Thermoplastic resin, process for producing same and...

Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...

Reexamination Certificate

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C525S241000, C525S390000, C525S391000, C525S393000, C528S038000, C528S043000, C528S041000, C528S025000, C528S029000, C568S608000, C568S852000

Reexamination Certificate

active

06414091

ABSTRACT:

FIELD OF THE INVENTION
The present invention relates to a thermoplastic resin, a process for producing such a thermoplastic resin and a thermoplastic resin composition. More specifically, the present invention relates to (i) a thermoplastic resin capable of giving a thermoplastic resin composition, which composition can exhibit a superior flame resisting property and superior mechanical properties without use of any flame retardant such as a halogen-containing flame retardant and a phosphorus-containing flame retardant, (ii) a process for producing such a thermoplastic resin, and (iii) the above-mentioned thermoplastic resin composition.
BACKGROUND OF THE INVENTION
A kind of flame retardant such as a halogen-containing flame retardant, a phosphorus-containing flame retardant and a metal hydroxide flame retardant have been extensively used as a flame retardant in order to give a flame resisting property to a thermoplastic resin.
However, the flame retardant such as a halogen-containing flame retardant and a phosphorus-containing flame retardant may give undesirable influences to the environment. And the metal hydroxide flame retardant has a problem that said retardant has to be used in a large amount in order to give a sufficient flame resistance to a thermoplastic resin, and as a result, the resulting thermoplastic resin composition is remarkably deteriorated in its mechanical properties.
As a flame retardant different from those mentioned above, U.S. Pat. Nos. 5,169,887 and 5,294,655 disclose a certain kind of polyorganosiloxane compound. More specifically, U.S. Pat. No. 5,169,887 discloses a flame resisting composition comprising a polyphenylene ether resin and a liquid straight chain phenylsiloxane, and U.S. Pat. No. 5,294,655 discloses another flame resisting composition comprising a polyphenylene ether resin, a liquid straight chain phenylsiloxane and a block copolymer elastomer. Each of these references referred to above is incorporated herein by reference in its entiety.
Although the compositions disclosed in said U.S. Patents are superior in their flame resistance to that of the polyphenylene ether resin per se, it is difficult to say that said compositions have a satisfactory flame resistance.
SUMMARY OF THE INVENTION
Accordingly, it is an object of the present invention to provide a thermoplastic resin capable of giving a thermoplastic resin composition, which composition can exhibit a superior flame resisting property and superior mechanical properties without use of any flame retardant such as a halogen-containing flame retardant and a phosphorus-containing-flame retardant.
It is another object of the present invention to provide a process for producing said thermoplastic resin.
It is a further object of the present invention to provide a thermoplastic resin composition superior in its flame resisting property and its mechanical properties.
The present inventors have undertaken extensive studies to develop a flame retardant, which does not give undesirable influences to the environment, and which is capable of giving a superior flame resistance to a thermoplastic resin without remarkable detriment to the mechanical properties of the thermoplastic resin. As a result, it has been found that a thermoplastic resin obtained by a reaction between a polyphenylene ether resin and a specific polyorganosiloxane is a superior flame retardant capable of giving a superior flame resisting property. Thereby, the present invention has been obtained.
The present invention provides a thermoplastic resin (X-1) obtained by a process comprising the step of reacting:
(1) a polyphenylene ether resin (A) with
(2) a polyorganosiloxane (B),
wherein the polyorganosiloxane (B) comprises:
(i) at least one functional group selected from the group consisting of amino, epoxy, hydroxyl, phenol, carboxyl, amide, methacryloyl, vinyl, alkoxy, carbonyl and imino groups, and
(ii) respective structure units represented by the following formulas (I), (II) and (III), provided that a molar ratio of the structure unit (I) to the structure unit (II), namely structure unit (I)/structure unit (II), is from 0.1 to 10
R
1
R
2
SiO
1.0
  (I)
R
3
SiO
1.5
  (II)
R
4
R
5
R
6
SiO
0.5
  (III)
wherein R
1
, R
2
and R
3
are independently of one another an alkyl group having 1 to 3 carbon atoms or an aryl group having 6 to 10 carbon atoms, and R
4
, R
5
and R
6
are independently of one another an alkyl group having 1 to 6 carbon atoms, an aryl group having 6 to 12 carbon atoms, an alkoxy group having 1 to 6 carbon atoms or a hydroxyl group.
The present invention also provides a thermoplastic resin (X-2) obtained by a process comprising the step of reacting:
(1) a polyphenylene ether resin (A), with
(2) a polyorganosiloxane (B) and
(3) a coupling agent (C),
wherein the polyorganosiloxane (B) comprises:
(i) at least one functional group selected from the group consisting of amino, epoxy, hydroxyl, phenol, carboxyl, amide, methacryloyl, vinyl, alkoxy, carbonyl and imino groups, and
(ii) respective structure units represented by the above-defined formulas (I), (II) and (III), provided that a molar ratio of the structure unit (I) to the structure unit (II), namely structure unit (I)/structure unit (II), is from 0.1 to 10.
The present invention further provides a process for producing a thermoplastic resin (X-1), which comprises the step of reacting:
(1) a polyphenylene ether resin (A) with
(2) a polyorganosiloxane (B),
wherein the polyorganosiloxane (B) comprises:
(i) at least one functional group selected from the group consisting of amino, epoxy, hydroxyl, phenol, carboxyl, amide, methacryloyl, vinyl, alkoxy, carbonyl and imino groups, and
(ii) respective structure units represented by the above-defined formulas (I), (II) and (III), provided that a molar ratio of the structure unit (I) to the structure unit (II), namely structure unit (I)/structure unit (II), is from 0.1 to 10.
The present invention still further provides a process for producing a thermoplastic resin (X-2), which comprises the step of reacting:
(1) a polyphenylene ether resin (A) with
(2) a polyorganosiloxane (B) and
(3) a coupling agent (C),
wherein the polyorganosiloxane (B) comprises:
(i) at least one functional group selected from the group consisting of amino, epoxy, hydroxyl, phenol, carboxyl, amide, methacryloyl, vinyl, alkoxy, carbonyl and imino groups, and
(ii) respective structure units represented by the above-defined formulas (I), (II) and (III), provided that a molar ratio of the structure unit (I) to the structure unit (II), namely structure unit (I)/structure unit (II), is from 0.1 to 10.
The present invention additionally provides a thermoplastic resin composition (Z-1) comprising:
(i) the above-defined thermoplastic resin (X-1) and
(ii) a thermoplastic resin (D).
The present invention still additionally provides a thermoplastic resin composition (Z-2) comprising:
(i) the above-defined thermoplastic resin (X-2) and
(ii) a thermoplastic resin (D).
In the present invention, the thermoplastic resin (X-1) and the thermoplastic resin (X-2) are hereinafter together referred to as “thermoplastic resin (X)”, and the thermoplastic resin composition (Z-1) and the thermoplastic resin composition (Z-2) are also hereinafter together referred to as “thermoplastic resin composition (Z)”.
DETAILED DESCRIPTION OF THE INVENTION
The “polyphenylene ether resin (A)” used in the present invention means a (co)polymer resin obtained by oxidatively polymerizing at least one phenol compound represented by the following formula (IV) with oxygen or an oxygen-containing gas with the aid of an oxidative coupling catalyst,
wherein R
7
,R
8
,R
9
,R
10
and R
11
are independently of one another a hydrogen atom, a halogen atom, a hydrocarbon group or a substituted hydrocarbon group, provided that at least one of them is always a hydrogen atom.
Examples of R
7
,R
8
,R
9
,R
10
and R
11
in the formula (IV) are hydrogen, chlorine, bromine, fluorine, iodine, methyl, ethyl, n-propyl, iso-propyl, pri-butyl, sec-butyl, t-butyl, hydroxyethyl,

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