# US 5,708,098 A · Method of preparing solventless, thermoplastic silicone pellets and the pellets so-produced

> Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt

- Number: US 5,708,098 A
- Document ID: US5708098A
- Status: Granted
- Kind: A
- Application number: 08/705,106
- Filed: 1996-08-28
- Granted: 1998-01-13
- Earliest claimed: 1996-08-28
- Assignees: Dow Corning Corporation
- Inventors: Leon Neal Cook; Richard Allen Hessick, Jr.; Kevin Edward Lupton; David Joseph Romenesko; Randall Gene Schmidt; Hongxi Zhang
- Web page: https://patentgrep.com/patent/US5708098A

## CPC

- C08J 3/12: Powdering or granulating
- B29B 9/12: characterised by structure or composition
- B29C 48/00: Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor (extrusion blow-moulding B29C49/04)
- B29C 48/04: Particle-shaped (making granules B29B9/00)
- B29K 2083/00: Use of polymers having silicon, with or without sulfur, nitrogen, oxygen, or carbon only, in the main chain, as moulding material
- C08J 2383/04: Polysiloxanes
- C08J: WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H (working, e.g. shaping, of plastics B29)
- B29B: PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B29C: SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING (making preforms B29B11/00; making laminated products by combining previously unconnected layers which become one product whose layers will remain together B32B37/00 - B32B41/00)
- B29K: INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR {MOULDS, } REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS

## Abstract

Solventless, thermoplastic silicone pellets are prepared blending silicone resins (A) of the MQ-type and with predominantly linear silicone fluids (B), such as polydimethylsiloxane liquids and gums, to substantially homogeneity. The blends are heated to a predetermined compression-forming temperature, compression-formed to a densified mass and shaped into a pellet form. The composition of the pellets is balanced such that the pellets exhibit plastic flow at the predetermined compression-forming temperature and resist agglomeration at temperatures at or below a predetermined maximum storage temperature.

## Claims

### Claim 1

A method of preparing solventless, thermoplastic silicone pellets, which pellets resist agglomeration at temperatures less than a predetermined maximum storage temperature, said method comprising the steps of:
(I) blending:
(A) an organosilicone resin of the empirical formula
(R.sub.3 SiO.sub.1/2).sub.a (R.sub.2 SiO.sub.2/2).sub.b (RSiO.sub.3/2).sub.c (SiO.sub.4/2).sub.d
wherein: a and d are or positive numerical values and b and c are zero or positive numerical values with the provisos that a+b+c+d=1, 0.ltoreq.(b+c).ltoreq.0.2; and R is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R groups may be the same or different, with the proviso that at least sixty mole percent of said R radicals are methyl;
said organosilicone resin (A) having a number average molecular weight (Mn) between about 2,000 and about 15,000; and
(B) a predominantly linear silicone fluid having the empirical formula
(R'.sub.3 SiO.sub.1/2).sub.x (R'.sub.2 SiO.sub.2/2).sub.y (R'SiO.sub.3/2).sub.z
wherein: x and y are positive numerical values and z is 0 or a positive numerical value with the provisos that x+y+z=1, y/(x+y+z).gtoreq.0.8; and R' is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R' groups may be the same or different, with the proviso that at least sixty mole percent of said R' radicals are methyl;
said predominantly linear silicone fluid having a degree of polymerization greater than about 10;
said blending step (I) being carried out to form a substantially homogenous mixture of components (A) and (B);
(II) heating the substantially homogeneous mixture of components (A) and (B) to a predetermined compression-forming temperature;
(III) compression-forming said heated mixture of components (A) and (B) at said compression-forming temperature to form a densified mass therefrom;
(IV) shaping said densified mass into the form of a pellet; and
(v) cooling said densified mass to a temperature less than said predetermined maximum storage temperature;
said organosilicone resin (A) and said predominantly linear silicone fluid (B) being present in relative amounts such that: said substantially homogeneous mixture of components (A) and (B) has a complex viscosity (.eta.*) less than 10.sup.8 centipoise at said predetermined compression-forming temperature; and said pellets have a dynamic shear modulus (G*), measured at a frequency of 10 radians/sec, of at least 5.times.10.sup.7 dyne/cm.sup.2 at temperatures less than said predetermined maximum storage temperature.

### Claim 2 (depends on 1)

A method in accordance with claim 1 wherein said predetermine maximum storage temperature is between about 0.degree. C. and 50.degree. C.

### Claim 3 (depends on 2)

A method in accordance with claim 2 wherein said predominantly linear silicone (B) has a degree of polymerization in excess of about 100.

### Claim 4 (depends on 2)

A method in accordance with claim 2 wherein said predominantly linear silicone (B) is a gum.

### Claim 5 (depends on 2)

A method in accordance with claim 2 wherein said predetermined maximum storage temperature is about 25.degree. C. and said organosilicone resin (A) and said predominantly linear silicone fluid (B) are present in relative amounts such that the ratio of the weight of resin (A):fluid (B) is between about 2.3:1 and 4:1.

### Claim 6 (depends on 1)

A method in accordance with claim 1 wherein said organosilicone resin (A) and said predominantly linear silicone fluid (B) are present in relative amounts such that said pellets have a dynamic shear modulus (G*), measured at a frequency of 10 radians/sec, of less than 10.sup.9 dyne/cm.sup.2 at said predetermined maximum storage temperature.

### Claim 7 (depends on 1)

A method in accordance with claim 1 wherein said predetermined compression-forming temperature is between about 50.degree. C. and 200.degree. C.

### Claim 8 (depends on 1)

A method in accordance with claim 1 further comprising: said blending step (I) including the step of dissolving said organosilicone resin (A) and said predominantly linear silicone fluid (B) in a co-solvent; and the additional step of removing said co-solvent from said substantially homogeneous mixture prior to said compression-forming step (III).

### Claim 9 (depends on 8)

A method in accordance with claim 8 wherein said co-solvent is an organic aromatic solvent.

### Claim 10 (depends on 8)

A method in accordance with claim 8 wherein said co-solvent is hexamethyldisiloxane.

### Claim 11 (depends on 1)

A method in accordance with claim 1 wherein said compression-forming step (III) is carried out in a mold.

### Claim 12 (depends on 11)

A method in accordance with claim 11 wherein said compression-forming step (III) and said shaping step (IV) are carried out in a mold.

### Claim 13 (depends on 1)

A method in accordance with claim 1 wherein said heating step (II) and said compression-forming step (III) are carried out with an extrusion apparatus, said densified mass exiting said apparatus as an extrudate.

### Claim 14 (depends on 13)

A method in accordance with claim 13 further comprising: said blending step (I) including the step of dissolving said organosilicone resin (A) and said predominantly linear silicone fluid (B) in a co-solvent; and the additional step of removing said co-solvent from said substantially homogeneous mixture prior to said compression-forming step (III), said co-solvent blending step (I) and said additional co-solvent removing step being carried out in an extrusion apparatus having vacuum ports formed therein.

### Claim 15 (depends on 13)

A method in accordance with claim 13 wherein said shaping step (IV) is carried out by a cutting said extrudate with a reciprocating knife blade.

### Claim 16 (depends on 1)

A method in accordance with claim 1 wherein said organosilicone resin (A) has a number average molecular weight (Mn) between about 3,000 and about 7,000.

### Claim 17 (depends on 1)

A silicone pellet prepared by the method of claim 1.

### Claim 18

A plurality of solventless, thermoplastic silicone pellets, which pellets resist agglomeration at temperatures less than about 25.degree. C., said pellets having a formulation comprising:
(A) 23 to 40 parts, by weight, of an organosilicone resin of the empirical formula
(R.sub.3 SiO.sub.1/2).sub.a (R.sub.2 SiO.sub.2/2).sub.b (RSiO.sub.3/2).sub.c (SiO.sub.4/2).sub.d
wherein: a and d are or positive numerical values and b and c are zero or positive numerical values With the provisos that a+b+c+d=1, 0.ltoreq.(b+c).ltoreq.0.2 and the ratio of a:(b+c+d) is between about 0.3 and 1.0; and R is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R groups may be the same-or different, with the proviso that at least sixty mole percent of said R radicals are methyl;
said organosilicone resin (A) having a number average molecular weight (Mn) between about 2,000 and about 7,000;
(B) about 10 parts, by weight of a predominantly linear silicone fluid having the empirical formula
(R'.sub.3 SiO.sub.1/2).sub.x (R'.sub.2 SiO.sub.2/2).sub.y (R'SiO.sub.3/2).sub.z
wherein: x and y are positive numerical values and z is 0 or a positive numerical value with the provisos that x+y+z=1, y/(x+y+z).gtoreq.0.8; and R' is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R' groups may be the same or different, with the proviso that at least sixty mole percent of said R' radicals are methyl;
said predominantly linear silicone fluid (B) having a degree of polymerization greater than about 10; and
said pellets having a dynamic shear modulus (G*), measured at a frequency of 10 radians/sec, of at least 5.times.10.sup.7 dyne/cm.sup.2 at temperatures less than about 25.degree. C.

### Claim 19 (depends on 18)

A plurality of solventless, thermoplastic silicone pellets in accordance with claim 18, said predominantly linear silicone fluid having a degree of polymerization in excess of 100.

### Claim 20 (depends on 18)

A plurality of solventless, thermoplastic silicone pellets in accordance with claim 18, said predominantly linear silicone fluid being a gum.

### Claim 21

A plurality of solventless, thermoplastic silicone pellets, which pellets resist agglomeration at temperatures less than a predetermined storage temperature, said pellets having a formulation comprising:
(A) an organosilicone resin of the empirical formula
(R.sub.3 SiO.sub.1/2).sub.a (R.sub.2 SiO.sub.2/2).sub.b (RSiO.sub.3/2).sub.c (SiO.sub.4/2).sub.d
wherein: a and d are or positive numerical values and b and c are zero or positive numerical values with the provisos that a+b+c+d=1, 0.ltoreq.(b+c).ltoreq.0.2; and R is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R groups may be the same or different, with the proviso that at least sixty mole percent of said R radicals are methyl;
said organosilicone resin (A) having a number average molecular weight (Mn) between about 3,000 and about 7,000; and
(B) a predominantly linear silicone fluid having the empirical formula
(R'.sub.3 SiO.sub.1/2).sub.x (R'.sub.2 SiO.sub.2/2).sub.y (R'SiO.sub.3/2).sub.z
wherein: x and y are positive numerical values and z is 0 or a positive numerical value with the provisos that x+y+z=1, y/(x+y+z).gtoreq.0.8; and R' is a monovalent radical independently selected from the group consisting of hydrogen, hydroxyl, alkyl, alkenyl, alkoxy, oximo, aryl, epoxide, carboxyl, ether, polyether, amide and alkyl amino radicals, which R' groups may be the same or different, with the proviso that at least sixty mole percent of said R' radicals are methyl;
said predominantly linear silicone fluid having a degree of polymerization greater than about 10;
said organosilicone resin (A) and said predominantly linear silicone fluid (B) being present in relative amounts such that said pellets have a dynamic shear modulus (G*), measured at a frequency of 10 radians/sec, of at least 5.times.10.sup.7 dyne/cm.sup.2 at temperatures less than said predetermined maximum storage temperature.

### Claim 22 (depends on 21)

A plurality of solventless, thermoplastic silicone pellets in accordance with claim 21 wherein said organosilicone resin (A) and said predominantly linear silicone fluid (B) are present in relative amounts such that said pellets have a dynamic shear modulus (G*), measured at a frequency of 10 radians/sec, of less than 10.sup.9 dyne/cm.sup.2 at said predetermined maximum storage temperature.