JP2008502573A - Aliphatic amide composition for chopped strand glass fiber for wet use - Google Patents

Abstract

One or more film forming agents, at least one coupling agent, and (poly) containing an aliphatic amide lubricant synthesized from ethylene amines and C ₅ -C ₂₀ unsaturated fatty acid, size composition is provided . The fatty acid is preferably a conjugated fatty acid, and the (poly) ethyleneamine is preferably tetraethylenepentamine. Aliphatic amide lubricants may be employed by maleated rubber or carboxylated rubber. This size is advantageously applied to glass fibers such as wet use chopped strand glass and is used to form roofing composites such as roofing boards. Aliphatic amide lubricants promote interfacial bonding between glass and asphalt through a vulcanization mechanism. Unsaturation of the aliphatic amide changes the surface energy of the glass fiber, making the glass more compatible with asphalt, increasing compatibility between glass and asphalt, and glass / asphalt interaction via reduced interfacial tension To improve.
[Selection figure] None

Description

The present invention relates generally to a sizing composition for glass fibers, in particular, (poly) containing an aliphatic amide lubricant synthesized from a C ₅ -C ₂₀ fatty acid ethylene amines and unsaturated, wet applications chopped The present invention relates to a sizing composition for strand glass fibers.

  Glass fibers are useful in a variety of techniques. For example, glass fibers are commonly used as reinforcements in the building composite industry because they do not shrink or stretch in response to changing atmospheric conditions. Roofing materials such as roofing boards, roll roofing, and commercial roofing typically consist of a glass fiber mat, an asphalt coating on the fiber mat, and a granular surface layer embedded in the asphalt coating Is done.

  To form a roofing sheet, glass fibers are first formed by narrowing the flow of molten glass material from a bushing or orifice. The molten glass may be thinned by a winder that collects the collected filaments into a package, or a roller that pulls the fibers prior to collection and chopping. In order to protect the fibers from breakage during subsequent processing, delay wear between the filaments and improve the compatibility of the fibers with the matrix resin to be reinforced, after they have been drawn from the bushing Specifically, an aqueous sizing composition is applied to the fiber. After being treated with the sizing composition, the fibers are packaged wet as wet use chopped strand glass (WUCS).

  This wet chopped fiber is then suspended in an aqueous slurry that may contain a surfactant, viscosity modifier, or other chemical agent. The slurry containing the dispersed fibers is then deposited on a moving screen where a significant portion of the water is removed to form a web. A binder is then applied and the resulting mat is heated to remove residual water and to cure the binder. Next, for example by spraying asphalt on one or both sides of the mat, or by passing the mat through a bath of molten asphalt and placing a layer of asphalt on both sides of the mat, and the gaps between the individual glass fibers Asphalt is applied and applied to the mat. The coated mat is then cut into a suitable shape and size to form a roofing sheet.

  Conventional sizing compositions for wet use chopped strand glass typically include a film-forming polymer or resin component dissolved or dispersed in a liquid medium, a coupling agent, and a lubricant. Unfortunately, such conventional size compositions are not always compatible with the asphalt used to coat the fiber mat to form the roofing sheet. Such incompatibility makes processing difficult and can result in roofing sheets with poor physical properties, such as low tear strength. Furthermore, the amount of binder used with conventional sizing compositions can significantly increase the cost of roofing boards.

  Accordingly, in the art, wet use chopped products that increase the compatibility of glass fiber mats with asphalt coatings on glass fiber composite articles, reduce manufacturing costs, and improve the physical properties of the composite. There is a need for improved sizing compositions for use in strand glass fibers.

The object of the present invention is a wet process comprising one or more film formers, at least one coupling agent, and an aliphatic amide lubricant synthesized from (poly) ethyleneamine and a C _{5 to} C ₂₀ unsaturated fatty acid. It is to provide a sizing composition for chopped strand fibers of use. This synthesized aliphatic amide compound is formed with a hydrophilic intermediate based on an amine with a hydrophobic tail on both ends. The hydrophobic tail is preferably conjugated and contains a high degree of unsaturation. In a preferred embodiment, the (poly) ethyleneamine is tetraethylenepentamine and the fatty acid is a conjugated fatty acid. The aliphatic amide lubricant may or may not be modified by an elastomer such as a maleinized rubber or a carboxylated rubber during the synthesis of the aliphatic amide lubricant. Good. Secondary lubricants, viscosity modifiers, pH modifiers, biocides, and flocculants such as glycols and glycol ethers may also be included in the sizing composition. The reinforcing fiber material may be glass, natural fiber, carbon fiber, or one or more strands of one or more synthetic polymers. In at least one embodiment, the glass fiber is coated with a sizing composition and packaged as a wet use chopped strand glass, which is then reinforced building or roofing composite such as a roofing sheet. Used to form.

Another object of the present invention, one or more film forming agents, at least one coupling agent, and described in the above (poly) ethylene amine and C ₅ -C ₂₀ synthetic aliphatic amides from an unsaturated fatty acid It is to provide a composite roofing board material formed of a plurality of glass fibers coated with a sizing composition containing a lubricant.

A further object of the present invention, one or more film forming agents, at least one coupling agent, and described in the above (poly) ethylene amine and C ₅ -C ₂₀ aliphatic amides lubricant synthesized from unsaturated fatty acids It is to provide a reinforced roofing sheet product formed with a randomly oriented glass fiber mat coated with a sizing composition containing an agent.

  The advantage of the synthesized aliphatic amide lubricant is its inherent reactivity to asphalt when forming asphalt roofing products. A covalent bond between the glass and the asphalt is established by a vulcanization mechanism in which the unsaturated hydrophobic tail reacts with the asphalt at high temperatures in the presence of sulfur and crosslinks the glass and asphalt. This interfacial bond results in increased mechanical properties and improved shear strength in composite articles formed from fibers treated with the sizing composition of the present invention.

  A further advantage of the synthesized aliphatic amide lubricant is that the high hydrophobicity and low surface energy of the hydrophobic tail in the aliphatic amide lubricant is such that when forming asphalt roofing products, the glass and asphalt To improve the glass / asphalt interaction through reduced interfacial tension.

  The above-described objects, features and advantages of the present invention, as well as other objects, features and advantages, will become more fully apparent hereinafter in view of the following detailed description.

  Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art. Although methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention, the preferred methods and materials are described herein. It should be noted that the terms “size composition”, “sizing composition” and “size” are used interchangeably herein.

The present invention relates to a sizing composition for chopped strand glass fibers used in a wet process. The sizing composition comprises one or more film forming agent contains at least one coupling agent, and (poly) ethylene amine and C ₅ -C ₂₀ aliphatic amides lubricant synthesized from unsaturated fatty acids. The aliphatic amide lubricant may or may not be modified with an elastomer. Conventional lubricants, viscosity modifiers, pH adjusters, biocides, and flocculants such as glycols and glycol ethers may also be included in the sizing composition.

  The film-forming polymer component of the sizing composition can be any suitable polymer that can be dispersed or dissolved in an aqueous medium and that aggregates to form a film when the sizing composition is dried. In addition, the former membrane is desirably selected to be compatible with the matrix resin in which sized glass fibers are used. Examples of film formers for use in the size composition include polyester polymers, polyurethanes, acrylic polymers, vinyl polymers, mixtures of such polymers, copolymers of corresponding monomers, carboxylic acids or acid anhydrides. Modified polyolefins, cellulose, polyvinyl alcohol (PVA), and mixtures thereof are included. In a preferred embodiment, the film-forming polymer is polyvinyl alcohol, and in a more preferred embodiment, the film-forming polymer is partially hydrolyzed having a hydrolysis of about 87-89% and a low intermediate molecular weight. Polyvinyl alcohol. Examples of suitable polyvinyl alcohols for use in the size include Celvol 203, 205, and 325, available from Celanese Chemicals. The film former may be present in the size composition in an amount of about 30-80% by weight of the dry solid.

  In addition, the size composition includes one or more coupling agents. Preferably, the at least one coupling agent is a silane coupling agent. The silane coupling agent functions to increase the adhesion of the film-forming polymer to the glass fibers and reduce the level of fluff or chopped fiber filaments during subsequent processing. Examples of silane coupling agents that can be used in the size composition may be characterized by amino, epoxy, vinyl, methacryloxy, ureido, isocyanato, and azamide functional groups.

  Suitable silane coupling agents for use in size include γ-aminopropyltriethoxysilane (A-1100), n-trimethoxy-silyl-propyl-ethylene-diamine (A-1120), γ-glycidoxy Propyltrimethoxysilane (A-187), γ-methacryloxypropyltrimethoxysilane (A-174), n-β-aminoethyl-γ-aminopropyltrimethoxysilane (A-1120), methyl-trichlorosilane (A -154), methyl-trimethoxysilane (A-163), γ-mercaptopropyl-trimethoxy-silane (A-189), γ-chloropropyl-trimethoxy-silane (A-143), vinyl-triethoxy-silane (A -151), vinyl-tris- (2-methoxyethoxy) silane (A-2) 71), vinyl-triacetoxysilane (A-188), octyltriethoxysilane (A-137), methyltriethoxysilane (A-162), methyltrimethoxysilane (A-1630), silkest RC-1 vinylsilane, And silkest RC-2 sulfur silane. All of the silane coupling agents listed here are sylkest products available from GE Silicones. Preferably, the size composition includes both an amino silane coupling agent and a vinyl silane coupling agent. The coupling agent may be present in the sizing composition in an amount of 5-30% by weight of the dry solid, preferably in an amount of 10-20% by weight.

The sizing composition also comprises (poly) ethylene amine, a C ₅ -C ₂₀ aliphatic amides lubricant synthesized from unsaturated fatty acids such as linoleic acid or oleic acid. In addition, plant-based unsaturated fatty acids, such as, but not limited to, Agri-Pure 130 (Cargill) and Agripure 150 (Cargill) for synthesizing aliphatic amide lubricants May be used. Preferably, the unsaturated fatty acid is a fatty acid containing a conjugated double bond, such as linoleic acid, Edenor UKD5010 (Coginis), edenol UKD5020 (Coginis), edenol UKD6010 (Coginis). Non-exclusive examples of (poly) ethyleneamine that may be used to form an aliphatic amide lubricant include tetraethylenepentamine (TEPA), diethylenetriamine (DETA), tetraethylenetriamine (TETA), ethylenediamine, diethylenetriamine , Triethylenetetramine, and pentaethylenehexamine. In a preferred embodiment, the (poly) ethyleneamine is tetraethylenepentamine. The synthesized aliphatic amide compound is formed of a hydrophobic intermediate compartment based on an amine with a hydrophobic tail on both ends. The hydrophobic tail is preferably conjugated and contains a high degree of unsaturation. The aliphatic amide lubricant may be present in the size in an amount of 5-30% by weight of the dry solid, more preferably in an amount of 10-20% by weight of the dry solid.

  The aliphatic amide lubricant may be modified with an elastomer by incorporating maleated or carboxylated rubber during the synthesis of the aliphatic amide. Incorporating a hydrophobic rubber or elastomer into the synthesized aliphatic amide helps to reduce the surface energy of the glass fiber and increase the interaction between glass and asphalt. In addition, the elastomer can act as an energy buffer or barrier to dissipate energy between the high modulus rigid glass and the low modulus soft asphalt when the asphalt roofing product is subjected to impact forces. Examples of suitable maleated rubbers include maleic anhydride and polybutadiene adducts, and maleic anhydride and polybutadiene-styrene copolymer adducts. The maleated rubber or carboxylated rubber may be present in an amount of 5-40% by weight of the aliphatic amide lubricant, more preferably in an amount of 10-30% by weight.

  In addition to the synthesized aliphatic amide lubricant, the size composition may also contain a secondary lubricant to facilitate manufacturing. The secondary lubricant may be any conventional lubricant, such as, but not limited to, water soluble ethylene glycol stearate (eg, polyethylene glycol monostearate, butoxyethyl stearate, And polyethylene glycol monostearate), ethylene glycol oleate, ethoxylated aliphatic amine, glycerin, emulsified mineral oil, organopolysiloxane emulsion, stearic acid ethanolamide (trade name Lubesize K-12 (Alpha / Owens Corning)) ), Stantex G-8145 (Cognis), SF-8275 (Cognis), and Emery 6760 (Cognis). This secondary lubricant may be present in the size from 0 to 10% by weight of the dry solids.

  Optionally, the sizing composition may include a viscosity modifier such as polyacrylamide, hydroxyethyl cellulose, or a polyamine viscosity modifier. Specific examples of viscosity modifiers include: Nalco 7530 (ONDEO Nalco), 01PF067 (ONDEO Nalco), Superfloc C-507 (Cytec Industries), Superflox MX 40 (Cytec Industries, Inc.), Cyc Industries, Inc. And Superfloc SD-2065 (Cytec Industries). The viscosity modifier acts as a secondary dispersant in the size composition. The viscosity modifier may be present in the sizing composition in an amount of 0-5% by weight of the dry solid.

  In addition, the size composition may optionally include a pH adjusting agent, such as acetic acid, citric acid, sulfuric acid, or phosphoric acid, sufficient to adjust the pH to the desired level. The pH may be adjusted depending on the intended use or to facilitate compatibility of the components of the size composition. Preferably, the sizing composition has a pH of 3-6, more preferably a pH of 4-5.

  In addition, the size can optionally be conventional additives such as dyes, oils, fillers, heat stabilizers, antifoams, antioxidants, dust suspending agents, wetting agents, and / or other conventional adjuvants. May be included. In addition, the size contains flocculants such as glycols and glycol ethers to aid fiber storage stability, and / or biocides such as Amerstad 250 (Ashland Chemicals) and Nalco 9380 (ONDEO Nalco). Good.

  The balance of the size composition is composed of water. In particular, water may be added to dilute the aqueous sizing composition to a viscosity suitable for its application to glass fibers and to achieve a desired solids content. The sizing composition may contain up to about 99.5% water.

  The sizing composition may be applied to glass strands formed by conventional techniques of drawing molten glass through a heated bushing to form a substantially continuous glass fiber. Any type of glass, such as A-type glass, C-type glass, E-type glass, S-type glass, or variations thereof, is suitable for use as the fiber material. For example, in one variation of E-type glass, boron oxide is replaced with magnesium oxide. Such glasses are commercially available from Owens Corning Fiberglass Corporation under the trade name Advantex®.

  Alternatively, the sizing composition may be applied to one or more synthetic polymer strands, such as polyester, polyamide, aramid, and mixtures thereof. The polymer strand may be used alone as a reinforcing fiber material or may be used in combination with a glass strand as described above. As a further alternative, natural fibers may be used as the reinforcing fiber material. The term “natural fiber” as used in connection with the present invention means plant fiber extracted from any part of the plant including, but not limited to, trunk, seed, leaf, root or sieve. To do. Examples of natural fibers suitable for use as a reinforcing fiber material include cotton, jute, bamboo, ramie, hemp, flax. Carbon fiber may also be used.

  The size composition is preferably such that the size is present on the fibers in an amount of about 0.02 to 0.50 wt%, more preferably about 0.05 to 0.30 wt%, based on the total fiber weight. And applied to the fibers. This can be determined by the loss on combustion (LOI) of the WUCS fiber, which is the weight loss experienced by the fiber after heating to a temperature sufficient to burn or pyrolyze organic sizes from the fiber. The size composition may be applied to fibers having a diameter of about 6-23 microns, more preferably about 11-20 microns in diameter.

  The sizing composition is applied to the fiber in any conventional manner, for example by spraying or by drawing the fiber to be sized across a rotating or stationary roll wetted with the sizing composition. It's okay. The size composition is preferably applied to the fiber in an amount sufficient to provide a fiber having a moisture content of about 10% to about 15% by weight of the WUCS fiber.

  In a preferred embodiment, the glass fiber is sized with a sizing composition and packaged as a wet use chopped strand glass, which then forms a reinforced architectural or roofing composition such as a roofing sheet. Used for. For example, the sized glass fibers are chopped while wet and dispersed in a water slurry that may contain a surfactant, viscosity modifier, or other chemical. The slurry containing the dispersed fibers is then deposited on a moving screen where a significant portion of the water is removed. Next, a binder (eg, urea formaldehyde binder or polycarboxylic acid based binder) is applied, and the resulting mat is dried to remove residual water and to cure the binder. This formed nonwoven mat is an assembly of randomly oriented and dispersed individual glass filaments. The mat may be dried by any conventional method such as passing the mat through an oven. The asphalt is then applied to the dried / cured mat in any known manner, such as by passing the mat through a bath containing molten asphalt, fibers, and optionally an asphalt mixture that may contain sulfur. A layer of asphalt is placed on at least one side of the mat and the gaps between the individual glass fibers are filled. The asphalt-coated mat is then cut into a suitable shape and size to form a roofing sheet. This hot asphalt-coated mat is then passed under one or more granule applicators, which protect the part of the asphalt-coated mat before cutting it into the desired shape. Apply surface granules.

  The synthesized aliphatic amides are designed not only to function as lubricants and dispersants, but also to interact with asphalt in the asphalt mixture. Thus, one advantage provided by the aliphatic amide is its inherent reactivity with other components. For example, the covalent bond (interface bond) between glass and asphalt is established by a vulcanization mechanism, in which the unsaturated hydrophobic tail of the synthetic fat amide reacts with asphalt at high temperatures in the presence of sulfur. Crosslink glass and asphalt. In this reaction, sulfur acts as a catalyst. This interfacial bond between glass and asphalt increases the mechanical strength of the resulting composite article.

  In addition, nitrogen present in the intermediate compartment based on the hydrophilic amine of the synthetic aliphatic amide becomes cationic nitrogen when neutralized with acid. These cationic nitrogens can then form ionic bonds with the anionic charge of the glass fiber, which aids in anchoring the aliphatic amide lubricant to the glass fiber.

  Another advantage provided by the synthetic aliphatic amide is that the aliphatic amide changes the surface energy of the glass, making the glass more compatible with asphalt. The high hydrophobicity and low surface energy of the hydrophobic tail in the aliphatic amide lubricant increases compatibility between glass and asphalt and improves glass / asphalt interaction through reduced interfacial tension. Thus, the new dark aliphatic amide also acts as an adhesion promoter.

  Having generally described the invention, a further understanding can be obtained by reference to the following detailed examples, which are provided for purposes of illustration only, It is not intended to be inclusive or limiting unless specified otherwise.

表２は、表１に記載の成分に基づく、１ｋｇ充填物を示している。

Example 1 Synthesis of Conventional Lubricant (Lubesize · K-12) Lubesize · K-12 is a conventional lubricant that is an adduct of tetraethylenepentamine (TEPA) and stearic acid. Has no degree of unsaturation. The components used to synthesize Lubesize · K-12 are listed in Table 1 below.

Table 2 shows a 1 kg fill based on the ingredients listed in Table 1.

  Stearic acid was filled and melted at 200 ° F. under a light nitrogen blanket. When all the stearic acid had melted, it was stirred under a nitrogen blanket. Heat was removed when the temperature was controlled at 200 ° F. Next, tetraethylenepentamine (TEPA) was gradually added from the dropping funnel. Heating resumed after the exothermic peak. Once all of the TEPA was added, the temperature was raised at a rate that allowed foaming. It was measured that about 50% of distillate was removed at about 380 ° F. At this point, the nitrogen blanket was removed and a low nitrogen sparging was applied.

  After applying the low nitrogen sparging, heat was applied again to a maximum temperature of 480 ° F. until the distillate stopped. When the distillate stopped, the reaction mixture was cooled to a temperature of about 160-170 ° F. with ambient air. The total distillate removed from stearic acid and TEPA was determined to be about 12% of the total charge. Acetic acid was then added over about 15 minutes. A slight exotherm of about 10 ° F. was observed when acetic acid was added. After all the acetic acid had been added, the mixture was stirred for about 10 minutes, then it was poured out onto a release paper where it was allowed to cool and solidify.

  The 1% final product in water had a pH in the range of 4.5-5.0. In addition, the final product before neutralization with acid had a residual acid value of 0.4% and an undetectable iodine value. This solidified product was determined to be Lubesize K-12.

Example 2 Synthesis of Unsaturated Aliphatic Amide Lubricant Containing Conjugated Diene Structure The experiment described in Example 1 was repeated except that stearic acid was replaced with linoleic acid on an equivalent basis. The linoleic acid used was Emersol 315 linoleic acid from Cognis Corp. The final finished product before neutralization with acid had a residual acid value of 0.29% and an iodine value of 24.8%. The iodine value of Emersol 315 linoleic acid was 27.4. It was determined that about 90.5% of the unsaturation in the fatty acids was maintained in the synthesized product.

Example 3 Synthesis of Unsaturated Aliphatic Amide Lubricant Containing No Conjugated Diene Structure The experiment described in Example 1 was repeated except that stearic acid was replaced with oleic acid on an equivalent basis. The oleic acid used was Emersol 213 oleic acid from Cognis. The product synthesized before acid conditioning had a residual acid value of 0.18% and an iodine value of 21.8%. The iodine value of Emersol 213 oleic acid was 24.3. It was determined that about 90% of the unsaturation in the fatty acids was maintained in the synthesized product.

Example 4 Synthesis of Rubber Modified Unsaturated Aliphatic Amides Stearic acid was replaced on a weight basis with 90% Emersol 315 linoleic acid (Cognis) and 10% Ricon 130MA13 maleated polybutadiene (Sartomer) The experiment described in Example 1 was repeated. The synthesized product before neutralizing the acid had a residual acid value of 0.21% and an iodine value of 27.7%. Prior to the condensation reaction, the iodine value of the raw material mixture of reelic acid and maleated polybutadiene was 36.3. It was determined that about 76.3% of the unsaturation in the fatty acids was maintained in the synthesized product.

Example 5: Synthesis of Polybutadiene Styrene Copolymer Rubber Modified Unsaturated Aliphatic Amides Stearic acid was added on a weight basis by 90% Emersol 315 linoleic acid (Cognis) and 10% Ricon 184MA6 maleated polybutadiene. The experiment described in Example 1 was repeated except that it was replaced with styrene rubber (Sartomer). The iodine content of the raw material mixture of reelic acid and polybutadiene styrene rubber before the condensation reaction was 32.2. The synthesized product before acid neutralization had a residual acid value of 0.25% and an iodine value of 30.7%. It was determined that about 95.3% of the unsaturation in the fatty acids was maintained in the synthesized product.

註： ＣＤ＝交叉方向
破断強度は、ＡＳＴＭ・Ｄ−３４６２に記載の方法に従うエルメンドルフ
（Ｅｌｍｅｎｄｏｒｆ）破断強度試験機で測定した。
破断強度の単位はグラムである。 Example 6: Comparison of Lubesize K-12 with an unsaturated aliphatic amide lubricant containing a conjugated diene structure Fiber samples were prepared with a sizing composition containing the aliphatic amide prepared in Examples 1 and 2 above. Coated. This sized fiber sample was formed into a roofing mat on a sheet former. These mat samples were then converted to laboratory roofboard samples by coating the mat with an asphalt mixture containing 0%, 0.2% or 0.8% post-added elemental sulfur. The results are summarized in Table 3.

註: CD = crossing direction
The strength at break is Elmendorf according to the method described in ASTM D-3462.
(Elmendorf) Measured with a breaking strength tester.
The unit of breaking strength is gram.

  The property improvement data in this example shows that a laboratory roofing board formed from fibers sized with a sizing composition containing an aliphatic amide synthesized from TEPA and conjugated fatty acids with external sulfur in an asphalt coating formulation. It shows having an improved breaking strength, with or without. While not wishing to be bound by theory, the increased properties in the sizing composition when no sulfur is added are due to the higher hydrophobicity and reduced surface energy of the glass surfaces with the aliphatic amides of the present invention. I think that the. It also appears that the reduction in surface energy improves the interaction between the glass and the asphalt added to form the experimental roofing sheet.

註： ＣＤ＝交叉方向
破断強度は、ＡＳＴＭ・Ｄ−３４６２に記載の方法に従うエルメンドルフ
（Ｅｌｍｅｎｄｏｒｆ）破断強度試験機で測定した。
破断強度の単位はグラムである。 Example 7: Comparison of Lubesize K-12 with an unsaturated aliphatic amide lubricant that does not contain a conjugated diene structure Fiber samples are sizing compositions containing the aliphatic amide prepared in Examples 1 and 3 above. Coated with. This sized fiber sample was formed into a roofing mat on a sheet former. These mat samples were then converted to laboratory roofboard samples by coating the mat with an asphalt mixture containing 0% and 0.2% post-added elemental sulfur. The results are summarized in Table 4.

註: CD = crossing direction
The strength at break is Elmendorf according to the method described in ASTM D-3462.
(Elmendorf) Measured with a breaking strength tester.
The unit of breaking strength is gram.

  The property improvement data in this example shows that a laboratory roofing board formed from fibers sized with a sizing composition comprising an aliphatic amide synthesized from TEPA and a non-conjugated unsaturated fatty acid is an external sulfur in an asphalt coating formulation. It has been shown that it had improved breaking strength with or without.

  The invention of this application has been described above both in general and with respect to specific embodiments. Although the present invention has been described in what is considered to be the preferred embodiment, other broad variations known to those skilled in the art can be selected within the scope of this general disclosure. The present invention is not limited in all respects except the claims.

Claims (34)

A sizing composition for glass fiber,
At least one film-forming polymer;
One or more silane coupling agents;
(Poly) ethylene amine and unsaturated conjugated C ₅ -C ₂₀ aliphatic synthesized from fatty acid amides lubricant,
The composition characterized by containing.   The sizing composition according to claim 1, wherein the (poly) ethyleneamine is selected from the group consisting of tetraethylenepentamine, diethylenetriamine, tetraethylenetriamine, ethylenediamine, diethylenetriamine, methylenetetramine, and pentaethylenehexamine.   The sizing composition according to claim 2, wherein the one or more silane coupling agents include an aminosilane coupling agent and a vinylsilane coupling agent.   The sizing composition according to claim 2, further comprising a component selected from the group consisting of a secondary lubricant, a pH adjuster, a viscosity modifier, a biocide, a glycol, and a glycol ether.   The sizing composition of claim 1, wherein the aliphatic amide lubricant is modified by incorporating an elastomeric material.   6. A sizing composition according to claim 5, wherein the elastomeric material is selected from the group consisting of maleated rubber and carboxylated rubber.   The at least one film-forming polymer is present in the sizing composition in an amount of 30-80% by weight of total solids, and the one or more silane coupling agents are 5-30% by weight of total solids. The sizing composition according to claim 1, wherein the sizing composition is present in the sizing composition in an amount and the aliphatic amide lubricant is present in the sizing composition in an amount of from 5 to 30% by weight of total solids. At least one film-forming polymer;
One or more silane coupling agents;
(Poly) aliphatic amides lubricant synthesized from ethylene amines and unsaturated C ₅ -C ₂₀ fatty acids,
A reinforced composite roofing material comprising a plurality of glass fibers sized with a sizing composition comprising:   The composite roofing material according to claim 8, wherein the fatty acid is a conjugated fatty acid.   The composite roofing material according to claim 8, wherein the one or more silane coupling agents include an aminosilane coupling agent and a vinylsilane coupling agent.   The composite roofing material of claim 8, wherein the (poly) ethyleneamine is selected from the group consisting of tetraethylenepentamine, diethylenetriamine, tetraethylenetriamine, ethylenediamine, diethylenetriamine, methylenetetramine, and pentaethylenehexamine.   9. The composite roofing material of claim 8, wherein the aliphatic amide lubricant is modified with an elastomeric material selected from the group consisting of maleated rubber and carboxyl or rubber.   The at least one film-forming polymer is present in the sizing composition in an amount of 30-80% by weight of total solids, and the one or more silane coupling agents are 5-30% by weight of total solids. 9. A sizing composition according to claim 8, wherein the sizing composition is present in an amount in the sizing composition and the aliphatic amide lubricant is present in the sizing composition in an amount of 5-30% by weight of total solids.   9. The composite roofing material according to claim 8, wherein the composite roofing material is in the form of an asphalt roofing board.   10. The composite roofing material of claim 9, wherein the aliphatic amide lubricant changes the surface energy of the glass fiber and improves the compatibility of the glass fiber with asphalt present in the asphalt roofing sheet.   The composite roofing material according to claim 8, further comprising at least one component selected from the group consisting of a secondary lubricant, a viscosity modifier, a pH adjuster, a biocide, glycol and glycol ether. Roofing material comprising. A roofing roofing board,
At least one film-forming polymer, one or more coupling agents, and (poly) is sized with a sizing composition comprising a fatty amide lubricant is the reaction product of ethylene amines and C ₅ -C ₂₀ unsaturated fatty acid A mat formed of a plurality of randomly oriented glass fibers;
An asphalt coating on at least a portion of one outer surface of the mat;
The roof board characterized by comprising.   The roofing roof board according to claim 17, wherein the fatty acid is a conjugated fatty acid.   The roofing roofing board according to claim 17, wherein the (poly) ethyleneamine is selected from the group consisting of tetraethylenepentamine, diethylenetriamine, tetraethylenetriamine, ethylenediamine, diethylenetriamine, methylenetetramine, and pentaethylenehexamine.   The roofing roofing board according to claim 19, wherein the one or more silane coupling agents include an aminosilane coupling agent and a vinylsilane coupling agent.   The at least one film-forming polymer is present in the sizing composition in an amount of 30-80% by weight of total solids, and the one or more silane coupling agents are 5-30% by weight of total solids. 18. A roofing roofing board according to claim 17, wherein said roofing board is present in said sizing composition in an amount and said aliphatic amide lubricant is present in said sizing composition in an amount of 5 to 30% by weight of total solids. .   18. The roofing of claim 17, wherein the fiber is a glass fiber and the aliphatic amide lubricant changes the surface energy of the glass fiber and improves the compatibility of the glass fiber with the asphalt. Roof plate.   The roofing roofing board according to claim 17, wherein the aliphatic amide lubricant is modified by incorporating an elastomeric material during the synthesis of the aliphatic amide lubricant.   The roofing roofing sheet of claim 17, wherein the aliphatic amide lubricant alters the surface energy of the glass fiber and improves the compatibility of the glass fiber with the asphalt.   18. The roofing roofing sheet of claim 17, wherein the unsaturated hydrophobic tail on the synthesized aliphatic amide reacts with asphalt to crosslink the glass and asphalt.   The roofing roofing sheet of claim 17, further comprising a sulfur catalyst that promotes interfacial bonding between the glass and asphalt. A method of forming a roofing roof slab,
At least one film-forming polymer,
One or more silane coupling agents, and (poly) aliphatic amides lubricant is the reaction product of ethylene amines and unsaturated C ₅ -C ₂₀ fatty acids,
Forming a mat composed of randomly oriented glass fibers sized with a sizing composition comprising:
Applying an asphalt coating to at least one surface of the mat;
A method comprising the steps of:   28. The method of claim 27, wherein the (poly) ethyleneamine is selected from the group consisting of tetraethylenepentamine, diethylenetriamine, tetraethylenetriamine, ethylenediamine, diethylenetriamine, methylenetetramine, and pentaethylenehexamine.   28. The method of claim 27, wherein the one or more silane coupling agents comprise an amino silane coupling agent and a vinyl silane coupling agent.   28. The method of claim 27, wherein the fatty acid is a conjugated fatty acid.   28. The method of claim 27, further comprising the step of cutting the mat into a roofing roofboard of appropriate shape and size.   28. The method of claim 27, further comprising coating the asphalt with protective granules.   28. The method of claim 27, further comprising reacting the unsaturated hydrophobic tail on the synthesized aliphatic amide with asphalt to crosslink the glass and asphalt.   34. The method of claim 33, further comprising providing a sulfur catalyst that promotes interfacial bonding between the glass and asphalt.