強用ゴムは湿式粉砕されることにより単位
量当りの単量体液との接触表面積が広くなり溶解し易く
なるので、攪拌工程のみからなる方法よりも効率良く溶
解できる。
The present invention includes a step of wet-pulverizing the undissolved reinforcing rubber when dissolving the reinforcing rubber in the monomer liquid, and by wet-pulverizing the undissolved reinforcing rubber, the amount per unit amount of the undissolved reinforcing rubber is reduced. Since the surface area of contact with the monomer liquid becomes larger and it becomes easier to dissolve, the monomer can be dissolved more efficiently than a method consisting only of a stirring step.

〔実施例〕〔Example〕

以下、実施例及び比較例に基ついて、本発明を具体的に
説明する。
Hereinafter, the present invention will be specifically explained based on Examples and Comparative Examples.

実施例 第1図に示したフローシートに基づいてゴム補強スチレ
ン系樹脂原料を製造した。単量体液としては、スチレン
とエチルベンセンとを80/20の重量比で混合したも
のを用い、補強用ゴムとしては25℃で測定した5%ス
チレン溶液の粘度か820センチポイズでムーニー粘度
が142(ML++4.1lO−であるポリブタジェン
ゴムを用いた。
EXAMPLE A rubber-reinforced styrenic resin raw material was manufactured based on the flow sheet shown in FIG. The monomer liquid used was a mixture of styrene and ethylbenzene in a weight ratio of 80/20, and the reinforcing rubber had a Mooney viscosity of 142 (820 centipoise), which is the viscosity of a 5% styrene solution measured at 25°C. Polybutadiene rubber with ML++4.11O- was used.

また、攪拌槽(2)への単量体液及び補強用ゴムの供給
は単量体液に含まれるスチレンと補強用ゴムとの重量比
が92/8となるように連続的に行った。
Further, the monomer liquid and the reinforcing rubber were continuously supplied to the stirring tank (2) so that the weight ratio of the styrene contained in the monomer liquid to the reinforcing rubber was 92/8.

なお、第一の攪拌槽(2)及び第二の攪拌槽(8)での
単量体液の滞留時間はそれぞれ4時間とし、トリゴナル
ポンプ(6)のギャップは0,4市とした。
The residence time of the monomer liquid in the first stirring tank (2) and the second stirring tank (8) was 4 hours each, and the gap between the trigonal pump (6) was 0.4 hours.

タンク00)内でのゴム状物質の沈澱や、濾過装置01
)での目詰まり等の問題はなく、濾過装置(11)も含
めて3ケ月間以上安定して連続運転できた。
Sedimentation of rubbery substances in tank 00) and filtration device 01
) There were no problems such as clogging, and stable continuous operation including the filtration device (11) was possible for more than three months.

比較例 トリゴナルポンプ(6)に替えて粉砕作用のないギヤポ
ンプを用いた他は実施例と同様にした。−週間後、タン
ク00)内を目視で観察したところ、底部にゴム状物質
か沈澱していた。その状態で、タンク00)から単量体
液を流出して濾過装置(11)で濾過したところ3時間
で目詰まりし、運転を続行することができなかった。
Comparative Example The procedure was the same as in the example except that a gear pump without a crushing action was used in place of the trigonal pump (6). After - weeks, the inside of tank 00) was visually observed, and a rubbery substance had precipitated at the bottom. In this state, when the monomer liquid flowed out from the tank 00) and was filtered through the filtration device (11), it became clogged in 3 hours and the operation could not be continued.

〔発明の効果〕〔Effect of the invention〕

本発明によれば、補強用ゴムを単量体液に効率よく溶解
できるので、安定した特性を有するゴム補強用スチレン
系樹脂原料を長期間に亘って連続して製造することがで
きる。
According to the present invention, since the reinforcing rubber can be efficiently dissolved in the monomer liquid, it is possible to continuously produce a styrenic resin raw material for rubber reinforcing having stable characteristics over a long period of time.

【図面の簡単な説明】[Brief explanation of the drawing]

第1図は、本発明の実施例の工程を示すフローシートで
ある。 符号の説明 (2)・・・第一の攪拌槽、  (4)・・・切断機、
(6)・・・トリゴナルポンプ、(8)・・・第二の攪
拌槽、00)・・・タンク、     OD・・・濾過
装置。 特許出願人   新日鐵化学株式会社
FIG. 1 is a flow sheet showing the steps of an embodiment of the present invention. Explanation of symbols (2)...first stirring tank, (4)...cutting machine,
(6)... Trigonal pump, (8)... Second stirring tank, 00)... Tank, OD... Filtration device. Patent applicant: Nippon Steel Chemical Co., Ltd.

Claims (4)

【特許請求の範囲】[Claims] (1)スチレン系単量体を含む単量体液に補強用ゴムを
溶解してゴム補強スチレン系樹脂原料を製造する方法で
あって、予め切断した補強用ゴムを第一の攪拌槽内の単
量体液に添加して撹拌し、該第一の攪拌槽の底部から未
溶解の補強用ゴムを含む単量体液を流出し、該単量体液
に含まれている未溶解の補強用ゴムを湿式粉砕してから
第二の攪拌槽に流入して撹拌・溶解することを特徴とす
るゴム補強スチレン系樹脂原料の製造方法。
(1) A method for producing a rubber-reinforced styrenic resin raw material by dissolving reinforcing rubber in a monomer liquid containing a styrene monomer, in which pre-cut reinforcing rubber is placed in a monomer liquid in a first stirring tank. The monomer liquid containing undissolved reinforcing rubber flows out from the bottom of the first stirring tank, and the undissolved reinforcing rubber contained in the monomer liquid is wet-mixed. A method for producing a rubber-reinforced styrenic resin raw material, which comprises pulverizing the material and then flowing it into a second stirring tank where it is stirred and dissolved.
(2)湿式粉砕をトリゴナル、アトリションミル、コロ
イドミル及びピン型ミルから選ばれた粉砕機で行う請求
項1記載のゴム補強スチレン系樹脂原料の製造方法。
(2) The method for producing a rubber-reinforced styrenic resin raw material according to claim 1, wherein the wet pulverization is carried out using a pulverizer selected from trigonal, attrition mill, colloid mill, and pin type mill.
(3)補強用ゴムと単量体液中のスチレン系単量体との
重量比が2/98〜15/85である請求項1又は2記
載のゴム補強スチレン系樹脂原料の製造方法。
(3) The method for producing a rubber-reinforced styrenic resin raw material according to claim 1 or 2, wherein the weight ratio of the reinforcing rubber to the styrene monomer in the monomer liquid is from 2/98 to 15/85.
(4)補強用ゴムが、25℃で測定した5%スチレン溶
液の粘度が300〜1300センチポイズでムーニー粘
度が80〜150(ML_1_+_4_、_1_0_0
_c^*)である請求項1〜3のいずれかに記載のゴム
補強スチレン系樹脂原料の製造方法。
(4) The reinforcing rubber has a viscosity of 300 to 1300 centipoise of a 5% styrene solution measured at 25°C and a Mooney viscosity of 80 to 150 (ML_1_+_4_, _1_0_0
_c^*) The method for producing a rubber-reinforced styrenic resin raw material according to any one of claims 1 to 3.
JP24878190A 1990-09-20 1990-09-20 Method for producing rubber-reinforced styrene resin raw material Expired - Lifetime JPH0794510B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP24878190A JPH0794510B2 (en) 1990-09-20 1990-09-20 Method for producing rubber-reinforced styrene resin raw material

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP24878190A JPH0794510B2 (en) 1990-09-20 1990-09-20 Method for producing rubber-reinforced styrene resin raw material

Publications (2)

Publication Number Publication Date
JPH04130111A true JPH04130111A (en) 1992-05-01
JPH0794510B2 JPH0794510B2 (en) 1995-10-11

Family

ID=17183298

Family Applications (1)

Application Number Title Priority Date Filing Date
JP24878190A Expired - Lifetime JPH0794510B2 (en) 1990-09-20 1990-09-20 Method for producing rubber-reinforced styrene resin raw material

Country Status (1)

Country Link
JP (1) JPH0794510B2 (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0870787A1 (en) * 1997-04-08 1998-10-14 Toyo Engineering Corporation Method of continuously dissolving rubber

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0870787A1 (en) * 1997-04-08 1998-10-14 Toyo Engineering Corporation Method of continuously dissolving rubber
US5929205A (en) * 1997-04-08 1999-07-27 Toyo Engineering Corporation Method of continuously dissolving rubber
KR100352015B1 (en) * 1997-04-08 2002-11-22 도요엔지니어링 코포레이션 Continuous dissolution of rubber
CN1109690C (en) * 1997-04-08 2003-05-28 东洋工程公司 Method of continuously dissolving rubber

Also Published As

Publication number Publication date
JPH0794510B2 (en) 1995-10-11

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