LT3106B - Process for the polymerisation of epoxycompounds - Google Patents

Description

The present invention relates to polymerization catalysts: i <'- / a

is one of the epoxy compounds involved in the reaction

To the bases of Louis. It enables the polymerization to be carried out by the reaction mechanism so as to obtain universal adhesive, layered and formable masses used in medicine, environmental protection and especially in the optics industry for the bonding of adhesive parts.

Another advantage of the proposed process is that epoxy resin can be used to produce masses without the use of solvents. The masses can be used, for example, as universal formable and layered materials in the medical, environmental and optical industries. The proposed polymerization process is also suitable for obtaining prepregs and epoxy resins as a binding agent. It is even better to use this method in the manufacture of materials for the production of printed circuit boards and highly resistant binders.

Lewis bases, such as imidazoles, are known to be quite active catalysts for polymerization reactions, especially for compounds containing · ... . ··. · · '· A ···,' ··., .. ·. a:, epoxy or oxirane groups (Ricciardi, F. et al., J. Polym. Sci. Polym. Chem. Ed. 1983, 21, 1475-90; Farkas, A. et al., J. Appl. Polym. . Sci. 1968, 12, 15968). The disadvantage of these suggestions is that during the polymerization process, the temperature rises sharply, which results in an undesirable change in the color of the polymer masses and renders their structure inhomogeneous.

The temperature also rises if imidazole or substituted imidazole and epoxy. as described in U.S. Patent 4,487,914, which provides an adduct which reacts with.

metal salt. The resulting 7 resinous product is used as a curing agent.

. , //, /. 1: ./-/ 7- ^ 27-, '(' .'7.7 .:. 7, {.

VFR exhibit application 28 10 428 refers to the possibility of reducing the reactivity of the original Lewis bases in epoxy · o. ·. · · 7. · (. ··. -.

addition of such solvents to the compounds, such as; methanol, ethanol or a mixture thereof.

The disadvantage of this method is that additional processing steps are required to remove the solvent after polymerization and the shrinkage creates voids that degrade the properties of the polymer and the polymer is more moisture absorbent. .

U.S. Patent Nos. 3,638,007, 3,792,016, and 4,101,514, as well as U.S. Patent 23,004,889, investigate the possibility of using imidazole-metal compounds as Lewis bases for catalyzing polymerization reactions. These compounds. . are thermostable coordination polymers that only release high imidazole acting as Louis base. No catalytic activity was observed at temperatures below 170 ° C.

Lack of polymerisation reactions with epoxy compounds at these temperatures: formation of by-products due to ring breaking. These products degrade the cross-linked structure of the polymer and, consequently, have adverse effects such as shrinkage, moisture absorption and so on.

By using auxiliary bases, it is possible to reduce the temperature and thus regulate the catalytic action of the reaction.

However, these bases have the following disadvantages:

- auxiliary bases are expensive,

- the bases themselves can react with cheetahs / compounds. / - .. / / 77 ·

-: = //.:, /. / ./ /-.3//=- / / // = /: - '7' / '

U.S. Patent 3,677,978 describes the use of imidazole complex compounds with metal salts, such as CuCl ₂ , CuSO ₄ -, NiCl ₂ , - CoCl ₂ , containing from 1 to 6 moles of imidazole per mol of metal salt as a latent catalyst.

Disadvantages of this method:

- high gel formation temperature (about 160260 ° C) causing inhomogeneity of product and blackening to black color,

- non-uniform solubility of the polymerizable mixture., 15

U.S. Patent 3,553,166 also describes the use of imidazole complexes and an additional nitrogen compound for curing epoxy resins. Here, too, the treatment temperature is about 180 ° C.

^20th

In addition, there is a known method for converting imidazoles into _ύ latent curing agents and catalysts by reacting their salts with various acids such as polycarbonic (U.S. Patent 3,746,686), isocyanuric (VFR Patent 28,11664), phosphorous (U.S. Patent 3,632,427). , 3,642,698, 3,635,894). These solutions raise the following issues:

- high toxicity of imidazole compounds,

- the presence of anions stops the polymerization before the reaction is complete,

-related to this is the increased monomer content = in the polymer. epoxy, / also dew and '/ increased moisture absorption.

It is known from VFR patent 20 19 816 and US patent 4 137 275 that the polymerization of epoxide compounds also uses acetylacetonate complexes in the presence of carbonic acid anhydrides. Here, too, the high processing temperature (over '150 ° C) is considered to be a drawback. The high temperature disadvantages listed are not the only ones. High temperatures result in significant cost increases and severely limit the use of the resulting products.

VFR Patent 25 25 248 describes an epoxy resin hardener such as Cr (acac) ₃ (where acac is acetylacetonate). The disadvantage of this curing agent is that an unstable hydrogen compound is required in the reaction mixture for polymerization and curing with the oxygen oxirane-like compound. Mixtures of a similar nature have another disadvantage: polymerization often begins immediately after the addition of a curing agent and thus it is not possible to obtain stable polymer mixtures.

The resin curing agent Co (III) -acetylJ, in Patent No. 4,473,674 used epoxy as well as acetonate as a component. Because acetylacetonate is used in combination with a solvent, aromatic. with diamine and phenylnovolac, the solvent is released and the resin hardens only when the temperature is raised accordingly. in the first stage, the temperature is raised and maintained under vacuum for 45-55 minutes · the gas is removed. The temperature is then raised to a curing temperature for several hours at normal pressure, and then a further 2-3 hours at 175-177 ° C. Product quality does not deteriorate.

The acetyl acetic acid .35 catalysts described in VFR A 2 - 334 467, which are used to cure epoxy resins, are very expensive and therefore unprofitable (this follows from Example 1 of the reference). Also, separate

Component I reacts with each other non-stoichiometrically, which results in a different quality of the hardener obtained. It can be concluded that these hardeners are suitable only for printing inks and coatings, but not from them

5. Get high quality products.

Attempts have also been made to reduce primary amines, which are already present. However, the data in Table · 1 indicate that the corresponding diamino complexes, known from CH-A 629 230, have a high temperature jump (<120 ° C) and a very long period of subsequent curing. (3 hours), even at relatively high temperatures. · ·

The aromatic amine complexes described in U.S. Patent No. 3,310,602 are latent curing agents. For fast and economical resin curing, the temperature must be raised to 150 ° C, which again results in higher temperatures

- the deficiencies described. The same can be said for the aminophenolic complexes known from U.S. Patent No. 3,367,913, which hardens only at about 150 ° C.

One of the major drawbacks of imidazoles as catalysts is that they, when used directly or in the form of compounds, induce a very rapid reaction of polymer curing. As a result, the resin mass is simultaneously in two states: unsewn and fully sewn. This is based on the use of epoxy resins as layered materials with optimum gel formation times which vary with the imidazole derivative used; however, the addition of a catalyst prevents the introduction of a slow pre-curing step prior to solidification of the mass, leaving no room for a single step such as justification, mass, technological alignment of the adhesive,

It is an object of the present invention to provide a process for the polymerization of epoxy compounds in the presence of Lewis bases to provide cost-effective, ecologically clean and non-toxic * compounds with optimal gel formation.

- Periods, epoxy 'resins based on metal complexes'.

The object of the present invention was to provide a polymerization process for epoxide compounds * using Lujis bases as the initiator for the latent initiation of the polymerization - by separating the initiator from the complex at a temperature below 140 ° C, for example at a temperature not lower than 50 ° C.

This object is achieved by applying the polymerization process of epoxy compounds according to claims 1-5 of the formula of the invention by applying mixtures of epoxy compounds which are polymerized according to the proposed process according to claims 6 and 7 / as well as by applying the proposed measures according to claims 820-12.

In accordance with the invention, the object is achieved by the polymerization of epoxy compounds by the reaction catalyzed by Lewis base, namely: 0 * 01-50 is added to 100 parts by weight of the epoxy compound, preferably 1-10 parts by weight of a metal complex compound having the following general formula:

ML _x B _y , or M [SR] _x B _z , in which

M - a metal ion of the major or subgroup II or III of the periodic-element system,

L - chelating ligand * belonging to the group of dioximes, alpha- and beta-oxycarbonyl compounds or 1,3-diketones to be lysed, / \ · -, 7 + / -. /

SR - acidic residue of inorganic acid, B Lujis base, 7

x .-. kind y -natural number from 1 to 3, number from 1 to 5, 5  z - natural number from 7th to 8,

provided that Lujis base-is not a polyvalent phenolic compound '/ + -' - + ^;

Suggested: The method allows the use of any epoxy / compound containing at least. as two epoxy bonds.

More preferred epoxide compounds are glycidyl and polyether derivatives, such as / εoxidized, novolac, or epichlorohydrine reactions with bisphenol A or bisphenol? B products. The epoxy equivalent of such epoxy resins / ranges from '160 to 500. The polyfunctional epoxy compounds listed above (this term + also includes .epoxide resins) are available. Polymerization / alone - or / when mixed with one another, the solvent is / is not necessary.These compounds can / can be used in mixtures with / monoepoxides which act as a solubilizing agent.

25th

Metals (M) ^ can be used with ions of all metals, but • elements of Groups II and III of the Periodic Table are more suitable for use.

Cobalton nickel, iron, zinc and

7 / manganese ions. // + /'.'///-4/;/:/ / '.' .. --7 -.- + -.,. ·. '/'/'/'/+'·.'/: //: Z +. / + 7 ' _:

Ligands (L) -: Chelating ligands are organic compounds with at least 7 electron donor atomic groups. Example: Dioximes, alpha- and / or 4-beta-oxycarbonyl compounds or enolysed: T, 3-diketbn. - / .-, 7 / + - 44 // '- /' to /

More appropriate

the residue is acetylacetone, benzoylacetone or dipivaloylmethane.

An acidic 'residue (SR} may be a residue of any inorganic acid,

Lujis Base (B). the proposed metallophore complex compounds can utilize all nucleophilic molecules or ions / having a free electron pair. Examples include pyridine or imidazole compounds, ethers including cyclic (tetrahydrofuran), alcohols, ketones, thioethers or mercaptans, except phenolic compounds.

Lewis bases in complex compounds of the formula ML 4 may also be CH-acidic compounds, i.e. compounds containing a motile proton. An example of such CH-acid Louis' bars is. ACidic pyridines, dinitriles or diesters of malonic acid with acetoacetic acid. ester, cyanoacetic acid ester or nitromethane.

Metal cations * are used in metal complexes, exchanging charges through ligands as well as ionic Lujis bases. It is understood that in cases where. of the complex. contains the Louis base, the number of charged ligands decreases.

Another way to obtain the proposed complexes is to link the CH acid · Louis bases to the metal bathrobe through nitrogen and / or oxygen and / or sulfur and / or phosphorus atoms or through hydrogen bonds.

u

These metal complexes are prepared by known methods by reacting the corresponding metal salts with the desired ligands and Louis bases.

L.T3106B. : · / 7. ...: / 9 / - //// - /. / 7 /

Particularly suitable for the preparation of metal complexes are /./these / metal complexes:

bis (acetylacetonate) -cobalt-1 H -diimidazole ,. 5 bis. (Ace thiacetonat) -nickel-1X-di imidazole, bis (acetylacetonate) -zinc- / XI-dimethidazole, bls7 (acetyl eetonate j -manganae-II-di'-imidazole, bis (acetyl acetbnat) -gel-II- diimidazole, bis (acetylacetate) -coba11as-1110 di-dimethylimidazole, bis (acetylacetonat) -cobalt-II-dibenzimidazole / bis (acGtat) 'cobaltac-2-diimidazole, bis (2-ethylhexanate) - cobalt-II-diimidazole, bis (salicylaldehyde) -cobalt-II-diimidazole.

The complexes are mixed with / with the epoxy compounds at a lower non-initiation temperature, preferably from room temperature to -50 ° C.

In this way, // obtain: (mixtures at the specified - temperature A 77xiJoose7; / harden and can be used as / moldable; or molding, adhesive mixtures / or prepregs.

Epoxy compounds are cured by energy supply; at which time the tension increases above the initiation temperature.

The energy can be supplied by heat, light, microwave, various radiations, laser beams and '/ 730.77' /./ in a different form /.../'-/ '' A //// 7/7 - ///: 7. //// 7

The main advantages of the present invention are as follows:

- Ensures the ability to dissolve the metal

A 7 / Compound 7 in the polymerizable ε-oxidase compound or

- ./7/---/ ^? of epoxy compounds at temperature,

..37 ..- 5 3 which is below the polymerization ihici j avis »temperature,

·. · .. · '7 „7. τ / ·; & · · ·. '7:.' '555 this ensures a homogeneous mass of 5 of the resulting polymeric mass,

- it is possible to obtain transparent polymeric masses (for example, Uganda using benzoylacetopate or dipivolylisethane) or dyed (using

-acid anions such as sulfates, nitrates, halides, phosphates and the like),

-no need to use · to reduce LuL base reactivity of solvent, /

-no additional solvent removal required »

· this prevents the possibility of the formation of 20 shrinkage cavities in the polymer which impairs its properties,

- this avoids increased moisture absorption, •. · '' '7-. '' '7' -.7¼ 5 - ./5.57- 7 f 7 '' '.7.' '.' / 7.-. '/' j .; '7

-no toxic effect of imi dye compounds, 25 ^z Ruryse In this case, acts as initiators of polymerization,

-the decomposition reaction of the metal ^and Lewis base compound is carried out at room temperature above 58 ° C to 14 ° C,

-appears the possibility of storing and forming so-called '* one-component systems'. ; / 11 / '· these systems; only after reaching the initialization temperature.

of polymerization

Metal complexes with polymerizable compounds can be used with or without additives, such as curing agents, which means that the composition of the polymeric mixtures can be varied within wide limits.

The onset of polymerization, vol. y. Initial temperature, 10 is determined by optional ions for Uganda, Louis base and acid residues. The reaction of complexes with anions begins at temperatures lower than those of complexes with chelating ligands. Also, using modified

Lewis bases such as alkylated imidazoles have a lower polymerization initiation temperature than unmodified imidazole.

By appropriately 'selecting the composition of the complexes from the appropriate ligands, Louis' bases and metals, the polymerization initiation temperature can be varied within wide limits.

Unexpected is that the initiator of the reaction of a polymerizable compound is carried out at much lower temperature ^1, neither the wait could be known from the literature complexes decomposition temperatures.

In addition, polymerization of epoxy compounds with the proposed metal complexes not only achieves optimum gel formation times, but also reduces the absorption of water and acetone as compared to conventional Lewis bases (such as iodine).

# The advantages of the proposed process include: polymerization reaction- 50-140 ° C is more suitable;

. . . .,. . ..7 .: /../ 12 .. 77 // </.7-/.7-. / '/ / 77 .7 7'.

^ single component systems ** / does not control time below the polymerization initiation temperature. and the ability to harden these systems only after reaching the 7 polymerization initiation temperature; undetectable toxicity of imidazole compounds which act as initiators in this case.

The proposed solution enables the production of economically viable and non-toxic

10 ′ latencies; epoxy resins based on metal complexing compounds with an optimal gel-forming time.

These mixtures contain 100 parts by weight of the epoxy compound _; 0.01 to 50 parts by weight (preferably 1-10 parts by weight) of a metal complex compound having the general formula:

ML _x B _y , or M [SR] _x B _z , in which

77- /. '/', · '17'S'77.7,7./7 .: 7 7 ··' /'.7 '7 77.7 · / 7. ·. '/ 7' P · ///.; -7 7./,../7: 7 / · '

M is a metal ion from a major group or subset II or III of the periodic table system,

L - a chelating ligand belonging to the dioxyl / group, alpha- and beta-oxycarbonyl compounds or enolizable 1,3-diketones,

SR - acidic inorganic acid residue,

B - Lu j iso Base »

#. '* - natural number from 1 to 8 »

-y - .. an integer of 1 to 5, z of an integer of 7 to 8 #, provided that Luis base is not a poly-aseptic phenolic compound.

Suggested mixtures due to the properties of the bond »plus # if necessary, known additives and fillers

used for bonding and. For use in the manufacture of sealing compoundsThey can be used as a bonding and forming mass, for example, for the manufacture of bulk molded parts which do not undergo stress when cured.

Despite the presence of ions in metal complexes, .epoxide resins polymerized according to the proposed process exhibit excellent dielectric properties. properties. Therefore, the proposed blends can be used in the production of 10 high quality printed circuit boards and as a binder for molding compounds such as electrical engineering and electronics.

R 'RR / -' + '''' ^V /, '.. +; '' · + '-'oh; . · '''···' + '' + '·. + R Λ //., +. - '' R '

In addition, they can be used in the manufacture of highly resistant binders, as the low polymerization temperature ensures the bonding of materials without internal stresses.

Examples

The invention is illustrated by various examples below:

In each case, 1 mol of the epoxy compound is mixed with 0.05 mol of the metal complex at room temperature.

'''+ - +''·+'+.;'·'<+'' ·· · - + '' + * R- R. . + + ·. R + '> + ·. + R + R-' ^Λ + / · / + ^: r '

100 grams of the mixture is used to determine the gel formation time (Method DIN 16945, para 6.3, Method A).

Drain a portion of the mixture and polymerize samples for determination of moisture and acetone absorption;

The remainder of the mixture is stored at room temperature. No signs of polymerization were observed after more than 6 months.

^ The test results are listed in the table below

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o 0 P P ra ra XJ Ό P . P n U ^: ra ra ra 3 (β ra 3 ra n ra ra P Φ ra p ra P © © P © © P © c P © C -P © , / '-P X • rl. X -P 7/7 X // - ra ra X '.rH P i -P t 1 1-1 t p- 1 > © o Φ m <n o oh tn , P 00 CP P -s} · cn CM e CM 77 o o Oh o □ ° o o o CM o O CM ^s o CM O O O <y> et. r-ί 00 p; : P t " r-l. L0 co r * · 04 P ra c ... Λ, P ra c P 0 0 ra 1 P P c 0 Φ © 0 c υ ra P -H υ ra et • P P © o .//-ra-,. et & 0. • p § Ό P © O 0 P N M O P R 3 G N Q P ι. ····. · * τ. · ^ © and © Λ I S c n © cn 0 -  Oops  -p (N P o o M 0 H 0 o 'j oo υ υ M o + Ό P n to ra P • P • P P P P © I 0 © © P ra q m P P © P • p ra © © P £ P < 0 φ ra ra < 0 < 0  V t p P -P P 1 P t rM o .P » Ό © o • P 0 • ri et Ό » et, £ r-4 d P ό 0 • P Z • p p 0 -P 0 P ft 0  Λ ' U -p c 0 c 0 Φ P Z P C © P © • P P r-l o φ  P p. P p ra tP Z -P P n (JI ra 0> P P '* Mon p P • P / P • P man p z b »Ό 0 B4 -d., // ffl Ό P CM m ra * . · '+

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ra  A £ Q Ά (B M - / 'οι / (0 ' w tn m P <0 ω 7 -, - 3- JJ . <· en (.- (/ 3-. ¹ . <d <d tn Φ JJ id ' '(ra- Φ 4J td m jj JJ · <d Ή Φ JJ ra Φ jj Φ • Φ Φ - Yeah • H Φ c A - . Φ C • Ή • r | Φ Λί . * rj f • rj ': • rj I Round 7 ra ' ./ 'P, -P 1 U ~) 1 · '-R-J ΛΟ . r: . · * —4 1 * 3 * O 70) \ O CM Φ O O rH kO θ ' r-J r-1 kO ^; d> c \ CM CM O O O O O CM / - E- | ' O O t- · o O O r "1 f 7 Oh 00 vJ : rrj . & io co ΟΊ

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. t-l 7-U A. - Λ ·. · / h 7 7 u ra · w 7 '' ra ( ra . -p • rrj .-p. 77 • P NO P M:. · P - P ··> <· φ Φ - '( ra P p: -JJ _r ^: - P 43 -H CP ^: Φ. .... Φ '· 7 / Υ -'. · . ra /./.:.:- ra C 0 / < b L , '7 < 0 /. / <: o 3 1 i-i  1 • rH z '. ·. · . . 1 i-4 ' 1 t-1  'ΓΊ 0 • P Z 0 ' • H / ((/ (O- Ή o Ή r— ( d 3-4 r - t .d . * —1 d d • H 0 • H  0 • P. . .-- - / - 0 • H C 0 - . q ϋ ..---. (C 0 . - C d 0: / · '' . ra -P /;·.· ra • H Φ • P ra . Ή - U_, 3P . M rH : m-ι r-In 7 · M-1 A ' & 9 ra &> ra & V / 'ra - θ '·: /. 'M φ • P • H • P ♦ H • H • P : 'P Ή CQ d * 0. CQ t 'P • . v £. * to he . 'r-

Claims (12)

DEFINITION OF INVENTION CLAIMS 1. A method for polymerizing epoxy compounds with metal complexes having a weight of 100 5 parts by weight of epoxy compound mixed with 0.01 to 50 parts by weight of a metal compound of general formula ML _x B _y „or M {SR1, B ₂ , · '· f ..-: ·' - ·· 'V · .......,. .... <. ·. where H is a metal ion from a major group or subset II or III of the periodic table system, 15 L '- chelating ligand belonging to the group - dioximes, alpha- and beta-oxycarbonyl compounds or enolizable 1,3-diketones, SR - acidic inorganic acid residue, · B - Louis Base, 20 x - Numbers 1 to 8, y - Numbers 1 to 5, ₍ .z - Numbers 7 to 8, provided that the Lewis base is not polyvalent phenol Compound 25. 2. A process according to claim 1, wherein the metal complex is a compound containing benzoylacetonate, acetylacetone or 30 dipivaloiImethane. 3. A process according to any one of claims 1 to 2, wherein the metal complex is used as metal ions containing cobalt, nickel, iron, zinc, 35 'or manganese ions. '. // ¹⁷ ' ^: Process according to one of Claims 1 to 3, characterized in that a metal complex compound is used which contains as pyridine, imidazole, tetrahydrofuran, alcohol, ketone, thioether or as a Luisobase. 5 mercaptans. 5. A method according to any one of claims 1 to 4, characterized in that it utilizes a metal complex compound containing CH-acid pyridine as Louis base, 10 diester or dinitrile of malonic acid, ester of acetylacetic acid, ester of cyanoacetic acid or nitromethane. 6. Mixtures of epoxy compounds and Lewis bases, characterized 15, characterized in that they contain 100 parts by weight of one or more epoxy compounds and 0.01 to 50 parts by weight of a metal complexing compound having the general formula ML _x B _y , or M [SR] _x B _z ,. in which.-b '' · // · '' /.3/ · /b\..//· ^; - ·· '· /.''' / ·· ''_; - '- /'. ''/'' ^- //', · / - .. 7 / - '7''/•' b ./''/. , / ·. · '// M - a metal ion from the major group or subgroup II or III of the periodic table system, 25 L chelating ligand belonging to the group of dioximes, alpha- and beta-oxycarbonyl compounds or enolizable 1,3-diketones, SR - acidic inorganic acid residue, B - Louis Base, 30th X - in kind number from 1 to 8, y - in kind number from 1 to 5, Z - in kind number from 7th to 8, with the proviso that the Lu j iso .base is not a poly valence phenolic 35 compound. . .7 -; ..; // = / ==== / /: -. - /-.::/,:-:</=/:/·/νΓ3ίΟ6-.Β / = / = 18 = /// = Mixtures according to claim 6, characterized in that 100 parts by weight of the epoxy compound contains ΙΙΟ parts by weight of the metal complex compound. 5 ' Use of mixtures according to claim 6 or 7 for the production of adhesive or sealant masses. Use of mixtures according to claim 6 or '7' as binders in molding masses. Use of mixtures according to claim 6 or 7 as binders for high-quality molding compounds used in electrical engineering and electronics. 15 .. Use of mixtures according to claim 6 or 7 for the production of printed circuit boards. Use of mixtures according to claim 6 or 7 for the production of high-resistance binders.