CA2069861A1 - Processes for preparing polymer composites based cellulose - Google Patents

Processes for preparing polymer composites based cellulose

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Publication number
CA2069861A1
CA2069861A1 CA 2069861 CA2069861A CA2069861A1 CA 2069861 A1 CA2069861 A1 CA 2069861A1 CA 2069861 CA2069861 CA 2069861 CA 2069861 A CA2069861 A CA 2069861A CA 2069861 A1 CA2069861 A1 CA 2069861A1
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agents
bonding agent
process according
organic material
group
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CA 2069861
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French (fr)
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Alphons D. Beshay
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Abstract

ABSTRACTS

Polymer composites based cellulose prepared by admixing finely organic filler with ground polymeric material of thermoplastic or rubber without using hot-melting compounding machinery. Those composites are shaped into articles directly through processing plastic or rubber machines.

Description

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"PROCESSES EOR PREPARING POLYMER COMPOSITES BASED CELLULOSE"

BACKGKOUND OF THE INVENTION

This invention is a continuation-in-part of Beshay's U.S. Pat. Nos. 4,717,742, 4,820,749 & 5,008,310; CA Pat.
Nos. 1,252,586 and 1,269,187 and the U.S. Pat. Application Nos. 07/229,844, 07/779,946 and 07/828,357 and U.K. Pat.

Application No. 2,205,569.
(1) Field of the Invention:

This invention relates to polymer composites based cellulose. More particularly, this invention relates to the processes for preparing composite materials made from polymers, or copolymers, or rubber, and treated cellulosic fibers with a bonding agent.
(2) Description of Prior Art:

The published literatures include a number of proposals, which essentially consist of thermoplastic resinous matrix having dispersed therein cellulosic fillers mixed or not with inorganic fillers. Such materials are described as per the following examples.

- U~S. Pat. No. 3,485,777, 1969, Gaylord, deals with compatibilization of polyvinylchloride or polymethylmetha-crylate with grafted cellulose.

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- ``, ' '' ' ' ' ' ' ' ' - U.S. Pat. No. 3,645,939, also shows that polyethylene or polyvinyl chloride or acryloc rubber can be compatibilized with cellulosic fibers, in presence of an ethylenically un-saturated carboxylic acid or anhydride, under conditions which generate free radicals on said polymers and celluloses.

- U.K. Pat. Application No. 2,090,849, Hishida, I., prepared composites from thermoplastic resins by compatibi-lizing flax fibers coated with a surface treating agent, such as silanes, titanates..etc., in absence of a free radical initiator.

- U.S. Pat. No. 4,554,215, Robbart, made composites coated with alkylhalogeno-silane, also in absence of an initiator.

- U.S. Pat. No. 4,374,178, Kulkarni, prepared composites by filling with calcium carbonate, or sodium silicate, and a microcrystalline cellulose as a carrier by coating with silane bonding agent.

- EP. Pat. No. 0008143, Solvay & Cie and the Japanese Pat. No. 8011-537, Showa, both teach the application of organic and inorganic fillers in presence of a peroxide and an acid anhydride. Resulting composite materials were relatively having little improvements in their mechanical strengths.

- J 5 Pat. No. 7192-466, Showa, teaches the addition of an unsaturated silane coupling agent onto the polyolefin matrix, by the effect of a catalytic peroxide and then by ~ .~

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2069~1 adding wood flour as a filler. But, silylating the matrix lead to consume more silane than in case of silylating the filler itself. Furthermore, the composite performances were not highly improved.

In summary, we believe to be the first one to prepare polymer composites based cellulose by following different compounding processes, The cellulosic fibers, or starch are treated with a bonding agent and, optionally, with a small guantity of polymerizable functional monomer, or oligomer, which could be grafted as per Beshay's said U.S. Pat. Ap-plication No. 07/828,357. Those processes are characterized by having cost, time and machinery savings.

SUMMARY OF THE INVENTION

An object of the current invention is to provide a polymeric or copolymeric material of thermoplastic or thermo-setting or rubber.

Another object of the current invention is to provide the treatment of said cellulosic fibers by coating, bonding or grafting with a bonding agent and, optionally, with a poly-merizable monomer or oligomer thereof. Said treated cellulosic fibers are optionally substituted or mixed or admixed with starch, whether treated or not with said bonding agents and, also optionally, with polymerizable monomer or oligomer thereof.

Furthermore, the inorganic material(s), whether treated or not, . , - . . ..
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hybridized or not with a bonding agent and/or with a polymerizable monomer, or oligomer thereof, are optionally mixed or admixed with said treated cellulosic fibers or starch. One of the following processes can be applied for said treated cellulosic fibers or starch, admixed or not with the said inorganic fillers, to be mixed, admixed or compounded with a matrix of thermoplastics-~r:rubbers, wherein such matrix may be precompounded or not with at least one ingredient:

1. Admixing pre-finely granulated two components of said organic filler and said resin together, whether compounded or not 2. Adhering polymeric or copolymeric films or sheets with flat surfaced materials.

DETAILED DESCRIPTION OF THE IN~ENTION

An organic material is selected from the group consisting of short or continuous cellulosic or lignocellulosic fibers or starch. Said selected organic material is provided to be coated or grafted with a bonding agent by any effective process and, optionally, furtherly coated or grafted with a polymerizable monomer or oligomer thereof. Said treated organic material is mixed or admixed with polymeric or co-polymeric thermoplastic material or rubber, which may be compounded with at least one ingredient.

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The organic material used in the current invention includes starch or short, or continuous cellulosic or lignocellulosic fibers,and may be mixed or admixed with inorganic filler material before or after the treating steps. The cellulosic and lignocellulosic fibers are derived from soft wood and/or hard wood pulps, e.g. mecha-nical pulp, chemical or chemi-mechanical or refiner or stone ground wood or thermo-mechanical or chemi-thermo-mechanical or explosion or low yield or high yield or ultra high yield pulp, nut shells, corn cobs, rice, hulls, vegeta-ble fibers, certain bamboo-type reeds, grasses, bagasse" cotton, rayon (regenerated cellulose), sawdust, wood flour, wood shavings, jute, linen or flax and the like. Said organic material could be mixed or admixed with inorganic material selected from the group consisting of a compound containing hydroxyl group, clay, calcium carbonate, asbestos, sand, wollastonite, quartz, glass, mica, diatomaceous earth, silica, talc, caolinite, hydrated or partially hydrated metal oxide, metal powders or metal fibers, or metal compounds, ceramic fibers, carbon, graphite, synthetic or naturally occurring material and if naturally occurring, they could be used in either purified or unpurified form. Said inorganic material could be treated or hybridized with a bonding agent before, during or after the mixing or admixing step with the said organic material. Also, more than one kind of inorganic , . . . . .
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material can be mixed or admixed with the said organic material.

Said organic or inorganic material could be in the form of powder, crystals, fibers, particles, sheets, papers, cartons, threads, cloths, chips, pannels, boards, preshaped forms or articles. Those organic and inorganic materials could be bonded or coated with grafted wax as per the U.S.
Pat. Application No. 07/779,946.

The bonding agents used in the current invention are organo-silicon compounds, isocyanate bonding agents, stearate bonding agents, zirconate bonding agents, titanate bonding agents, alu~inate bonding agents, alumino-zirconate bonding agents or the like.

Those treated cellulosic or lignocellulosic fibers or starch could be furtherly and op~ionally coated, bonded or grafted with polymerizable monomer or oligomer thereof.
Thc.se polymerizable monomers or oligomers thereof are as per the CA Pat. No. 1,269,187.

Those said treated organic materiala,whether mixed or admixed or not with treated or non-treated inorganic materials are mixed, admixed or compounded with a matrix of thermoplastics or rubbers, wherein such matrix may be precompounded or not with at least one ingredient.

Those polymeric or copolymeric thermoplastics or rubbers, whether compounded or not, are as mentioned per the U.S. Pat.

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No. 5,008,310, providing if compounded to be with at least one ingredient.

Those ingredients are such as the treated or untreated inorganic fillers, carbon black, graphite, metallic fibers or powders, ceramic fibers; bonding agents, dispersing agents, plasticizers or other additives which could be among those said ingredients, are also mentioned in the U.S.Pat. No.
5,008,310, and the U.S. Pat. Application Nos. 07/779,946 &
07/828,357.

The current invention deals with the processes for pre-paring said composite materials based cellulose. Such pro-cesses are as follows:

l.a) Grinding a certain amount of dried organic material selected from cellulosic or lignocellulosic fibers at a proper mesh size, to be mixed or not with a certain weight ratio of said inorganic material.

b) Coating said organic material prepared in a) by a bonding agent,whether or not dissolved in a solvent, or subject-ing said material of a) to be grafted with a bonding agent as per the U.S. Pats.No. 4,820,749, or 5,008,310, or cografted as per the CA Pat. No. 1,269,187; or c) Bonding said organic material prepared in a), either by spraying, wetting, coating or admixing with a grafted wax with a bonding agent, prepared according to the U.S. Pat. Application No. 07/779,946.

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d) Mechanical mixing or admixing a certain weight ratio of the organic material prepared as per b) or c) with another certain weight ratio of preground polymeric or copolymeric thermoplastic or rubber, whether precom-pounded with at least one ingredient or not. Said mixing or admixing is to exclude passing through heat-melting compounding machinery.

The finally ground treated organic filler prepared ac-cording to b) or c) regularly surrounds the ground particles of said thermoplastic or rubber materials by the effect of the electrostatic forces to give said composite materials.

e) Preparing articles from the composites obtained ~rom d) by compression moulding, injection moulding, extrusion moulding, extrustion sheeting or film extrusion.

2.a) Preparing the filler as per l.a).
b) Treating the filler as per l.b).

c) Treating the filler as per l.c).

d) Compounding the filler obtained from b) or c) by using compounding machinery, with compounded polymeric or copolymeric thermoplastic or rubber materials. Said compounded materials are compounded with at least one ingredient. Said compounding is provided to be carried out while the said matrix is hot-molten.

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e) Preparing articles as per l.e).
3.a) Preparing flat surface materials such as wood boards, wood lumbers, textile fabrics, cartons or papers.

b) Treating the surfaces of those materials as per the processes Nos. l.b) or c).

c) Adhering said treated materials obtained from 3.b) with films or sheets of compounded or not compounded polymeric or copolymeric thermoplastics or rubbers by hot-pressing or laminating processes.

EXAMPLES:

The experimentation results in the examples of the invention could be improved or be reached their optimum values by changing the preparation conditions, and/or the weight percentages of the applied materials or the substances.
This invention will now be furtherly described by non-limiting examples.

STEP A.:

20 g of dry and ground at mesh 60 of semichemical pulp of bagasse, chemical thermomechanical wood pulp of aspen or birch were placed in a beaker of 500 ml. capacity. A mixture of 0.16g dicumyl peroxide, 0.2g maleic anhydride and 0.2, 0.4 or 0.8g of gamma-amino-propyltriethoxysilane, gamma-methacryloxy-propyltrimethoxysilane or propyltriethoxysilane were well dissolved together in 15ml acetone as a solvent and were added by spraying to the pulp while stirring. The stirring ,., ' , .
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continued for another 5 minutes. The beaker contents were then subjected to a warm air current for 10 minutes.

STEP B.:
Treating chemical thermomechanical wood pulp derived from aspen with 5% of its weight with grafted wax with gamma-amino-propyltriethoxysilane (A-1100) prepared as per the U.S. Pat.
Application No. 07/779,946.

STEP C.:
Finally grinding linear low density polyethylene (LLDPE), polypropylene (PP), polyvinylchloride (PVC), compounded linear low density polyethylene with carbon black (CLL~PE), compounded PVC with carbon black (CPVC)& compounded polypropylene with calcium carbonate (CaPP).

STEP D.:
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Mechanical admixing of one of the fillers prepared as per Step A or B, with one of the resins o. Step C., to give admixed composites for moulding and testing.

STEP E.:
Hot-molten compounding of one of the compounded resins of Step C, with one of the fillers prepared as per Step A or ~, by using a compounding machine such as a brabender.

STEP F.:

Moulding the resulted composites obtained from Step D or Step E for testing according to ASTM standard D 1822-79, which comprises energy (KJ), stress (MPa) & Modulus (MPa).

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2069~61 The following examples are prepared from the previous steps and are as follows:

Ex- Employed Filler Employed Resin Mixing ._ _ _ , .
No. Step Treating Method Wt.% Wt.% Method 1 A Grafted aspen pulp with 25 LLDPE 75 D
2% silane A-llOO
2 A Same as above 25 PP 75 D
3 A Same as above 25 PVC 75 D
4 A Grafted aspen pulp with 25 LLDPE 75 D
2% silane A-174 5 A Grafted aspen pulp with 25 LLDPE 75 D
2% silane A-172 6 B ~onded aspen pulp with 25 LLDPE 75 D
5% grafted wax with silane A-llOO
7 B Same as above 25 PP 75 D
8 B Same as above 25 PVC 75 D
9 A Grafted aspen pulp with 25 CLLDPE 75 D
2% silane A-llOO
10 A Same as above 25 CLLDPE 75 E
11 B Bonded aspen pulp with 25 CLLDPE 75 D
5% grafted wax with silane A-llOO
; 12 B Same as above 25 CLLDPE 75 E
13 A Grafted aspen pulp with 25 CPVC 75 D
; 2% silane A-llOO
14 A Same as above 25 CPVC 75 E
15 B Bonded aspen pulp with 25 CPVC 75 D
5% grafted wax with silane A-llOO
16 B Same as above 25 CPVC 75 E
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20698~1 Ex- Employed Flller Employed Resin Mixing No. Step Treating Method Wt.% Wt.% Method 17 A Grafted aspen pulp with 25 CaPP 75 D
2% silane A-llO0 18 A Same as above 25 CaPP 75 E
19 B Bonded aspen pulp with 25 CaPP 75 D
5% grafted wax with silane A-llO0 20 B Same as above 25 CaPP 75 N.B.:- Silane A-llO0 is gamma-aminopropyltriethoxysilane - Silane A-174 is gamma-methacryloxypropyltrimethoxysilane - Silane A-172 is vinyltri(2-methoxyethoxy) silane - LLDPE is produced by Novacor.
- PVC is produced by ESS0.
- PP is produced by Shell.

The results of the above examples show improvements from 15 to 270%, based on their related neat resins.

STEP F.:
The same procedure is followed as per example No. 4, U.S. Pat. Application No. 07/779,946, but here the polyethylene film is substituted with compounded polyethylene film with 60% carbon black. The results are showing excellent adhesion.

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It will be understood that the aforementioned descrip-tion of the present invention is susceptible to various modifications, changes and adaptations, and the same are intended to be comprehended within the meaning and the scope of equivalents of the appended claims.

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Claims (20)

1. A process for preparing a composite material based cellulose, which comprises, (a) providing a finally ground organic material selected from the group consisting of cellulosic or ligno-cellulosic fibers or starch, (b) coating said organic material with a bonding agent, or (c) subjecting the organic material obtained in (a) to be grafted with bonding agent, (d) mechanical admixing said coated or grafted organic material obtained in (d) or (c) with ground poly-meric or copolymeric thermoplastic material or rubber, to give said composite material, (e) shaping said composite material obtained in (d) in articles by compression molding, injection molding, extrusion molding, film extrusion, or extrusion sheeting.
2. A process according to claim 1, wherein the organic material is selected from the group consisting of soft wood, or hard wood pulps, nut shells, corn cobs, rice hulls, vegetable fibers, bagasse, cotton, rayon, sawdust, wood flour, wood shavings, jute, linen, flax or starch.
3. A process according to claim 1, wherein the bonding agent is selected from the group consisting of silylating agents, titanate agents, isocyanate agents, stearate agents, zirconate agents, aluminate agents, alumino-zirconate agents and grafted wax with a bonding agent.
4. A process according to claim 1, wherein the organic material is mixed or admixed with inorganic material.
5. A process according to claim 4, wherein the inorganic material is bonded with a bonding agent.
6. A process according to claim 1, wherein the polymeric or copolymeric thermoplastic material or rubber is precompounded with at least one ingredient.
7. A process according to claim 6, wherein the compounding ingredient is selected from the group consisting of inorganic filler, treated inorganic filler with a bonding agent, carbon black, graphite, metallic fibers, metallic powders, ceramic fibers, bonding agent, dispersing agent, plasticisers, colorants, anti-oxidants, opacifiers, heat-stabilizers, impact modifiers, photostabilizers, anti-static agents, biostabilizers& crystalnucleating agents.
8. A process according to claim 1, wherein the polymeric or copolymeric thermoplastic material or rubber, whether compounded with at least one ingredient or not, is selected from the group consisting of polyester-thermoplastic, polyethyleneterphthalate, polyethylene, polypropylene, polyurethane, polyurethane-isocyanate, polyvinylchloride, polyvinylidene chloride, polystyrene, polymethylmethacrylate, polyacrylicbutadienestyrene (ABS) and polycarbonate.
9. A process according to claim 1, wherein the organic material is additionally coated or grafted with a polymeriza-ble functional monomer or oligomer thereof.
10. A process for preparing a composite material which comprises, (a) providing an organic material selected from the group consisting of short or continuous cellulosic or lignocellulosic fibers or starch, (b) coating said organic material with a bonding agent, or (c) subjecting the organic material obtained in (a) to be grafted with a bonding agent, (d) compounding said coated organic material obtained in (d), or the grafted organic material obtained in (c) with hot-molten compounded matrix of polymeric or copolymeric thermoplastic or rubber, wherein said matrix is compounded with at least one ingredient, to give said composite material, (e) shaping articles from the composite material obtained in (d) by compression molding, injection molding,
11. A process according to claim 10, wherein the organic material is selected from the group consisting of wood pulps, nut shells, corn cobs, rice hulls, vegetable fibers, bagasse, cotton, rayon, sawdust, wood flour, wood shavings, jute, linen, flax or starch.
12. A process according to claim 10, wherein the bonding agent is selected from the group consisting of silylating agents, titanate agents, isocyanate agents, stearate agents, zirconate agents, aluminate agents, alumino-zirconate agents and grafted wax with a bonding agent.
13. A process according to claim 10, wherein the organic material is mixed or admixed with inorganic material.
14. A process according to claim 13, wherein the inorganic material is bonded with a bonding agent.
15. A process according to claim 10, wherein the com-pounding ingredient is selected from the group consisting of inorganic filler, treated inorganic filler with a bonding agent, carbon black, graphite, metallic fibers, metallic powders, ceramic fibers, bonding agent, dispersing agent, plasticisers, colorants, anti-oxidants, opacifiers, heat-stabilizers, impact modifiers, photostabilizers, anti-static agents, biostabilizers and crystalnucleating agents.
16. A process according to claim 10, wherein the compounded polymeric or copolymeric thermoplastic or rubber is selected from the group consisting of polyester thermoplastic, polyethyleneterphthalate, polyethylene, polypropylene, polystyrene, polyurethane, polyurethane-isocyanate, polyvinylchloride, polyvinylidene chloride, polymethylmethacrylate, polyacrylic-butadienstyrene (ABS) and polycarbonate.
17. A process for preparing a composite material which comprises, (a) providing a flat material selected from the group consisting of fabrics, wood boards, wood lumbers, cartons, and papers, (b) bonding said organic material with a bonding agent, or (c) subjecting the organic material obtained in (a) to be grafted with a bonding agent, (d) bonding said coated or grafted organic material obtained in (d) or (c) with a film or a sheet of polymeric or copolymeric thermoplastic material or rubber, whether compounded with at least one ingredient or not, to give said composite material.
18. A process according to claim 17, wherein the bonding agent is selected from the group consisting of silylating agents, titanate agents, isocyanate agents, stearate agents, zirconate agents, aluminate agents, alumino-zirconate agents and grafted wax with a bonding agent.
19. A process according to claim 17, wherein the compounding ingredient is selected from the group consisting of inorganic filler, treated inorganic filler with a bonding agent, carbon black, graphite, metallic fibers, metallic powders, ceramic fibers, bonding agent, dispersing agent, plasticisers, colorants, anti-oxidants, opacifiers, heat-stabilizers, impact modifiers, photostabilizers, anti-static agents, biostabilizers and crystalnucleating agents.
20. A process according to claim 17, wherein the compounded polymeric or copolymeric thermoplastic or rubber is selected from the group consisting of polyester thermo-plastic, polyethyleneterphthalate, polyethylene, polypropy-lene, polystyrene, polyurethane, polyurethane-isocyanate, polyvinylchloride, polyvinylidene chloride, polymethyl-methacrylate, polyacrylic-butadienstyrene (ABS) and polycarbonate.
CA 2069861 1992-05-28 1992-05-28 Processes for preparing polymer composites based cellulose Abandoned CA2069861A1 (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0747419A3 (en) * 1995-06-07 1997-07-30 Andersen Corp Advanced compatible polymer wood fiber composite
EP0789049A1 (en) * 1996-02-09 1997-08-13 Ciba SC Holding AG Antistatically equipped polymers
WO2000017270A1 (en) * 1998-09-22 2000-03-30 Novamont S.P.A. Polymers of a hydrophobic nature, filled with starch complexes
US8133552B2 (en) * 2008-12-12 2012-03-13 Great Eastern Resins Industrial Co., Ltd. Primer composition for cured silicon-containing surface and its uses
US8414987B2 (en) 2008-12-12 2013-04-09 Great Eastern Resins Industrial Co., Ltd. Primer composition for cured silicon-containing surface and its uses

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0747419A3 (en) * 1995-06-07 1997-07-30 Andersen Corp Advanced compatible polymer wood fiber composite
EP0789049A1 (en) * 1996-02-09 1997-08-13 Ciba SC Holding AG Antistatically equipped polymers
WO2000017270A1 (en) * 1998-09-22 2000-03-30 Novamont S.P.A. Polymers of a hydrophobic nature, filled with starch complexes
US6962950B1 (en) 1998-09-22 2005-11-08 Novamont S.P.A. Polymers of a hydrophobic nature, filled with starch complexes
US8133552B2 (en) * 2008-12-12 2012-03-13 Great Eastern Resins Industrial Co., Ltd. Primer composition for cured silicon-containing surface and its uses
US8414987B2 (en) 2008-12-12 2013-04-09 Great Eastern Resins Industrial Co., Ltd. Primer composition for cured silicon-containing surface and its uses

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