Heat-accelerated adhesive composition based on silane-terminated polymer

Abstract

The present invention relates to a reactive one-component adhesive composition that is liquid at room temperature and comprises 3-90% by weight of at least one alpha silane-terminated organic polymer, 0-80% by weight of at least one silicone resin, 0.1-5% by weight of at least one thermal accelerator, 0.001-5% by weight of at least one low molecular weight silane having primary or secondary amino groups or blocked amino groups that cure to form primary or secondary amino groups, and 0-85% by weight of at least one extender. The present invention also relates to a method for bonding two substrates using the adhesive composition described above, and to the system bonded in this manner.

Description

[Technical Field]

[0001] The present invention relates to a reactive one-component adhesive composition that is liquid at room temperature, comprising, based on the total weight of the composition, 3% to 90% by weight of at least one alpha-silane-terminated organic polymer, 0% to 80% by weight of at least one silicone resin, 0.1% to 5% by weight of at least one heat accelerator, 0.001% to 5% by weight of at least one low molecular weight silane having primary or secondary amino groups or blocked amino groups that become primary or secondary amino groups upon hydrolysis, and 0% to 85% by weight of at least one filler. The present invention further relates to a method for joining two substrates with this adhesive composition, and to the system thus joined. [Background technology]

[0002] Heat-accelerated reactive adhesives are widely used in industrial applications to meet requirements regarding feed time (often relatively long due to process influences) and the need for relatively rapid curing to allow for further processing (e.g., sawing). A typical application is the manufacture of insulation panels with metal outer plies. In this case, curing occurs in a heated press, which accelerates chemical curing. In many applications, substrates with significantly different expansion coefficients are joined, so the press temperature must not be so high as to prevent the assembly from flexing. In the field of 2K (two-component) polyurethane adhesives, heat-unstable accelerators are used, such as those available from Tosoh under the trade name Toyocat®.

[0003] The isocyanate component of these adhesives is generally based on (polymer) methylenediphenyl diisocyanate (MDI). Monomer MDI has sensitizing properties, as revealed by regulatory proposals from the European Chemicals Agency, and for this reason, its use has only recently been restricted by REACH.

[0004] 2K adhesives are typically processed using a mixing / measuring unit, during which the specified mixing ratio must be constantly monitored. Deviating from the predetermined mixing ratio can result in quality defects. Typical application techniques include spray application or bead application using a coating rake. In the case of spray application, the spray mist can be released into the surrounding environment and must be considered in the context of workplace hygiene. In the context of bead application using a coating rake, the reactive mixture can accumulate in the coating rake over time, potentially clogging it. This effect is particularly exacerbated if the coating rake and adhesive are not compatible.

[0005] Alternatively, a moisture-crosslinked 1K (one-component) polyurethane adhesive can be used. However, a drawback of this method is that CO2 is generated during curing, and this must be removed during the pressing process. If the pressing time is too short or the moisture content is too low, so-called post-expansion may occur, which can lead to defects and / or a decrease in strength of the assembly.

[0006] A silane-based hot-melt adhesive is described in a German patent application (application number 102020111278.5).

[0007] For example, a further requirement in the manufacture of panels used in the fields of architecture, ships, or railways is fire prevention. Adhesives used in the fields exemplified above that meet Class A2 of DIN EN 13501:2019-05 have a maximum heat output of 4 MJ / m³ for non-critical components inside buildings in accordance with EN ISO 1716 (2018-10). 2 It is required that the adhesive meets certain criteria. Low-flammability polyurethane adhesives with a low heat generation of less than 15 MJ / kg are described, for example, in WO03 / 051954A1.

[0008] Further application areas where liquid reactive adhesives undergo a thermosetting process include the manufacture of automotive roof linings or panels. US5,007,976A describes a method for pressing a sandwich-type composite consisting of a foam core, fiberglass, and a fabric outer ply at temperatures above 90°C using an MDI-based 1K polyurethane adhesive. [Overview of the Initiative] [Problems that the invention aims to solve]

[0009] The object of the present invention is to provide a heat-accelerated adhesive composition that does not contain isocyanates, does not generate gas during curing, is manufactured as a single component, and, advantageously, generates relatively low heat. [Means for solving the problem]

[0010] The objective is a reactive, one-component adhesive composition that is liquid at room temperature, based on the total weight of the composition. a) At least one alpha-silane-terminated organic polymer in an amount of 3% to 90% by weight, b) At least one silicone resin in an amount of 0% to 80% by weight, c) At least one heat accelerator in an amount of 0.1% to 5% by weight, d) At least one low molecular weight silane having primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, in an amount of 0.001% to 5% by weight, e) This is achieved by a composition containing at least one bulking agent in an amount of 0% to 85% by weight.

[0011] Furthermore, the above-mentioned objective is a method for joining two substrates, (a) A step of applying the reactive one-component adhesive composition according to the present invention to a first substrate to provide an adhesive area, (b) A step of bringing a second substrate into contact with the adhesive area from step (a), (c) This can also be achieved by a method that includes the step of thermally curing the adhesive composition at a temperature of at least 50°C.

[0012] Furthermore, the above-mentioned objective can also be achieved by a bonding substrate system comprising two substrates, wherein the two substrates have a common adhesive region, and in the common adhesive region, the two substrates are bonded together by the use of a thermally cured adhesive composition according to the present invention, particularly by the method according to the present invention.

[0013] Surprisingly, it has become clear that the bonding of two substrates, particularly for manufacturing sandwich-type elements, can meet manufacturing cycle times using the adhesive compositions of the present invention. The adhesive compositions of the present invention are noteworthy for their ease of processing, broad adhesive spectrum, and low odor during curing in a wide range of applications, particularly in the automotive and construction sectors, where there is a need to replace existing solvent-containing or isocyanate-containing adhesives (e.g., sealants, flooring adhesives, assembly adhesives). Their rapid complete curing enables a wide range of industrial applications. Therefore, the present invention also relates to the use of the adhesive compositions of the present invention in the automotive and construction sectors.

[0014] Even more surprisingly, it has become clear that the above-mentioned objectives can be satisfactorily achieved in the presence of low molecular weight silanes and optionally fillers and further additives, by combining a mixture containing so-called alpha-silanes, optionally a silicone resin as described in WO2003 / 014226A1, WO2010 / 066826A1, or WO2013 / 026654A1, with a thermally unstable accelerator as described in DE60116825T2. [Modes for carrying out the invention]

[0015] Thus, it is possible to manufacture a roof lining for an automobile by a conventional method for joining two substrates. Therefore, a further aspect of the present invention relates to a method according to the present invention for joining two substrates, wherein the resulting joined substrate system constitutes a roof lining for an automobile. Therefore, the substrate system according to the present invention may be a roof lining for an automobile.

[0016] Therefore, the reactive one-component adhesive composition according to the present invention is different from both two-component adhesives and surface coating materials. Furthermore, since the reactive one-component adhesive composition according to the present invention is liquid at room temperature, it is also different from hot-melt adhesives that are solid at room temperature. Therefore, in the context of the present invention, the term "liquid" is considered to be delimitation from "solid". In any case, the maximum viscosity measured by the Brookfield method is 1000 Pa at 20 rpm and 25°C. * It must not exceed s.

[0017] The reactive one-component adhesive composition according to the present invention preferably does not contain monomer isocyanates. In the context of the present invention, "does not contain monomer isocyanates" means that the fraction is less than 1% by weight based on the total amount of the composition. This fraction is preferably less than 0.1% by weight.

[0018] The reactive one-component adhesive composition according to the present invention is preferably, based on the total weight of the composition, a) At least one alpha-silane-terminated organic polymer in an amount of 3% to 90% by weight, b) At least one silicone resin in an amount of 0% to 50% by weight, c) At least one heat accelerator in an amount of 0.1% to 5% by weight, d) At least one low molecular weight silane having primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, in an amount of 0.001% to 5% by weight, e) Contains at least one bulking agent in an amount of 0% to 80% by weight.

[0019] More preferably, the reactive one-component adhesive composition according to the present invention is, based on the total weight of the composition, a) 3% to 50% by weight of at least one alpha-silane-terminated organic polymer, b) At least one type of silicone resin in an amount of 1% to 30% by weight, c) At least one heat accelerator in an amount of 0.1% to 2.5% by weight, d) At least one low molecular weight silane having primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, in an amount of 0.01% to 5% by weight, e) Contains at least one bulking agent in an amount of 10% to 80% by weight.

[0020] More preferably, the reactive one-component adhesive composition according to the present invention is, based on the total weight of the composition, a) 5% to 25% by weight of at least one alpha-silane-terminated organic polymer, b) At least one silicone resin in an amount of 5% to 20% by weight, c) At least one heat accelerator in an amount of 0.1% to 1% by weight, d) At least one low molecular weight silane having primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, in an amount of 0.1% to 4% by weight, e) Contains at least one bulking agent in an amount of 30% to 80% by weight.

[0021] More preferably, the reactive one-component adhesive composition according to the present invention is, based on the total weight of the composition, a) 15% to 25% by weight of at least one alpha-silane-terminated organic polymer, b) 10% to 12% by weight of at least one type of silicone resin, c) At least one heat accelerator in an amount of 0.2% to 0.5% by weight, d) At least one low molecular weight silane having primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, in an amount of 1% to 3% by weight, e) Contains at least one bulking agent in an amount of 59.5% to 73.8% by weight.

[0022] The reactive one-component adhesive composition according to the present invention contains components a) to e), and components b) and e) are optional (0% by weight). Therefore, the reactive one-component adhesive composition according to the present invention contains components a), c), d), or component a), 0.1% by weight or more of b), c), d), or components a), c), d), 0.1% by weight or more of e), or components a), 0.1% by weight or more of b), c), d), and 0.1% by weight or more of e).

[0023] The compositions according to the present invention may further comprise additional components. Thus, one embodiment of the present invention relates to a reactive one-component adhesive composition according to the present invention comprising the components described above. A further embodiment of the present invention relates to a reactive one-component adhesive composition according to the present invention further comprising one or more components, such as 2, 3, 4, 5, 6, 7, 8, 9, or 10, in addition to the components described above.

[0024] The reactive one-component adhesive composition according to the present invention contains at least one alpha-silane-terminated organic polymer. Therefore, the reactive one-component adhesive composition according to the present invention may comprise one alpha-silane-terminated polymer, or two or more polymers, such as two, three, or four. In this case, it will be apparent to those skilled in the art that the polymer does not represent a pure substance, but rather a mixture of multiple substances having a characteristic substance distribution as a result of its manufacture, and therefore "polymer" is a simplified term for such a mixture of substances.

[0025] Alpha-silane-terminated organic polymers are well known to those skilled in the art and are available commercially, for example. For instance, Wacker Chemie AG, Munich, Germany, sells such alpha-silane-modified polymers under the trade name Geniosil®, such as Geniosil® STP-E10 or Geniosil® XB 502.

[0026] It is noteworthy that alpha-silanes possess the so-called alpha effect. This effect activates the alkoxy group on the silicon atom near a negatively charged donor, such as nitrogen or oxygen, located at the alpha position relative to the silicon atom (i.e., for example, with only a methylene crosslink present). As a result, the reactivity of these groups to nucleophiles such as water increases. This promotes hydrolysis without the need for, for example, a tin-containing catalyst. This silane can be hydrolyzed to form a crosslinked siloxane. Therefore, the reactive one-component adhesive composition according to the present invention is an alpha-silane-terminated adhesive that can form a siloxane through a water crosslinking reaction.

[0027] At least one alpha-silane-terminated organic polymer is preferably an alpha-silane-terminated organic polymer of the following formula (I): Y-[(CR 1a 2)-Si(R 2a ) b1 (OR3a ) 3-b1 x (I) In the formula, Y is an x-valent polymer radical group bonded via nitrogen, oxygen, or sulfur, R 2a may be the same or different and is a monovalent, optionally substituted, SiC-bonded hydrocarbon radical group, R 1a may be the same or different and is a hydrogen atom or a monovalent, optionally substituted, hydrocarbon radical group that may be attached to a carbon atom via a nitrogen, phosphorus, oxygen, sulfur, or carbonyl group, R 3a may be the same or different and is a hydrogen atom or a monovalent, optionally substituted, hydrocarbon radical group, x is an integer from 1 to 10, b1 may be the same or different and is 0, 1, or 2.

[0028] Such an alpha-silane-terminated organic polymer is well-known from WO2003 / 014226A1, WO2010 / 066826A1, or WO2013 / 026654A1.

[0029] Therefore, the radical group R 2a ​Examples include alkyl radical groups such as methyl, ethyl, n-propyl, isopropyl, 1-n-butyl, 2-n-butyl, isobutyl, tert-butyl, n-pentyl, isopentyl, neopentyl, and tert-pentyl radical groups; hexyl radical groups such as n-hexyl radical groups; heptyl radical groups such as n-heptyl radical groups; octyl radical groups such as n-octyl radical groups and isooctyl radical groups, and 2,2,4-trimethylpentyl radical groups; nonyl radical groups such as n-nonyl radical groups; decyl radical groups such as n-decyl radical groups; dodecyl radical groups such as n-dodecyl radical groups; n-oc These include octadecyl radical groups such as tadecyl radical groups; cycloalkyl radical groups such as cyclopentyl, cyclohexyl, cycloheptyl radical groups, and methylcyclohexyl radical groups; alkenyl radical groups such as vinyl, 1-propenyl, and 2-propenyl radical groups; aryl radical groups such as phenyl, naphthyl, anthryl, and phenanthryl radical groups; alkaryl radical groups such as o-, m-, and p-tolyl radical groups; xylyl radical groups and ethylphenyl radical groups; and aralkyl radical groups such as benzyl radical groups, alpha-, and beta-phenylethyl radical groups. The substituted radical group R 2a Examples include haloalkyl radical groups such as the 3,3,3-trifluoro-n-propyl radical group, the 2,2,2,2',2',2'-hexafluoroisopropyl radical group, and the heptafluoroisopropyl radical group, as well as haloaryl radical groups such as the o-, m-, and p-chlorophenyl radical groups. 2a Preferably, it comprises a monovalent hydrocarbon radical group having 1 to 6 carbon atoms and optionally substituted with a halogen atom, more preferably an alkyl radical group having 1 or 2 carbon atoms, and particularly a methyl radical group.

[0030] Radical group R 1a Examples include the hydrogen atom, R 2aRadical groups as explicitly defined, and furthermore, optionally substituted hydrocarbon radical groups bonded to a carbon atom via nitrogen, phosphorus, oxygen, sulfur, carbon, or a carbonyl group. Radical group R 1a Preferably, it comprises a hydrogen atom and a hydrocarbon radical group having 1 to 20 carbon atoms, particularly a hydrogen atom.

[0031] Radical group R 3a Examples include a hydrogen atom or a radical group R 2a This is an example that explicitly states the radical group R. 3a Preferably, it comprises a hydrogen atom or an alkyl radical group having 1 to 10 carbon atoms and optionally substituted with a halogen atom, and more preferably, an alkyl radical group having 1 to 4 carbon atoms, particularly a methyl and an ethyl radical group.

[0032] The polymers that give rise to the polymer radical group Y are, in the sense of the present invention, all polymers such that at least 50%, preferably at least 70%, and more preferably at least 90% of all bonds in the main chain are carbon-carbon bonds, carbon-nitrogen bonds, or carbon-oxygen bonds. The polymer radical group Y is preferably a polymer chain comprising polyoxyalkylenes such as polyoxyethylene, polyoxypropylene, polyoxybutylene, polyoxytetramethylene, polyoxyethylene-polyoxypropylene copolymer, and polyoxypropylene-polyoxybutylene copolymer; hydrocarbon polymers such as polyisobutylene, polyethylene, or polypropylene, and copolymers of polyisobutylene and isoprene; polyisoprene; polyurethane; polyester; polyamide; polyacrylate; polymethacrylate and polycarbonate, and preferably (one or more) groups-[(CR 1a 2)-Si(R 2a ) b1 (OR 3a ) 3-b1] is connected via -OC(=O)-NH-, -NH-C(=O)-O-, -NH-C(=O)-NH-, -NR'-C(=O)-NH-, NH-C(=O)-NR'-, -NH-C(=O)-, -C(=O)-NH-, -C(=O)-O-, -OC(=O)-, -OC(=O)-O-, -SC(=O)-NH-, -NH-C(=O)-S-, -C(=O)-S-, -SC(=O)-, -SC(=O)-S-, -C(-O)-, -S-, -O-, and -NR'-, where R' may be the same or different, 2a It has a clearly defined term, or the group is -CH(COOR'')-CH2-C(O)OR'' (wherein R'' may be the same or different). 2a The polymer comprises an organic polymer radical group (having a clearly defined definition). Examples of radical groups R' include cyclohexyl, cyclopentyl, n- and isopropyl, n-, iso- and t-butyl, as well as various stereoisomers of pentyl radical groups, hexyl radical groups, or heptyl radical groups, and phenyl radical groups. The radical group R' preferably comprises the group -CH(COOR'')-CH2-COOR'', or an optionally substituted hydrocarbon radical group having 1 to 20 carbon atoms, more preferably a linear, branched, or cyclic alkyl group having 1 to 20 carbon atoms, or an aryl group having 6 to 20 carbon atoms and optionally substituted with halogen atoms. The radical group R'' preferably comprises an alkyl group having 1 to 10 carbon atoms, more preferably a methyl, ethyl, or propyl radical group.

[0033] Particularly preferably, the radical group Y in formula (I) comprises a polyurethane radical group and a polyoxyalkylene radical group, and more particularly, a polyoxypropylene-containing polyurethane radical group or a polyoxypropylene radical group.

[0034] In a particularly preferred configuration of the present invention, at least one alpha-silane-terminated organic polymer is a silane-terminated polyether and a silane-terminated polyurethane, particularly -OC(=O)-NH-C(R1a )2 units or -NH-C(=O)-NR'-C(R 1a )silane-terminated polypropylene glycol and silane-terminated polyurethane (wherein R' and R) each have dimethoxymethylsilyl, trimethoxysilyl, diethoxymethylsilyl, or triethoxysilyl terminal groups attached via two groups. 1a (It has one of the definitions described above.)

[0035] The average molecular weight Mn of the alpha-silane-terminated organic polymer is preferably at least 400 g / mol, more preferably at least 600 g / mol, particularly at least 800 g / mol, preferably up to 30,000 g / mol, more preferably up to 19,000 g / mol, and particularly up to 13,000 g / mol. The viscosity is preferably at least 0.2 Pas, more preferably at least 1 Pas, very preferably at least 5 Pas, preferably up to 1,000 Pas, and more preferably up to 700 Pas (measured at 20°C in all cases).

[0036] The alpha-silane-terminated organic polymers used in the present invention may be commercially available conventional products or may be prepared by conventional chemical methods. Alpha-silane-terminated organic polymers may also be prepared by various well-known processes, such as hydrosilylation, Michael addition, Diels-Alder addition, or addition reactions such as the reaction of an isocyanate-functional group-containing compound with an isocyanate-reactive group-containing compound.

[0037] Very preferably, at least one alpha-silane-terminated organic polymer is a polymer of the following formula having at least one terminal group, preferably at least two, and especially more than one terminal group.

[0038] * -XC(=O)-N(R)-C(R 1 R 2 )-Si(R 3 ) a (OR4 ) 3-a During the ceremony, X is O or N(R), Each R is independently either a hydrogen atom or a hydrocarbon radical group having 1 to 20 carbon atoms. R 1 and R 2 These are, independently of each other, hydrogen or hydrocarbon radical groups having 1 to 20 carbon atoms. R 3 and R 4 These are hydrocarbon radical groups having 1 to 20 carbon atoms, independently of each other. a is 0, 1, or 2, and “ * " indicates a bond for adhesion to the polymer.

[0039] More preferably, R is hydrogen or an alkyl radical group having 1 to 4 carbon atoms, and this alkyl radical group may be linear or branched. Even more preferably, R is H, methyl, or ethyl, and even more preferably hydrogen or methyl.

[0040] R is particularly preferably hydrogen. Comfortable, R 1 and R 2 They are identical. More preferably, R 1 and R 2 R is a hydrogen atom or an alkyl radical group having 1 to 4 carbon atoms, and this alkyl radical group may be linear or branched. More preferably, 1 and R 2 is H, methyl, or ethyl, and more preferably hydrogen or methyl.

[0041] R 1 and R 2 This is particularly preferably hydrogen. Comfortable, R 3 and R 4They are identical. More preferably, R 3 and R 4 R is an alkyl radical group having 1 to 4 carbon atoms, and this alkyl radical group may be linear or branched. More preferably, 3 and R 4 It is methyl or ethyl.

[0042] R 3 and R 4 It is particularly preferably methyl. Preferably, a is 0 or 1, and more preferably a is 1.

[0043] An example of at least one alpha-silane-terminated organic polymer is given by formula * It is a polymer having at least one terminal group of -OC(=O)-NH-CH2-Si(CH3)(OCH3)2.

[0044] The organic polymer is preferably a polyoxyalkylene, hydrocarbon polymer, polyurethane, polyester, polyamide, polysiloxane, polyacrylate, polymethacrylate, or polycarbonate. Polyoxyalkylene is preferred. The organic polymer preferably does not contain silane groups other than the terminal groups described above.

[0045] Preferred polyoxyalkylenes are polypropylenes having a number-average molecular weight in the range of, for example, 5000 g / mol to 50000 g / mol, more preferably 7500 g / mol to 30000 g / mol, and more preferably 10000 g / mol to 15000 g / mol.

[0046] The reactive one-component adhesive composition according to the present invention may further comprise at least one silicone resin. Therefore, there may be one or more different silicone resins, such as two, three, or four types. Preferably, there is only one silicone resin. Such a silicone resin is different from the alpha-silane-terminated organic polymer contained in component a).

[0047] Preferably, it is a phenyl silicone resin. Silicone resins are described, for example, in DE102013213835A1. If the silicone resin is not one of the components described above, it is considered a further component in the context of the present invention.

[0048] Therefore, the silicone resin described in DE102013213835A1 may contain the units of the following formula.

[0049] R 3’ c’ (R 4’ O) d’ R 5’ e’ SiO (4-c’-d’-e’) / 2 (II) During the ceremony, R 3’ These may be the same or different, and are either a hydrogen atom, a monovalent, SiC-bonded, optionally substituted aliphatic hydrocarbon radical group, or a divalent, optionally substituted aliphatic hydrocarbon radical group bridging two units of formula (II). R 4’ These may be the same or different, and are either a hydrogen atom or a monovalent, optionally substituted hydrocarbon radical group. R 5’ These may be the same or different, and are monovalent, SiC-bonded, and optionally substituted aromatic hydrocarbon radical groups. c' is 0, 1, 2, or 3. d' is 0, 1, 2, or 3, preferably 0, 1, or 2, more preferably 0 or 1. e' is 0, 1, or 2, preferably 0 or 1. However, the sum of c'+d'+e' is less than 3 or equal to 3, e' is non-zero in at least one unit, and the sum of c'+e' is 0 or 1 in at least 40% of the units of equation (II).

[0050] A suitable silicone resin is preferably composed of at least 90% by weight of units of formula (II), and more preferably composed solely of units of formula (II).

[0051] Radical group R 3’ Examples include alkyl radical groups such as methyl, ethyl, n-propyl, isopropyl, 1-n-butyl, 2-n-butyl, isobutyl, tert-butyl, n-pentyl, isopentyl, neopentyl, and tert-pentyl radical groups; hexyl radical groups such as n-hexyl radical groups; heptyl radical groups such as n-heptyl radical groups; octyl radical groups such as n-octyl radical groups and isooctyl radical groups, and 2,2,4-trimethylpentyl radical groups; nonyl radical groups such as n-nonyl radical groups; decyl radical groups such as n-decyl radical groups; and dodecyl radical groups such as n-dodecyl radical groups. These include octadecyl radical groups such as n-octadecyl radical groups; cycloalkyl radical groups such as cyclopentyl, cyclohexyl, cycloheptyl radical groups, and methylcyclohexyl radical groups; alkenyl radical groups such as vinyl, 1-propenyl, and 2-propenyl radical groups; aryl radical groups such as phenyl, naphthyl, anthryl, and phenanthryl radical groups; alkaryl radical groups such as o-, m-, and p-tolyl radical groups; xylyl radical groups and ethylphenyl radical groups; and aralkyl radical groups such as benzyl radical groups and o- and β-phenylethyl radical groups.

[0052] Substituted radical group R 3’ Examples include haloalkyl radical groups such as the 3,3,3-trifluoro-n-propyl radical group, the 2,2,2,2',2',2'-hexafluoroisopropyl radical group, and the heptafluoroisopropyl radical group, as well as haloaryl radical groups such as the o-, m-, and p-chlorophenyl radical groups.

[0053] Radical group R 3’The radical group R preferably comprises a monovalent hydrocarbon radical group having 1 to 6 carbon atoms and optionally substituted with halogen atoms, more preferably an alkyl radical group having 1 or 2 carbon atoms, particularly a methyl radical group. 3’ Alternatively, it may comprise a divalent aliphatic radical group that mutually bonds two silyl groups of formula (II), such as an alkylene radical group having 1 to 10 carbon atoms, such as a methylene, ethylene, propylene, or butylene radical group.

[0054] However, radical group R 3’ Preferably, it comprises a monovalent aliphatic hydrocarbon radical group having 1 to 18 carbon atoms and optionally substituted with a halogen atom, more preferably an aliphatic hydrocarbon radical group having 1 to 6 carbon atoms, and particularly a methyl radical group.

[0055] Radical group R 4’ Examples include a hydrogen atom or a radical group R 3’ This is an example that explicitly states this.

[0056] Radical group R 4’ Preferably, it comprises an alkyl radical group having 1 to 10 carbon atoms, which is a hydrogen atom or optionally substituted with a halogen atom, more preferably an alkyl radical group having 1 to 4 carbon atoms, and particularly methyl and ethyl radical groups.

[0057] Radical group R 5’ An example is R 3’ This refers to the aromatic radical group described above. Radical group R 5’ Preferably, it comprises an aromatic hydrocarbon radical group having 1 to 18 carbon atoms and optionally substituted with a halogen atom, such as an ethylphenyl, toluyl, xylyl, chlorophenyl, naphthyl, or styryl radical group, more preferably a phenyl radical group, which is SiC bonded.

[0058] Preferably, all radical groups R 3’ At least 90% of them are methyl radical groups, and all radical groups R 4’ At least 90% of the radical groups are methyl, ethyl, propyl, or isopropyl radical groups, and all radical groups R 5’ A silicone resin is used in which at least 90% of the groups are phenyl radical groups.

[0059] A preferred silicone resin is one in which, based on the total number of units of formula (II), c' in formula (II) is 0 for at least 40%, more preferably at least 60%.

[0060] Preferably, in either case, a silicone resin is used in which the value of d' in formula (II) is 0 or 1 for at least 70%, more preferably at least 80%, of the units of formula (II), based on the total number of units in formula (II).

[0061] Preferably, in any case, based on the total number of units of formula (II), a silicone resin is used in which the value of e' in formula (II) is 1 for at least 20%, more preferably at least 40%, of the units of formula (II). It is also possible to use a silicone resin having only units of formula (II) in which e' is 1, but it is particularly preferable that e' is 0 for at least 10%, more preferably at least 20%, up to 60%, and more preferably up to 80% of the units of formula (II).

[0062] Preferably, in any case, a silicone resin is used in which the sum of c'+e' is 1 in at least 50%, more preferably at least 70%, and especially at least 80% of the units of formula (II), based on the total number of units of formula (II).

[0063] In a particularly preferred embodiment of the present invention, in all cases, based on the total number of units of formula (II), a silicone resin is used in which the value of e' is 1 and the value of c' is 0 in at least 20%, more preferably at least 40% of the units of formula (II). Preferably, in this case, in at most 40%, more preferably in at most 70% of all the units of formula (II), d' is other than 0.

[0064] In an even more particularly preferred embodiment of the present invention, the silicone resin used is, in all cases, based on the total number of units of formula (II), in at least 20%, more preferably at least 40% of the units of formula (II), the value of e' in the formula is 1 and the value of c' is 0, and in at least 1%, preferably at least 10% of the units of formula (II), c' in the formula is 1 or 2, preferably 1, and e' is 0.

[0065] Examples of silicone resins are the (Q) units of formula SiO 4 / 2 , Si(OR 4’ )O 3 / 2 , Si(OR 4’ )2O 2 / 2 , and Si(OR 4’ )3O 1 / 2 , the (T) units of formula PhSiO 3 / 2 , PhSi(OR 4’ )O 2 / 2 , PhSi(OR 4’ )2O 1 / 2 , MeSiO 3 / 2 , MeSi(OR 4’ )O 2 / 2 , and MeSi(OR 4’ )2O 1 / 2 , the (D) units of formula Me2SiO 2 / 2 , Me2Si(OR 4’ )O 1 / 2 , Ph2SiO 2 / 2 and Ph2Si(OR 4’ )O 1 / 2 , MePhSiO 2 / 2 , and MePhSi(OR 4’ )O 1 / 2 , and the units of formula Me3SiO 1 / 2An organopolysiloxane resin substantially consisting of (M) units, preferably consisting only of these, wherein Me is a methyl radical group, Ph is a phenyl radical group, and R 4’ The group comprises a hydrogen atom, or an alkyl radical group having 1 to 10 carbon atoms and optionally substituted with a halogen atom, more preferably a hydrogen atom or an alkyl radical group having 1 to 4 carbon atoms, and the resin contains 0 to 2 moles of (Q) units, 0 to 2 moles of (D) units, and 0 to 2 moles of (M) units per mole of (T) units.

[0066] A preferred example of a silicone resin is one with the formula PhSiO 3 / 2 PhSi(OR 4’ )O 2 / 2 , and PhSi(OR 4’ )2O 1 / 2 T units, formula MeSiO 3 / 2 , MeSi(OR 4’ )O 2 / 2 , and MeSi(OR 4’ )2O 1 / 2 The T units and the formula Me2SiO 2 / 2 and Me2Si(OR 4’ )O 1 / 2 An organopolysiloxane resin substantially consisting of, preferably only, D units of, the formula, where Me is a methyl radical group, Ph is a phenyl radical group, and R 4’ (T) is a hydrogen atom, or optionally substituted with a halogen atom, and comprises an alkyl radical group having 1 to 10 carbon atoms, more preferably a hydrogen atom or an alkyl radical group having 1 to 4 carbon atoms, and the molar ratio of (T) units to (D) units is 0.5 to 2.0.

[0067] Among these examples, it is particularly preferable that at least 50%, preferably at least 70%, and especially at least 85% of the units of formula (II) be of the formula PhSiO 3 / 2 PhSi(OR 4’ )O 2 / 2 PhSi(OR 4’ )2O 1 / 2 MeSiO 3 / 2, MeSi(OR 4’ )O 2 / 2 , and MeSi(OR 4’ )2O 1 / 2 A silicone resin formed in units of T, of the formula PhSiO 3 / 2 PhSi(OR 4’ )O 2 / 2 , and PhSi(OR 4’ )2O 1 / 2 The T units of MeSiO are at least 30%, preferably at least 40%, and especially at least 50%. 3 / 2 , MeSi(OR 4’ )O 2 / 2 , and MeSi(OR 4’ )2O 1 / 2 The silicone resin contains at least 10%, preferably at least 15%, and especially at least 20% of the T units.

[0068] The silicone resin preferably has an average molar mass (number average) Mn of at least 500 g / mol, more preferably at least 600 g / mol. The average molar mass Mn is preferably at most 400,000 g / mol, more preferably at most 100,000 g / mol, and particularly at most 50,000 g / mol.

[0069] Such silicone resins may be solid or liquid at 23°C and 1000 hPa, and the silicone resin is preferably liquid.

[0070] The silicone resin can be a commercially available, conventional product (for example, Silres® IC 368 from Wacker Chemie (Germany)) or it can be prepared by conventional methods in silicon chemistry.

[0071] The reactive one-component adhesive composition according to the present invention further comprises at least one heat accelerator. Therefore, it may contain one heat accelerator. Alternatively, it may contain two or more heat accelerators, such as two, three, or four types.

[0072] Heat accelerators are described in the prior art, for example, DE60116825T2.

[0073] At least one heat accelerator is preferably the following formula (II) where n is an integer from 1 to 3:

[0074] [ka]

[0075] The bicyclic tertiary amine or a salt thereof. Particularly preferred is at least one heat accelerator being DBU(1,8-diazabicyclo[5.4.0]undeca-7-ene) or a salt thereof.

[0076] Preferably, a salt of a bicyclic tertiary amine, particularly a salt of a bicyclic tertiary amine and an aliphatic monocarboxylic acid, is used, the monocarboxylic acid is preferably selected from the group consisting of methacrylic acid, crotonic acid, and tiglic acid, and the mixing ratio is preferably established such that the molar ratio of the bicyclic tertiary amine to the aliphatic monocarboxylic acid is at most 1.3.

[0077] In particular, crotonic acid salts of DBU are preferred.

[0078] The reactive one-component adhesive composition according to the present invention further comprises at least one low molecular weight silane containing a primary or secondary, preferably primary, amino group, or a blocked amino group that becomes a primary or secondary amino group upon hydrolysis. Thus, component d) may comprise one or more such silanes, such as two, three, or four. Preferably, component d) consists of only one component. Unlike components a) to c), component d) is included in component d) only if it cannot be interpreted as one of components a) to c).

[0079] At least one low molecular weight silane of component d) has a primary amino group -NH2. This amino group may be part of a functional group such as an amide group -C(=O)NH2, or it may be a primary amine in the narrow sense. Advantageously, it is an amine. Alternatively, a low molecular weight silane having a secondary amino group may be used. Blocked aminosilanes may also be used. In such cases, the blocked amino group is hydrolyzed to a primary or secondary amino group, preferably a primary amino group. An example is ((triethoxysilyl)propyl)methylisobutylimine, sold by Evonik (Germany) under the trade name VPS 1262. Here, the amino group may be part of a functional group or it may be an amino group, which is preferable. Needless to say, there may be two or more primary amino groups, particularly two or more primary amino groups, two or more secondary amino groups, and at least one primary amino group and at least one secondary amino group. It goes without saying that block forms of primary or secondary amino groups may be present instead. However, preferably, primary or secondary, and more preferably, primary amino groups.

[0080] Advantageous low molecular weight silanes have molecular weights in the range of 100 g / mol to 500 g / mol.

[0081] Preferred low molecular weight silanes are described in DE102012200790A1. Therefore, preferred low molecular weight silanes contain the units of the following formula.

[0082] DSi (OR 7’ ) g’ R 8’ (3-g’) (IX) During the ceremony, R 7’ These may be the same or different, and represent a hydrogen atom or an optionally substituted hydrocarbon radical group. D may be the same or different, and represents a monovalent, SiC-bonded radical group having a primary, secondary, or block amino group basic nitrogen. R 8’ This refers to an organic radical group that is SiC-bonded, monovalent, optionally substituted, and does not contain a base nitrogen, and may be the same or different. g' is 1, 2, or 3, preferably 2 or 3.

[0083] Optionally substituted hydrocarbon radical group R 7’ An example is the radical group R below. 3’ This is an example that explicitly states this.

[0084] Radical group R 7’ Preferably, it comprises a hydrocarbon radical group having 1 to 18 carbon atoms substituted with a hydrogen atom and optionally a halogen atom, more preferably a hydrocarbon radical group having a hydrogen atom and 1 to 10 carbon atoms, particularly methyl and ethyl radical groups.

[0085] Radical group R 8’ An example is shown below in R 3’ This is an example that explicitly states this. Radical group R 8’ The hydrocarbon radical group preferably comprises a hydrocarbon radical group having 1 to 18 carbon atoms and optionally substituted with a halogen atom, more preferably a hydrocarbon radical group having 1 to 5 carbon atoms, and particularly a methyl radical group.

[0086] Examples of radical groups D are given by the formulas H2N(CH2)3-, H2N(CH2)2NH(CH2)3-, H2N(CH2)2NH(CH2)2NH(CH2)3-, H3CNH(CH2)3-, C2H5NH(CH2)3-, C3H7NH(CH2)3-, C4H9NH(CH2)3-, and C5H 11 NH(CH2)3-, C6H 13 NH(CH2)3-, C7H 15NH(CH2)3-, H2N(CH2)4-, H2N-CH2-CH(CH3)-CH2-, H2N(CH2)5-, Cyclo-C5H9NH(CH2)3-, Cyclo-C6H 11 NH(CH2)3-, phenyl-NH(CH2)3-, (CH3)2N(CH2)3-, (C2H5)2N(CH2)3-, (C3H7)2NH(CH2)3-, (C4H9)2NH(CH2)3-, (C5R 11 )2NH(CH2)3-,(C6H 13 )2NH(CH2)3-,(C7H 15 )2NH(CH2)3-, H2N(CH2)-, H2N(CH2)2NH(CH2)-, H2N(CH2)2NH(CH2)2NH(CH2)-, H3CNH(CH2)-, C2H5NH(CH2)-, C3H7NH(CH2)-, C4H9NH(CH2)-, C5H 11 NH(CH2)-, C6H 13 NH(CH2)-, C7H 15 NH(CH2)-, Cyclo-C5H9NH(CH2)-, Cyclo-C6H 11 NH(CH2)-, phenyl-NH(CH2)-, (CH3)2N(CH2)-, (C2H5)2N(CH2)-, (C3H7)2NH(CH2)-, (C4H9)2NH(CH2)-, (C5H 11 )2NH(CH2)-,(C6H 13 )2NH(CH2)-,(C7H 15 The radical groups of )2NH(CH2)-, (CH3O)3Si(CH2)3NH(CH2)3-, (C2H5O)3Si(CH2)3NH(CH2)3-, (CH3O)2(CH3)Si(CH2)3NH(CH2)3-, and (C2H5O)2(CH3)Si(CH2)3NH(CH2)3-, as well as the reaction products of the above-mentioned primary amino groups with compounds containing epoxide groups or double bonds that are reactive with primary amino groups (i.e., contain blocked amino groups).

[0087] Examples of silanes of formula (IX) are H2N(CH2)3-Si(OCH3)3, H2N(CH2)3-Si(OC2H5)3, H2N(CH2)3-Si(OCH3)2CH3, H2N(CH2)3-Si (OC2H5)2CH3, H2N(CH2)2NH(CH2)3-Si(OCH3)3, H2N(CH2)2NH(CH2)3-Si(OC2H5)3, H2N(CH2)2NH(CH2)3-Si (OCH3)2CH3, H2N(CH2)2NH(CH2)3-Si(OC2H5)2CH3, H2N(CH2)2NH(CH2)3-Si(OH)3, H2N(CH2)2NH(CH2)3-Si (OH)2CH3, H2N(CH2)2NH(CH2)2NH(CH2)3Si-(OCH3)3, H2N(CH2)2NH(CH2)2NH(CH2)3-Si(OC2H5)3, cyclo-C6H 11 NH(CH2)3Si-(OCH3)3, Cyclo-C6H 11 NH(CH2)3-Si(OC2H5)3, Cyclo-C6H 11 NH(CH2)3-Si(OCH3)2CH3, Cyclo-C6H 11 NH(CH2)3-Si(OC2H5)2CH3, Cyclo-C6H 11 NH(CH2)3-Si(OH)3, Cyclo-C6H 11 NH(CH2)3-Si(OH)2CH3, Phenyl-NH(CH2)3-Si(OCH3)3, Phenyl-NH(CH2)3-Si(OC2H5)3, Phenyl-NH(CH2)3-Si(OCH3)2CH3, Phenyl-NH(CH2)3-Si(OC2H5)2CH3, Phenyl-NH(CH2)3-Si(OH)3, Phenyl-NH(CH2)3-Si(OH)2CH3, HN((CH2)3-Si(OCH3)3)2, HN((CH2)3-Si(OC2H5)3)2HN((CH2)3-Si(OCH3)2CH3)2, HN((CH2)3-Si(OC2H5)2CH3)2, Cyclo-C6H 11 NH(CH2)-Si(OCH3)3, Cyclo-C6H 11 NH(CH2)-Si(OC2H5)3, Cyclo-C6H 11 NH(CH2)-Si(OCH3)2CH3, Cyclo-C6H 11NH(CH2)-Si(OC2H5)2CH3, Cyclo-C6H 11 NH(CH2)-Si(OH)3, Cyclo-C6H 11 NH(CH2)-Si(OH)2CH3, phenyl-NH(CH2)-Si(OCH3)3, phenyl-NH(CH2)-Si(OC2H5)3, phenyl-NH(CH2)-Si(OCH3)2CH3, phenyl-NH(CH2)-Si(OC2H5)2CH3, phenyl-NH(CH2)-Si(OH)3, and phenyl-NH(CH2)-Si(OH)2CH3, as well as partial hydrolysates thereof, preferably H2N(CH2)2NH(CH2)3-Si(OCH3)3, H2N(CH2)2NH(CH2)3-Si(OC2H5)3, H2N(CH2)2NH(CH2)3-Si(OCH3)2CH3, cyclo-C6H 11 NH(CH2)3-Si(OCH3)3, Cyclo-C6H 11 NH(CH2)3-Si(OC2H5)3, and cyclo-C6H 11 NH(CH2)3-Si(OCH3)2CH3, and partial hydrolysates in each of these cases, particularly preferably H2N(CH2)2NH(CH2)3-Si(OCH3)3, H2N(CH2)2NH(CH2)3-Si(OCH3)2CH3, cyclo-C6H 11 NH(CH2)3-Si(OCH3)3, Cyclo-C6H 11 NH(CH2)3-Si(OCH3)2CH3, and the partial hydrolysates in each of these cases.

[0088] Furthermore, particularly preferred examples include N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, 3-aminopropyltrimethoxysilane, 3-(2-aminoethylamino)propyltriethoxysilane, N-(2-aminoethyl)-3-aminopropyldimethoxysilane, or 3-ureidopropyltrimethoxysilane. Particularly preferred is 3-aminopropyltrimethoxysilane.

[0089] Furthermore, the reactive one-component adhesive composition according to the present invention may further comprise at least one bulking agent. Examples of bulking agents include, for example, calcium carbonate such as chalk, or alumina such as fused alumina.

[0090] The reactive one-component adhesive composition according to the present invention can achieve a high level of filling, which can be advantageous in various applications. Examples that can be cited here include applications that require good thermal conductivity or that require special conditions in terms of combustion behavior.

[0091] The reactive one-component adhesive composition according to the present invention can be used, for example, to manufacture sandwich-type elements. Formulations using a heat accelerator in the reactive one-component adhesive composition according to the present invention have been shown to be processable in a few minutes at room temperature, and as a result, the pressing time under high temperature conditions above about 60°C can be reduced. The use of amines as catalysts is described, for example, in WO2019 / 004922A1 for two-component coatings. Toyocat® DB 40, a known commercial product, is a blocked amine and is described, for example, in DE102016200704A1.

[0092] Furthermore, the reactive one-component adhesive composition according to the present invention may also include a water-scavenging agent such as vinyltrimethoxysilane.

[0093] To reduce the PCS value (heat of combustion), the reactive one-component adhesive composition according to the present invention may include the above-mentioned fillers, such as chalk. The use of at least one silicone resin can promote a lower heat generation.

[0094] In the curing of the reactive one-component adhesive composition according to the present invention, methanol is removed by a condensation reaction that forms a siloxane group.

[0095] In the method according to the present invention, the reactive one-component adhesive composition according to the present invention can be applied to a substrate by conventional techniques such as toothed spatula application, bead application, spray application, or slot die application, optionally sprayed with water, and then pressed at a temperature of, for example, at 60°C. The reactive one-component adhesive composition according to the present invention is particularly suitable for the manufacture of roof linings or panels in the automotive sector. The reactive one-component adhesive composition according to the present invention is particularly suitable for sandwich-type elements in which aluminum plates are used. Mineral wool panels, especially those having a stainless steel outer ply, are also suitable in the context of the present invention.

[0096] Therefore, the present invention also relates to a method according to the present invention for obtaining a bonded substrate system by joining two substrates, and to a substrate system according to the present invention comprising a roof lining or panel in the automotive field. Furthermore, the system may preferably be a sandwich-type element in which aluminum plates are used in particular. Preferred panels are mineral wool panels, particularly those having a stainless steel outer ply.

[0097] Furthermore, the present invention is particularly suitable for aluminum plates or stainless steel plates that are difficult to join, and is also very suitable for steel sheet outer plies that are easy to join, for example, with or without coating.

[0098] Therefore, the present invention also relates to a method according to the present invention for obtaining a bonded substrate system by joining two substrates, and to a substrate system according to the present invention in which at least the first or second substrate is an aluminum plate or a stainless steel plate, or a coated or uncoated steel sheet outer ply.

[0099] Remarkably, after just 2-3 minutes, it achieves a strength nearly equivalent to that of industrially used 1K and 2K polyurethane adhesives. [Examples]

[0100] Examples Example 1 of the adhesive formulation according to the present invention: 180 g of Geniosil STP-E10, 120 g of Silres 368, and 15 g of Dynasylan VTMO were added to a planetary mixer equipped with a butterfly stirrer. Subsequently, 700 g of CALCIT MX 30 was gradually added, and the mixture was stirred to thoroughly disperse the filler. This mixture was stirred at room temperature and under reduced pressure (50 mbar) for 30 minutes. Then, 15 g of vinyltrimethoxysilane, 4 g of the accelerator from Example 3 of DE60116825T2 (a mixture of DBU and crotonic acid), and 20 g of Geniosil GF95 were added, and the mixture was stirred for a further 5 minutes under reduced pressure (50 mbar) (see Table 1).

[0101] [Table 1]

[0102] The physicochemical properties of the resulting formulation are listed in Table 2.

[0103] [Table 2]

[0104] *) The film formation time is confirmed by pressing a wooden spatula into the adhesive bead and then lifting it out at 23°C and 50% relative humidity. Repeat this procedure every 60 seconds until the wooden spatula is no longer moist with adhesive.

[0105] Example 1 of the method according to the present invention (manufacturing of roof lining for an automobile): Approximately 100 g / m² of the adhesive from Example 1 of the invention described above. 2 Apply to a rigid foam-like material and add water at a rate of approximately 35 g / m². 2The adhesive is sprayed. The assembly, consisting of further fiberglass mats and fabrics produced from this system, is pressed at 120°C for 40 seconds. After the pressing time, the adhesive strength in the peel test is slightly stronger than the inherent strength of the foam material, indicating that the adhesive has penetrated the entire assembly.

[0106] Example 2 of the method according to the present invention (manufacturing of mineral wool panels): Using a toothed spatula, apply approximately 400 g / m of adhesive from the above-described examples. 2 (Coated) The material is applied to a metal sheet, and approximately 100g of water is sprayed on it, resulting in a density of approximately 110kg / m³. 3 The mineral wool was inserted so that its fibers stood perpendicular to the sheet. This assembly was pressed at 60°C for 3.5 or 4.5 minutes. Immediately after the pressing time, the assembly was pulled apart by hand, and many fibers came out. [Industrial applicability]

[0107] This invention presents an isocyanate-free alternative to reactive polyurethane adhesives used in the current prior art. The resulting strength is comparable to that of polyurethane adhesives. The reactive one-component adhesive composition according to the present invention is particularly suitable for sandwich-type elements using aluminum plates. Mineral wool panels, especially those with stainless steel outer plies, are also suitable in the context of this invention.

[0108] Currently, 2K polyurethane adhesive is used for manufacturing mineral wool panels, which is mixed using low-pressure or high-pressure machinery and applied by spraying or injection. These methods have stringent requirements, are prone to errors, and require investment in expensive machinery.

[0109] For the reactive one-component adhesive composition according to the present invention in Example 1, it was confirmed that the heat of combustion according to EN ISO 1716 was 7.8 MJ / kg. This relatively low value is due to a high proportion of filler, on the one hand, and the proportion of silicone resin, on the other hand. Therefore, the maximum is approximately 500 g / m 2 With this coating rate, it is possible to manufacture mineral wool panels that meet Class A2 of DIN EN 13501:2019-05. Furthermore, the reactive one-component adhesive composition according to the present invention in Example 1 exhibits good heat resistance.

Claims

1. A reactive one-component adhesive composition that is liquid at room temperature, wherein, based on the total weight of the composition, a) At least one alpha-silane-terminated organic polymer in an amount of 3% to 90% by weight, b) At least one silicone resin in an amount of 0% to 50% by weight, c) Formula (II) below, where n is an integer from 1 to 3, ranging from 0.1% by weight to 5% by weight: 【Chemistry 1】 A heat accelerator which is a salt of a bicyclic tertiary amine, d) At least one low molecular weight silane having a molecular weight in the range of 100 to 500 g / mol, having 0.001% to 5% by weight of primary or secondary amino groups or block amino groups that become primary or secondary amino groups upon hydrolysis, e) A composition containing at least one bulking agent in an amount of 0% to 80% by weight.

2. The reactive one-component adhesive composition according to claim 1, characterized in that the at least one alpha-silane-terminated organic polymer has the following formula (I): Y-[(CR １ａ ２ )-Si(R ２ａ ) ｂ１ (OR ３ａ ) ３－ｂ１ ] ｘ (I) During the ceremony, Y is an x-valent polymer radical group bonded via nitrogen, oxygen, or sulfur. R ２ａ These may be the same or different, and are monovalent, optionally substituted, SiC-bonded hydrocarbon radical groups. R １ａ may be the same or different and is a monovalent, optionally substituted hydrocarbon radical group which may be a hydrogen atom or may be attached to a carbon atom via a nitrogen, phosphorus, oxygen, sulfur or carbonyl group, R ３ａ These may be the same or different, and are either a hydrogen atom or a monovalent, optionally substituted hydrocarbon radical group. x is an integer between 1 and 10. b1 may be the same or different, and is 0, 1, or 2.

3. The at least one alphasilane-terminated organic polymer is, ＊ -X-C(=O)-N(R)-C(R １ R ２ )-Si(R ３ ) ａ (OR ４ ) ３－ａ It has at least one terminal group, in the formula, X is either O or N(R), Each R is independently either a hydrogen atom or a hydrocarbon radical group having 1 to 20 carbon atoms. R １ and R ２ These are, independently of each other, hydrogen or hydrocarbon radical groups having 1 to 20 carbon atoms. R ３ and R ４ These are hydrocarbon radical groups having 1 to 20 carbon atoms, independently of each other. a is 1 or 2, and " ＊ The reactive one-component adhesive composition according to claim 1 or 2, characterized in that it exhibits a bond for adhering to the polymer.

4. The reactive one-component adhesive composition according to any one of claims 1 to 3, characterized in that the at least one organic polymer is a polyoxyalkylene, a hydrocarbon polymer, a polyurethane, a polyester, a polyamide, a polysiloxane, a polyacrylate, a polymethacrylate, or a polycarbonate.

5. The reactive one-component adhesive composition according to any one of claims 1 to 4, characterized in that the at least one organic polymer is a polyoxyalkylene.

6. The reactive one-component adhesive composition according to any one of claims 1 to 5, characterized in that the at least one of the silicone resins is a phenyl silicone resin.

7. The reactive one-component adhesive composition according to any one of claims 1 to 6, characterized in that the salt of the bicyclic tertiary amine is a salt with an aliphatic monocarboxylic acid.

8. The reactive one-component adhesive composition according to claim 7, characterized in that the salt is a salt of DBU.

9. The reactive one-component adhesive composition according to any one of claims 1 to 8, characterized in that the at least one heat accelerator is a crotonic acid salt of DBU.

10. Based on the total weight of the aforementioned composition, a) 3% to 50% by weight of at least one alphasilane-terminated organic polymer, b) At least one of the silicone resins in an amount of 1% to 30% by weight, c) 0.1% to 2.5% by weight of at least one of the heat accelerators, d) 0.01% to 5% by weight of at least one low molecular weight silane having a primary or secondary amino group or a block amino group that becomes a primary or secondary amino group upon hydrolysis, e) A reactive one-component adhesive composition according to any one of claims 1 to 9, characterized by containing 10% to 80% by weight of at least one of the above-mentioned bulking agents.

11. Based on the total weight of the aforementioned composition, a) 5% to 25% by weight of at least one alphasilane-terminated organic polymer, b) 5% to 20% by weight of at least one of the silicone resins, c) 0.1% to 1% by weight of at least one of the heat accelerators, d) 0.1% to 4% by weight of at least one low molecular weight silane having a primary or secondary amino group or a block amino group that becomes a primary or secondary amino group upon hydrolysis, e) A reactive one-component adhesive composition according to any one of claims 1 to 10, characterized by containing 30% to 80% by weight of at least one of the above-mentioned bulking agents.

12. Based on the total weight of the aforementioned composition, a) 15% to 25% by weight of at least one alpha-silane-terminated organic polymer, b) 10% to 12% by weight of at least one of the silicone resins, c) 0.2% to 0.5% by weight of at least one of the heat accelerators, d) 1% to 3% by weight of at least one low molecular weight silane having a primary or secondary amino group or a block amino group that becomes a primary or secondary amino group upon hydrolysis, e) A reactive one-component adhesive composition according to any one of claims 1 to 11, characterized by containing 59.5% to 73.8% by weight of at least one of the bulking agents.

13. A method for joining two substrates, (a) A step of applying the reactive one-component adhesive composition according to any one of claims 1 to 12 to a first substrate to provide an adhesive area, (b) A step of bringing a second substrate into contact with the adhesive area from step (a), (c) A method comprising the step of heat-curing the adhesive composition.

14. A bonding substrate system comprising two substrates, wherein the two substrates have a common adhesive region, and in the common adhesive region, the two substrates are bonded together by the use of an adhesive composition according to any one of claims 1 to 12 that has been heat-cured.

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