Pumpable one-component adhesive composition

Abstract

The present invention relates to a curable one-component adhesive composition comprising (a) a liquid epoxy resin; (b) a latent epoxy curing agent; (c) silica; and (d) a metal oxide; wherein the weight content of the liquid epoxy resin is at least 20 wt.-% based on all the liquid epoxy resin contained in the composition and relative to the total weight of the one-component adhesive composition.

Description

[0001] Claiming priority from European patent application no. 22 190 696.9 filed on August 17, 2023.

[0002] The present invention relates to a curable one-component adhesive composition comprising (a) a liquid epoxy resin; (b) a latent epoxy curing agent; (c) silicon dioxide; and (d) a metal oxide; wherein the weight content of the liquid epoxy resin is at least 20 wt-%., based on all the liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0003] Epoxy paste adhesives are widely used in various technologies, for example in vehicle construction. Epoxy paste adhesives may contain various additives, such as curing agents, blowing agents, toughening agents, impact modifiers, fillers, etc. These epoxy paste adhesives are usually applied to the substrate in an uncured state, for example automatically, and activated (e.g. heated) at a later stage of manufacturing to achieve curing.

[0004] Epoxy paste adhesives need to exhibit good rheological properties to allow easy handling and application, for example by automated equipment. Good pumpability at low temperatures is particularly desirable. Epoxy paste adhesives should also be designed to withstand relatively high temperatures.

[0005] Prior to curing, epoxy paste adhesives need to withstand the various conditions they are commonly exposed to. Once the epoxy paste adhesive is applied to a substrate, such as a metal panel of a vehicle, the epoxy paste adhesive should adhere adequately to the surface of the substrate and not sag.

[0006] During further processing, for example after possible further construction steps have been carried out, the entire vehicle component is usually subjected to a series of sprays and baths for various purposes. Some treatments remove oil or dirt, other treatments provide corrosion resistance by applying a protective coating from a liquid bath. During these processing steps, the epoxy paste adhesive so applied is still present in its uncured state and needs to remain on the substrate. In particular, it may be difficult to achieve satisfactory properties when the substrate surface to which the epoxy paste adhesive has been applied is exposed to washing or dipping operations. If the epoxy paste adhesive cannot withstand these conditions, the epoxy paste adhesive will be "washed off" from the vehicle component and this is to be avoided. It must be ensured that after such washing or dipping operations, the adhesive bonding quality is not reduced and the washing or dipping liquid is not contaminated by the constituent components of the epoxy paste adhesive.

[0007] EP 0 899 300 A2 relates to an epoxy resin type composition comprising an epoxy resin, 100 parts by weight; a powdered methacrylate type polymer, 2 to 45 parts; a thermally active hardener, 1 to 20 parts; a thermally decomposable foaming agent, 0.5 to 20 parts; and a mixture comprising an inorganic salt having a predetermined aspect ratio and a granular inorganic salt, the mixture totaling 50 to 200 parts.

[0008] CN 110 885 656A relates to an amorphous sealant for automobiles and a preparation method thereof, wherein the amorphous sealant for automobiles comprises the following raw materials in percentage by weight: 20-30% of butadiene rubber, 20-30% of epoxy resin, 15-25% of inorganic flame retardant, 15-25% of wollastonite powder, 1.5-3% of crosslinking agent, 1-3% of crosslinking auxiliary agent and 2-4% of epoxy auxiliary agent.

[0009] US 2004 266899 A1 relates to expandable thermosetting compositions comprising at least one epoxy resin, at least one finely divided thermoplastic polymer powder, at least one blowing agent, at least one curing agent and at least one filler, said composition being suitable for producing thermosetting laminates having an adhesive surface.

[0010] US2006 188726A1 relates to a composition comprising at least one liquid epoxy resin, at least one solid epoxy resin, at least one propellant, at least one curing agent and at least one mica-containing filler, for producing an expandable, heat-curable adhesive system which can be used for producing reinforced and reinforced laminates and for producing reinforced and reinforced moldings without the addition of hollow glass beads.

[0011] US2009 0065143A1 relates to a two-component epoxy adhesive composition comprising a) a first component comprising a first epoxy resin and a second epoxy resin, the second epoxy resin being toughened by an elastomer, and b) a second component comprising at least one amine compound having one or more primary and / or secondary amino groups, the amine compound having a molecular weight of less than 450 g / mol. The mixing of the two components a) and b) produces a wash-off resistant composition. The wash-off resistant composition produces a crash stable structural adhesive when thermally cured.

[0012] US2010 0272908A1 relates to compositions useful as adhesives and more particularly to the preparation of heat-curable epoxy-based adhesive compositions that resist being washed off a substrate surface prior to curing.

[0013] US2011036497A1 relates to compositions useful as adhesives and more particularly to the preparation of heat-curable epoxy-based adhesive compositions that can be easily pumped under high shear at temperatures around room temperature but resist being washed off the substrate surface prior to curing.

[0014] US 2012 0207925 A1 relates to a two-component premix for preparing a heat-expandable and heat-curable epoxy-based material, which comprises an isocyanate, a diol or a polyol, an epoxy prepolymer, a heat-activatable hardener for the epoxy prepolymer and a heat-activatable blowing agent.

[0015] US2013 0149531A1 relates to adhesive materials and articles incorporating the same. The adhesive material comprises liquid epoxy resin and rubber, solid epoxy resin and rubber, one or more curing agents, and fillers.

[0016] US2016 0244603A1 relates to a curable resin composition comprising 1 to 100 parts by mass of polymer fine particles (B) relative to 100 parts by mass of epoxy resin (A), wherein the polymer fine particles have a core-shell structure, the core layer of the polymer fine particles is a diene rubber, and the content of epoxy groups in the polymer fine particles (B) is 0.01 to 0.2 mmol / g.

[0017] US2018 037708A1 relates to a pumpable thermally foamable filler composition based on a combination of a liquid epoxy resin and a polyvinyl chloride resin and / or an acrylic resin powder.

[0018] US2018 / 258329 A1 relates to a one-component toughened epoxy structural adhesive comprising a fibrous mineral filler having an aspect ratio ≥ 6. The presence of the fibrous filler is said to result in an increase in the elastic modulus with little adverse effect on other properties such as dynamic impact peel resistance.

[0019] US2020 0095418A1 relates to a curable composition comprising a diluent, an epoxy-functional resin derived from nutshell oil, an epoxy-rubber copolymer adduct and a curing agent.

[0020] US2020 0231849A1 relates to an epoxy-based crash-resistant adhesive composition which is pumpable at temperatures above 15°C; and exhibits improved wash-off resistance.

[0021] WO 2020 / 097050 A1 relates to a reinforcing patch for reinforcing a vehicle panel. The reinforcing patch may be fabric-free (e.g., without any reinforcing layer). The reinforcing patch may be cut into small shapes, complex shapes, or both. The reinforcing material may be mesh-free or fabric-free, which may allow the reinforcing patch material to be easily produced and easily reprocessed. The reinforcing patch may include one or more reinforcing particles combined with one or more discontinuous fiber components to obtain a stiffness comparable to that of a conventional patch including a mesh / fabric layer.

[0022] US2020 / 231849 A1 relates to an epoxy-based crash-resistant adhesive composition comprising: (I) a liquid resin system comprising: (a) at least one epoxy resin; and (b) at least one toughening agent; wherein the viscosity of the liquid resin system is less than about 800 Pa·s at a temperature of 15°C; and wherein the viscosity of the liquid resin system is greater than about 5 Pa·s at a temperature of 60°C; (II) a solid material comprising: (c) at least one hydrophobic fumed silica, wherein the fumed silica is present in the adhesive composition at a concentration greater than 5 weight percent; and (III) a curable material comprising: (d) at least one latent heat-activated curing agent; wherein the rheology of the epoxy-based crash-resistant adhesive composition is such that the adhesive composition is pumpable at a temperature above 15°C. The epoxy-based crash-resistant adhesive composition is said to exhibit an increase in wash-off resistance.

[0023] Epoxy paste adhesives known in the prior art are not satisfactory in every respect. Several known epoxy paste adhesives do not provide acceptable wash-off resistance and are not pumpable at low temperatures.

[0024] The object of the present invention is to provide a pumpable curable one-component adhesive composition having advantages over the curable one-component adhesive compositions of the prior art. The pumpable curable one-component adhesive composition should be resistant to washing off and aging. The pumpable curable one-component adhesive composition should provide excellent adhesion after curing and should be processable by conventional equipment. Pumpability should allow application to a substrate by means of conventional pumping and application equipment such as an automated dispenser.

[0025] This object has been achieved by the subject matter of the patent claims.

[0026] Surprisingly it has been found that silica, preferably fumed silica, and metal oxide, preferably calcium oxide, in particular in combination with one or more silicates, preferably inosilicates and / or layered silicates, provide pumpable, curable one-component adhesive compositions having advantageous properties. Wash-off resistance and aging resistance in terms of lap shear resistance in the humidcataplasma test can be significantly improved.

[0027] A first aspect of the present invention relates to a curable one-component adhesive composition comprising:

[0028] (a) a liquid epoxy resin, preferably comprising or consisting essentially of a liquid glycidyl ether of a bisphenol (e.g., DGEBA, DGEBF, etc.), a liquid epoxy novolac resin, or a combination thereof;

[0029] (b) a latent epoxy curing agent; preferably dicyandiamide;

[0030] (c) silica; preferably fumed silica; more preferably polydimethylsiloxane-treated fumed silica;

[0031] (d) a metal oxide; preferably calcium oxide (CaO);

[0032] (e) optionally, a layered silicate; preferably a clay (eg talc) and / or an organophilic layered silicate; and

[0033] (f) optionally, an inosilicate; preferably wollastonite;

[0034] The weight content of the liquid epoxy resin is at least 20 wt.-%, preferably at least 30 wt.-%, more preferably at least 40 wt.-%, and even more preferably at least 50 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0035] Components (e) and (f) of the composition according to the invention are optional independently of one another, whereas components (a), (b), (c) and (d) are mandatory. In addition to components (a) to (d), the composition according to the invention may comprise additional components or ingredients. In addition to optional components (e) and (f), additional optional components (g) to (p) are further specified below.

[0036] The composition according to the invention is a one-component composition. Therefore, the composition according to the invention is preferably a ready-to-use composition that already contains all the ingredients required for the desired purpose. In particular, before use, the composition according to the invention preferably does not require the addition of any other additives, nor does it need to be mixed with other compositions.

[0037] The composition according to the invention is curable, i.e., capable of undergoing a curing reaction autonomously after an appropriate stimulus, preferably by heating to an elevated temperature, usually by crosslinking. Partial curing or curing, i.e., complete curing, can be achieved by reacting one or more components contained in the composition with each other to form covalent bonds. The activation temperature for inducing curing is usually in the range of 80 to 210° C., preferably 120 to 160° C. The activation temperature can be adjusted by conventional means known to those skilled in the art. It is known that latent curing agents activate at different temperatures and react with epoxy resins, preferably glycidyl ethers of bisphenols and epoxy novolac resins, etc. The activation temperature can be further adjusted by a curing accelerator, which usually lowers the activation temperature.

[0038] The present invention provides a fast curing one-component adhesive.

[0039] In a preferred embodiment, the list of optional components that can be included in the composition according to the present invention extends from (e) and (f) to (g) to (p). Preferably, optionally, the curable one-component adhesive composition additionally comprises one or more of the following components (e) to (p):

[0040] (d) a metal oxide; preferably calcium oxide (CaO);

[0041] (e) a layered silicate; preferably a clay (e.g. talc) and / or an organophilic layered silicate; more preferably strontium zinc phosphosilicate;

[0042] (f) inosilicate; preferably wollastonite;

[0043] (g) a reactive diluent; preferably a glycidyl ether epoxy resin of cashew nutshell liquid;

[0044] (h) an additional curable epoxy resin; preferably a semi-solid curable epoxy resin;

[0045] (i) fibers; preferably discontinuous fibers; preferably glass fibers;

[0046] (j) polyhydroxycarboxylates;

[0047] (k) polyamides;

[0048] (l) a blowing agent; preferably a chemical blowing agent; more preferably azodicarbonamide;

[0049] (m) impact modifier;

[0050] (n) toughening agent and / or flexibilizer;

[0051] (o) a phenoxy resin; preferably a solid phenoxy resin; more preferably a solid phenoxy resin which is a copolymer of bisphenol A and epichlorohydrin; and / or

[0052] (p) Curing accelerator.

[0053] Components (e) to (p) of the composition according to the invention are, independently of one another, optional, whereas components (a), (b), (c) and (d) are mandatory.

[0054] In a preferred embodiment, the composition consists essentially of components (a), (b), (c) and (d) and optionally one or more of components (e) to (p).

[0055] In preferred embodiments, the composition comprises or consists essentially of components (a), (b), (c), (d) and (e); (a), (b), (c), (d) and (f); (a), (b), (c), (d) and (g); (a), (b), (c), (d) and (h); (a), (b), (c), (d) and (i); (a), (b), (c), (d) and (j); (a), (b), (c), (d) and (k); (a), (b), (c), (d) and (l); (a), (b), (c), (d) and (m); (a), (b), (c), (d) and (n); (a), (b), (c), (d) and (o); or (a), (b), (c), (d) and (p).

[0056] In preferred embodiments, the composition comprises or consists essentially of components (a), (b), (c), (d), (e) and (f); (a), (b), (c), (d), (e) and (g); (a), (b), (c), (d), (e) and (h); (a), (b), (c), (d), (e) and (i); (a), (b), (c), (d), (e) and (j); (a), (b), (c), (d), (e) and (k); (a), (b), (c), (d), (e) and (l); (a), (b), (c), (d), (e) and (m); (a), (b), (c), (d), (e) and (n); (a ), (b), (c), (d), (e) and (o); or (a), (b), (c), (d), (e) and (p); (a), (b), (c), (d), (f) and (g); (a), (b), (c), (d), (f) and (h); (a), (b), (c), (d), (f) and (i); (a), (b), (c), (d), (f) and (j); (a), (b), (c), (d), (f) and (k); (a), (b), (c), (d), (f) and (l); (a), (b), (c), (d), (f) and (m); (a), (b), (c), (d), (f) and (n); (a), (b), ( c), (d), (g) and (k); (a), (b), (c), (d), (g) and (l); (a), (b), (c), (d), (g) and (m); (a), (b), (c), (d), (g) and (n); (a), (b), (c), (d), (g) and (o); (a), (b), (c), (d), (g) and (h); (a), (b), (c), (d), (g) and (i); (a), (b), (c), (d), (g) and (j); (a), (b), (c), (d), (g) and (k); (a), (b), (c), (d), (g) and (l); (a), (b), (c), (d), (g) and (m); (a), (b), (c), (d), (g) and (n); (a), (b), (c), (d), (g) and (o); (a), (b), (c), (d), (g) and (p); (a), (b), (c), (d), (h) and (i); (a), (b), (c), (d), (h) and (j); (a), (b), (c), (d), (h) and (k); (a), (b), (c), (d), (h) and (l); (a), (b), (c), (d), (h) and (m); (a), (b), (c), (d), (h) and (n); (a), (b), (c), (d), (h) and (o); (a), (b), (c), (d), (h) and (p); (a), (b), (c), (d), (i) and (j); (a), (b), (c), (d), (i) and (k);(a), (b), (c), (d), (i) and (l); (a), (b), (c), (d), (i) and (m); (a), (b), (c), (d), (i) and (n); (a), (b), (c), (d), (i) and (o); (a), (b), (c), (d), (i) and (p); (a), (b), (c), (d), (j) and (k); (a), (b), (c), (d), (i) and (n); ), (c), (d), (j) and (l); (a), (b), (c), (d), (j) and (m); (a), (b), (c), (d), (j) and (n); (a), (b), (c), (d), (j) and (o); (a), (b), (c), (d), (j) and (p); (a), (b), (c), (d), (k) and (l); (a), (b), (c), (d), (k) and (m); (a), (b), (c), (d), (k) and (n); (a), (b), (c), (d), (k) and (o); (a), (b), (c), (d), (k) and (p); (a), (b), (c), (d), (l) and (m); (a), (b), (c), (d), (l) and (n); (a), (b), (c), (d), (l ) and (o); (a), (b), (c), (d), (l) and (p); (a), (b), (c), (d), (m) and (n); (a), (b), (c), (d), (m) and (o); (a), (b), (c), (d), (m) and (p); (a), (b), (c), (d), (n) and (o); or (a), (b), (c), (d), (n) and (p). ;

[0057] Besides components (a) to (p), the composition according to the invention may comprise additional ingredients.

[0058] Unless expressly stated otherwise, all percentages are by weight and are relative to the total weight of the curable one-part adhesive composition.

[0059] Unless explicitly stated otherwise, the official version of any standard, such as EN ISO and ASTM, is valid on 1 July 2022.

[0060] The expression "consisting essentially of" means a content of at least 95 wt.-%, preferably at least 99 wt.-%, relative to the total weight of the defined component.

[0061] The one-component adhesive composition according to the present invention comprises (a) a liquid epoxy resin, preferably comprises or consists essentially of a liquid epoxy novolac resin. The liquid epoxy resin is preferably a room temperature liquid epoxy resin, ie, liquid at room temperature (25° C.).

[0062] Preferably, the weight content of the liquid epoxy resin is at least 30 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0063] In a preferred embodiment, the liquid epoxy resin comprises or consists essentially of a liquid epoxy novolac resin.

[0064] In other preferred embodiments, the liquid epoxy resin comprises or consists essentially of a liquid bisphenol diglycidyl ether resin.

[0065] In yet other preferred embodiments, the liquid epoxy resin comprises or consists essentially of a mixture of a liquid epoxy novolac resin and a liquid bisphenol diglycidyl ether resin.

[0066] Preferably, the content of the liquid epoxy novolac resin is greater than the content of the liquid bisphenol diglycidyl ether resin.

[0067] Preferably, the content of the liquid bisphenol diglycidyl ether resin is greater than the content of the liquid epoxy novolac resin.

[0068] Preferably, the content of the liquid epoxy novolac resin is equal to the content of the liquid bisphenol diglycidyl ether resin.

[0069] Preferably, the liquid epoxy novolac resin is selected from ortho-cresol novolac type, phenol novolac type, BPA-novolac type, DCPD type, neophenol (xylok) type and multifunctional novolac resin; preferably phenol novolac type, ie liquid epoxy phenol novolac resin.

[0070] Epoxy phenol novolac (EPN) resins are epoxy resins in which epoxy functional groups are attached to the phenolic oxygen of a phenol novolac. A single EPN polymer contains many epoxy groups, making the molecule multifunctional. Suitable liquid epoxy phenol novolac (EPN) resins are known to those skilled in the art and are available, for example, under the trade name 424, 425, 426(Olin), EPN 9820,

[0071] EPN 9850 (Huntsman), 8220 and 8250 (Huntsman) and the like are commercially available.

[0072] Preferably, the liquid bisphenol diglycidyl ether resin is selected from the diglycidyl ether resin of bisphenol A or the diglycidyl ether resin of bisphenol F.

[0073] Bisphenol diglycidyl ether resins are epoxy resins in which the epoxy functional groups are attached to the phenolic oxygen of the bisphenol. Suitable liquid bisphenol diglycidyl ether resins are known to those skilled in the art and are available, for example, under the trade name 301, 317, 321, 322, 331,

[0074] 332, 336 (Olin) and 7200 (Huntsman) and the like are commercially available.

[0075] Liquid epoxy resins are generally distinguished from semi-solid epoxy resins and other epoxy resins. The viscosity of liquid epoxy resins is generally measured at 25°C, while the viscosity of semi-solid epoxy resins is generally measured at higher temperatures (52°C or 55°C) or in solution in a suitable solvent.

[0076] Preferably, the liquid epoxy resin (preferably comprising or essentially consisting of a liquid epoxy novolac resin, more preferably a liquid epoxy phenol novolac resin) has an epoxy equivalent as measured according to ASTM D1652 in the range of 145 to 200 g / eq, preferably 160 to 185 g / eq, and more preferably 165 to 178 g / eq.

[0077] Preferably, the liquid epoxy resin (preferably comprising or essentially consisting of a liquid epoxy novolac resin, more preferably a liquid epoxy phenol novolac resin) has a viscosity at 25°C measured according to ASTM D2196 of at most 70 Pa·s, preferably at most 50 Pa·s, more preferably at most 30 Pa·s.

[0078] Preferably, the viscosity of the liquid epoxy resin (preferably comprising or essentially consisting of a liquid epoxy novolac resin, more preferably a liquid epoxy phenol novolac resin) at 25° C. measured according to ASTM D2196 is in the range of 14 to 32 Pa·s, preferably 16 to 30 Pa·s, more preferably 18 to 28 Pa·s.

[0079] Preferably, the liquid epoxy resin (preferably comprising or consisting essentially of a liquid epoxy novolac resin, more preferably a liquid epoxy phenol novolac resin) has an epoxy functionality in the range of 1.3 to 3.9, preferably 1.7 to 3.5, more preferably 2.1 to 3.1.

[0080] Preferably, the weight content of the liquid epoxy resin is at least 32 wt.-%, preferably at least 34 wt.-%, more preferably at least 36 wt.-%, even more preferably at least 38 wt.-%, and still more preferably at least 40 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0081] Preferably, the weight content of the liquid epoxy resin is at most 74 wt.-%, preferably at most 70 wt.-%, more preferably at most 66 wt.-%, still more preferably at most 62 wt.-%, still more preferably at most 58 wt.-%, even more preferably at most 52 wt.-%, most preferably at most 48 wt.-%, and in particular at most 44 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0082] Preferably, the weight content of the liquid epoxy resin is in the range of 40±20 wt.-%, preferably 40±10 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

[0083] The one-component adhesive composition according to the present invention comprises (b) a latent epoxy curing agent. For the purpose of this specification, a latent epoxy curing agent does not spontaneously react with the epoxy resin in a curing reaction under ambient conditions (room temperature, 23°C), but requires a stimulus to induce curing, typically an elevated temperature, preferably at least 80°C, more preferably at least 120°C.

[0084] Preferably, the latent epoxy curing agent is selected from the group consisting of dicyandiamide, aliphatic or aromatic amines or their respective adducts, amidoamines, polyamides, alicyclic amines, acid anhydrides, polycarboxylic acid polyesters, isocyanates, phenolic resins (preferably selected from phenol or cresol novolac resins, copolymers of phenol terpenes, polyvinylphenol, or bisphenol A formaldehyde copolymers, bishydroxyphenylalkanes), modified and unmodified polyamines or polyamides (preferably selected from triethylenetetramine, diethylenetriamine, tetraethylenepentamine and cyanoguanidine); preferably dicyandiamide. Suitable latent epoxy curing agents such as dicyandiamide are known to those skilled in the art and can be obtained, for example, under the trade name 100S was purchased commercially.

[0085] In a particularly preferred embodiment, the latent epoxy curing agent is dicyandiamide.

[0086] Preferably, the weight content of the latent epoxy curing agent relative to the total weight of the one-component adhesive composition is at least 1.4 wt.-%, preferably at least 1.6 wt.-%, more preferably at least 1.8 wt.-%, even more preferably at least 2.0 wt.-%, still more preferably at least 2.2 wt.-%, even more preferably at least 2.4 wt.-%, most preferably at least 2.6 wt.-%, and in particular at least 2.8 wt.-%.

[0087] Preferably, the weight content of the latent epoxy curing agent relative to the total weight of the one-component adhesive composition is at most 4.5 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.8 wt.-%, even more preferably at most 3.6 wt.-%, still more preferably at most 3.4 wt.-%, even more preferably at most 3.2 wt.-%, most preferably at most 3.0 wt.-%, and in particular at most 2.8 wt.-%.

[0088] Preferably, the weight content of the latent epoxy curing agent is in the range of 2.8±1.5 wt.-%, preferably 2.8±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0089] The one-component adhesive composition according to the present invention contains (c) silicon dioxide.

[0090] Preferably, the silica is fumed silica, fused silica, silica gel or quartz; preferably fumed silica; more preferably surface-treated fumed silica; still more preferably hydrophobic fumed silica; still more preferably polydimethylsiloxane-treated fumed silica. Suitable silicas such as fumed silica are known to those skilled in the art and are available, for example, under the trade name Cab-O-Sil 5760、Cab-O-Sil 5780, HDK and etc. are commercially available.

[0091] Preferably, the silica has the form of particles, flakes, platelets, rods, needles and / or rectangles.

[0092] Preferably, the total weight content of silica, relative to the total weight of the one-component adhesive composition, is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%.

[0093] Preferably, the total weight content of silica, relative to the total weight of the one-component adhesive composition, is at most 19 wt.-%, preferably at most 17 wt.-%, more preferably at most 15 wt.-%, even more preferably at most 13 wt.-%, still more preferably at most 11 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 5.0 wt.-%.

[0094] Preferably, the total weight content of silica is in the range of 5.0±3.0 wt.-%, preferably 5.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0095] The one-component adhesive composition according to the present invention contains (d) a metal oxide.

[0096] Preferably, the metal oxide is selected from calcium oxide (CaO), magnesium oxide (MgO), barium oxide (BaO), potassium oxide (K 2 O), lithium oxide (Li 2 O), sodium oxide (Na 2 O) and mixtures thereof; preferably CaO. Suitable metal oxides such as CaO are known to those skilled in the art and are available, for example, under the trade name FG was purchased commercially.

[0097] Preferably, the metal oxide has the form of particles, flakes, platelets, rods, needles and / or rectangles.

[0098] Preferably, the weight content of the metal oxide is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0099] Preferably, the weight content of the metal oxide is at most 20 wt.-%, preferably at most 18 wt.-%, more preferably at most 16 wt.-%, even more preferably at most 14 wt.-%, still more preferably at most 12 wt.-%, even more preferably at most 10 wt.-%, most preferably at most 8.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0100] Preferably, the weight content of the metal oxide is in the range of 5.0±4.0 wt.-%, preferably 5.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0101] The one-component adhesive composition according to the invention optionally comprises (e) a phyllosilicate. As described above, the phyllosilicate forms sheets. Preferred phyllosilicates according to the invention are selected from the serpentine subgroup, clay minerals and the mica group, preferably in any case in organically modified form. Suitable phyllosilicates are known to the person skilled in the art and are available, for example, under the trade name 1958, SZP 391 and SW-111 and the like are commercially available.

[0102] Preferably, the layered silicate has the form of particles, flakes, platelets, rods, needles and / or rectangles.

[0103] Preferably, the layered silicate comprises or consists essentially of one or more clay minerals, preferably talc.

[0104] Preferably, the layered silicate comprises or consists essentially of an organically modified layered silicate; preferably an organophilic layered silicate.

[0105] Preferably, the layered silicate comprises or consists essentially of a phosphosilicate; preferably zinc phosphosilicate; more preferably an organomodified zinc phosphosilicate; still more preferably strontium zinc phosphosilicate.

[0106] Preferably, the total weight content of the layered silicate is at least 0.5 wt.-%, preferably at least 1.0 wt.-%, more preferably at least 1.5 wt.-%, even more preferably at least 2.0 wt.-%, still more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, most preferably at least 3.5 wt.-%, and in particular at least 4.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0107] Preferably, the total weight content of the layered silicate, relative to the total weight of the one-component adhesive composition, is at most 19 wt.-%, preferably at most 17 wt.-%, more preferably at most 15 wt.-%, even more preferably at most 13 wt.-%, still more preferably at most 11 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 5.0 wt.-%.

[0108] Preferably, the total weight content of the layered silicate is in the range of 4.0±3.0 wt.-%, preferably 4.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0109] In a preferred embodiment, the one-component adhesive composition according to the invention comprises a metal oxide, preferably CaO, and optionally a layered silicate, preferably an organophilic layered silicate.

[0110] The one-component adhesive composition according to the present invention optionally contains (f) chain silicates (chain silicates). Silicate minerals are divided into the following groups according to the structure of their silicate anions: neosilicates (orthosilicates), sorosilicates, cyclic silicates, chain silicates, layered silicates and tectosilicates. Cyclic silicates form rings, chain silicates form single or double chains, layered silicates form sheets, and tectosilicates form three-dimensional networks.

[0111] The chain silicate according to the present invention can be selected from single chain chain silicates and double chain chain silicates. Single chain chain silicates are preferred. The single chain chain silicate according to the present invention can be selected from the pyroxenoid family or the pyroxenoid family. Single chain chain silicates from the pyroxenoid family are preferred. Preferably, the chain silicate is selected from wollastonite, rhodonite or pectolite. Suitable chain silicates such as wollastonite are known to those skilled in the art and can be obtained, for example, under the trade name HR2000 was purchased commercially.

[0112] Preferably, the inosilicate has the form of particles, flakes, platelets, rods, needles and / or rectangles, preferably needles.

[0113] In a particularly preferred embodiment, the inosilicate comprises or consists essentially of wollastonite; preferably wollastonite needles.

[0114] Preferably, the inosilicate has an aspect ratio of at least 2.0, preferably at least 4.0, more preferably at least 6.0, still more preferably at least 8.0, still more preferably at least 10, and even more preferably at least 12.

[0115] Preferably, the inosilicate has an aspect ratio of at most 22, preferably at most 20, more preferably at most 18, still more preferably at most 16, still more preferably at most 14, and even more preferably at most 12.

[0116] Preferably, the aspect ratio of the inosilicate is in the range of 12±5.0, preferably 12±2.5.

[0117] Preferably, the volume median diameter D10 of the inosilicate determined by laser diffraction analysis according to ISO 13320 is at least 0.5 μm, preferably at least 1.0 μm, more preferably at least 1.5 μm, still more preferably at least 2.05 μm, still more preferably at least 2.5 μm, even more preferably at least 3.0 μm, most preferably at least 3.5 μm, and in particular at least 4.0 μm.

[0118] Preferably, the volume median diameter D10 of the chain silicate determined by laser diffraction analysis according to ISO 13320 is at most 12 μm, preferably at most 11 μm, more preferably at most 10 μm, still more preferably at most 9.0 μm, still more preferably at most 8.0 μm, even more preferably at most 7.0 μm, most preferably at most 6.0 μm, and in particular at most 5.0 μm.

[0119] Preferably, the volume median diameter D10 of the inosilicate, determined by laser diffraction analysis according to ISO 13320, is in the range of 4.0±2.0 μm, preferably 4.0±1.0 μm.

[0120] Preferably, the volume median diameter D50 of the inosilicate determined by laser diffraction analysis according to ISO 13320 is at least 10 μm, preferably at least 11 μm, more preferably at least 12 μm, still more preferably at least 13 μm, still more preferably at least 14 μm, even more preferably at least 15 μm, most preferably at least 16 μm, and in particular at least 17 μm.

[0121] Preferably, the inosilicate has a volume median diameter D50 determined by laser diffraction analysis according to ISO 13320 of at most 32 μm, preferably at most 30 μm, more preferably at most 28 μm, still more preferably at most 26 μm, still more preferably at most 24 μm, even more preferably at most 22 μm, most preferably at most 20 μm, and in particular at most 18 μm.

[0122] Preferably, the inosilicate has a volume median diameter D50 determined by laser diffraction analysis according to ISO 13320 in the range of 17±7.0 μm, preferably 17±3.5 μm.

[0123] Preferably, the volume median diameter D90 of the inosilicate determined by laser diffraction analysis according to ISO 13320 is at least 30 μm, preferably at least 35 μm, more preferably at least 40 μm, even more preferably at least 45 μm, still more preferably at least 50 μm, even more preferably at least 55 μm, most preferably at least 60 μm, and in particular at least 65 μm.

[0124] Preferably, the volume median diameter D90 of the inosilicate determined by laser diffraction analysis according to ISO 13320 is at most 120 μm, preferably at most 110 μm, more preferably at most 100 μm, still more preferably at most 90 μm, still more preferably at most 85 μm, even more preferably at most 80 μm, most preferably at most 75 μm, and in particular at most 70 μm.

[0125] Preferably, the inosilicate has a volume median diameter D90 determined by laser diffraction analysis according to ISO 13320 in the range of 65±30 μm, preferably 65±15 μm.

[0126] Preferably, the average length of the chain silicate is at least 30 μm, preferably at least 35 μm, more preferably at least 40 μm, even more preferably at least 45 μm, still more preferably at least 50 μm, even more preferably at least 55 μm, most preferably at least 60 μm, and in particular at least 65 μm.

[0127] Preferably, the average length of the chain silicate is at most 105 μm, preferably at most 100 μm, more preferably at most 95 μm, still more preferably at most 90 μm, still more preferably at most 85 μm, even more preferably at most 80 μm, most preferably at most 75 μm, and in particular at most 70 μm.

[0128] Preferably, the average length of the chain silicate is in the range of 65±30 μm, preferably 65±15 μm.

[0129] Preferably, the average width of the inosilicate is at least 1.0 μm, preferably at least 2.0 μm, more preferably at least 3.0 μm, still more preferably at least 4.0 μm, still more preferably at least 5.0 μm, even more preferably at least 6.0 μm, and most preferably at least 7.0 μm.

[0130] Preferably, the average width of the chain silicate is at most 20 μm, preferably at most 18 μm, more preferably at most 16 μm, even more preferably at most 14 μm, still more preferably at most 12 μm, even more preferably at most 10 μm, most preferably at most 9.0 μm, and in particular at most 8.0 μm.

[0131] Preferably, the average width of the inosilicate is in the range of 7.0±5.0 μm, preferably 7.0±3.5 μm.

[0132] Preferably, the weight content of the linear silicate relative to the total weight of the one-component adhesive composition is at least 3.0 wt.-%, preferably at least 4.0 wt.-%, more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, still more preferably at least 7.0 wt.-%, even more preferably at least 8.0 wt.-%, most preferably at least 9.0 wt.-%, and in particular at least 10 wt.-%.

[0133] Preferably, the weight content of the linear silicate relative to the total weight of the one-component adhesive composition is at most 30 wt.-%, preferably at most 28 wt.-%, more preferably at most 26 wt.-%, even more preferably at most 24 wt.-%, still more preferably at most 22 wt.-%, even more preferably at most 20 wt.-%, most preferably at most 18 wt.-%, and in particular at most 16 wt.-%.

[0134] Preferably, the weight content of the inosilicate is in the range of 15±7.0 wt.-%, preferably 15±3.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0135] The one-component adhesive composition according to the present invention optionally comprises (g) a reactive diluent. Preferably, the reactive diluent is an epoxy reactive diluent having a reactive epoxy functional group or a nucleophilic functional group capable of reacting with an epoxy functional group.

[0136] Reactive diluents can be added to the one-component adhesive composition according to the present invention to adjust its viscosity. Since reactive diluents generally have relatively low viscosities, reactive diluents generally reduce the viscosity of the composition. In this regard, reactive diluents can reduce the viscosity to values ​​that cannot be achieved using liquid epoxy resins alone.

[0137] Preferably, the reactive diluent comprises:

[0138] - Epoxy functional groups;

[0139] -Hydroxy functional group;

[0140] - aldehyde functional group;

[0141] - an oxazolidine functional group; and / or

[0142] - lactone functional group;

[0143] Epoxy functional groups are preferred.

[0144] Preferably, the reactive diluent is a glycidyl ether epoxy resin.

[0145] Preferably, the reactive diluent is selected from phenyl glycidyl ether, alkylphenol monoglycidyl ether, aliphatic monoglycidyl ether, alkylphenol monoglycidyl ether, alkylphenol monoglycidyl ether, 3-glycidyloxypropyl trimethoxysilane, 3-glycidyloxypropyl trimethoxysilane, 3-glycidyloxypropyl methyl dimethoxysilane, 1-(3-glycidyloxypropyl) 1,1,3,3,3-pentamethyldisiloxane, 1,4-butanediol diglycidyl ether, 1,6-hexanediol diglycidyl ether, 1, 4-cyclohexanedimethanol, glycidyl ether of soybean oil, glycidyl ether of linseed oil, glycidyl ether of cashew nut shell liquid, diglycidyl ether of resorcinol, diglycidyl ether of cyclohexanedimethanol, diglycidyl ether of neopentyl glycol, diglycidyl ether of cashew nut shell liquid, triglycidyl ether of trimethylolpropane dipentene, trimethylolpropane triglycidyl ether, glycerol triglycidyl ether, pentaerythritol tetraglycidyl ether and mixtures thereof; preferably glycidyl ether of cashew nut shell liquid, diglycidyl ether of cashew nut shell liquid and mixtures thereof. Suitable reactive diluents are known to those skilled in the art and can be obtained, for example, under the trade name E10P, NC 514S and etc. are commercially available.

[0146] Preferably, the reactive diluent has more than one epoxy functional group; preferably two epoxy functional groups.

[0147] Preferably, the reactive diluent is the diglycidyl ether of cashew nut shell liquid.

[0148] Preferably, the epoxy equivalent of the reactive diluent measured according to ASTM D1652 is in the range of 290 to 450 g / eq, preferably 305 to 435 g / eq, and more preferably 320 to 420 g / eq.

[0149] Preferably, the viscosity of the reactive diluent at 25° C. measured according to ASTM D2196 is in the range of 0.25 to 12 Pa·s, preferably 0.5 to 6.0 Pa·s, more preferably 1.0 to 3.0 Pa·s.

[0150] Preferably, the weight content of the reactive diluent relative to the total weight of the one-component adhesive composition is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, still more preferably at least 3.5 wt.-%, even more preferably at least 4.0 wt.-%, most preferably at least 4.5 wt.-%, and in particular at least 5.0 wt.-%.

[0151] Preferably, the weight content of the reactive diluent relative to the total weight of the one-component adhesive composition is at most 16 wt.-%, preferably at most 14 wt.-%, more preferably at most 12 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%.

[0152] Preferably, the weight content of the reactive diluent is in the range of 5.5±3.0 wt.-%, preferably 5.5±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0153] The one-component adhesive composition according to the present invention optionally comprises (h) an additional curable epoxy resin; preferably a semi-solid curable epoxy resin. The viscosity of the semi-solid epoxy resin is typically measured at elevated temperature (eg 52°C or 55°C).

[0154] Preferably, the additional curable epoxy resin is selected from bisphenol diglycidyl ether resins, epoxy novolac resins, preferably epoxy phenol novolac resins, and combinations thereof. Preferably, the additional curable epoxy resin is semi-solid.

[0155] Preferably, the additional curable epoxy resin comprises or consists essentially of an epoxy novolac resin, preferably an epoxy phenol novolac resin; preferably a semi-solid epoxy novolac resin, preferably an epoxy phenol novolac resin.

[0156] Preferably, the additional curable epoxy resin comprises or consists essentially of: a bisphenol diglycidyl ether resin; preferably a dimer acid modified epoxy resin.

[0157] Preferably, the additional curable epoxy resin comprises or consists essentially of an epoxy novolac resin and a bisphenol diglycidyl ether resin.

[0158] Suitable additional curable epoxy resins such as semisolid epoxy phenol novolac resins or dimer acid-modified epoxy resins are known to the person skilled in the art and are available, for example, under the trade name YDPN 638 and YD172 and others were purchased commercially.

[0159] Dimer acid modified epoxy resins are known to those skilled in the art and are commercially available. Epoxy resins can be divided into six main types, namely (i) epoxy resins based on bisphenol-A, (ii) epoxy resins based on bisphenol-F, (iii) multifunctional epoxy resins (novolac), (iv) alicyclic epoxy resins, (v) flame retardant epoxy resins, and (vi) modified epoxy resins. The latter main type includes (a) dimer acid modified epoxy resins, and (b) CTBN modified epoxy resins and (c) silicone modified epoxy resins (see, for example, A.S. Khanna, High-performance organic coatings, Woodhead Publishing, 2008, page 148).

[0160] Preferably, the dimer acid-modified epoxy resin according to the present invention has the following general formula

[0161]

[0162] in

[0163] R is the dimer acid moiety which may be optionally substituted aliphatic, alicyclic or aromatic;

[0164] m is an integer in the range of 0 to 10; and

[0165] n is an integer in the range of 0 to 10.

[0166] Preferably, the additional curable epoxy resin (preferably epoxy novolac resin, more preferably epoxy phenol novolac resin) has an epoxy equivalent determined according to ASTM D1652 in the range of 150 to 210 g / eq, preferably 160 to 200 g / eq, and more preferably 170 to 190 g / eq.

[0167] Preferably, the additional curable epoxy resin (preferably dimer acid-modified epoxy resin) has an epoxy equivalent measured according to ASTM D1652 in the range of 400 to 900 g / eq, preferably 500 to 800 g / eq, and more preferably 600 to 700 g / eq.

[0168] Preferably, the additional curable epoxy resin, preferably an epoxy novolac resin, more preferably an epoxy phenol novolac resin, has a solution viscosity of from H to K, measured according to the Gardner Holdt method, preferably in a 60% solution in butyl carbitol NV.

[0169] Preferably, the additional curable epoxy resin has a viscosity at 55° C. of at least 100 Pa·s, preferably at least 125 Pa·s, more preferably at least 150 Pa·s, as measured according to ASTM D2196.

[0170] Preferably, the additional curable epoxy resin, preferably the dimer acid modified epoxy resin, is semi-solid at 25°C.

[0171] Preferably, the epoxy functionality of the additional curable epoxy resin is in the range of 0.3 to 2.9, preferably 0.7 to 2.5, more preferably 1.1 to 2.1.

[0172] Preferably, the weight content of the additional curable epoxy resin relative to the total weight of the one-component adhesive composition is at least 0.5 wt.-%, preferably at least 0.8 wt.-%, more preferably at least 1.1 wt.-%, even more preferably at least 1.4 wt.-%, still more preferably at least 1.7 wt.-%, even more preferably at least 2.0 wt.-%, most preferably at least 2.3 wt.-%, and in particular at least 2.6 wt.-%.

[0173] Preferably, the weight content of the additional curable epoxy resin relative to the total weight of the one-component adhesive composition is at most 10 wt.-%, preferably at most 9.0 wt.-%, more preferably at most 8.0 wt.-%, even more preferably at most 7.0 wt.-%, still more preferably at most 6.0 wt.-%, even more preferably at most 5.0 wt.-%, most preferably at most 4.0 wt.-%, and in particular at most 3.0 wt.-%.

[0174] Preferably, the weight content of the additional curable epoxy resin is in the range of 2.6±2.0 wt.-%, preferably 2.6±1.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0175] The one-component adhesive composition according to the present invention optionally comprises (i) fibers, preferably discontinuous fibers.

[0176] Preferably, the fibers have the form of aggregates, hollow materials, chopped materials, or a mixture thereof.

[0177] Preferably, the fibers comprise or consist essentially of inorganic fibers, preferably glass (e.g. E-glass or S-glass) fibers or fiberglass; organic fibers, preferably polymer fibers, more preferably selected from polyamide (e.g. nylon) fibers, polyester fibers, carbon fibers, aramid fibers, polycarbonate fibers, polyethylene fibers, polypropylene fibers, polybutene (e.g. polybutylene terephthalate) fibers, polystyrene fibers, polyurethane fibers; or mixtures thereof.

[0178] Preferably, the fibers are selected from chopped glass fibers, chopped aramid fibers, aramid pulp, and mixtures thereof; preferably chopped glass fibers.

[0179] Suitable fibers, such as chopped glass fibers, are known to those skilled in the art and are commercially available, for example, under the trade name FGCS 3540 / 3 or the like.

[0180] Preferably, the average length of the fibers is at least 0.5 mm, preferably at least 1.0 mm, more preferably at least 1.5 mm, still more preferably at least 2.0 mm, still more preferably at least 2.5 mm, even more preferably at least 3.0 mm, most preferably at least 3.5 mm, and in particular at least 4.0 mm.

[0181] Preferably, the average length of the fibers is at most 45 mm, preferably at most 40 mm, more preferably at most 35 mm, still more preferably at most 30 mm, still more preferably at most 25 mm, even more preferably at most 20 mm, most preferably at most 15 mm, and in particular at most 10 mm.

[0182] Preferably, the average length of the fibers is in the range of 7.0±6.0 mm, preferably 7.0±3.0 mm.

[0183] Preferably, the average diameter of the fibers is at least 3.0 μm, preferably at least 4.0 μm, more preferably at least 5.0 μm, still more preferably at least 6.0 μm, still more preferably at least 7.0 μm, even more preferably at least 8.0 μm, most preferably at least 9.0 μm, and especially at least 10 μm.

[0184] Preferably, the average diameter of the fibers is at most 45 μm, preferably at most 40 μm, more preferably at most 35 μm, still more preferably at most 30 μm, still more preferably at most 25 μm, even more preferably at most 20 μm, most preferably at most 15 μm, and in particular at most 12 μm.

[0185] Preferably, the average diameter of the fibers is in the range of 10±4.0 mm, preferably 10±2.0 mm.

[0186] Preferably, the weight content of the fibers, relative to the total weight of the one-component adhesive composition, is at least 1.5 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, still more preferably at least 3.5 wt.-%, even more preferably at least 4.0 wt.-%, most preferably at least 4.5 wt.-%, and in particular at least 5.0 wt.-%.

[0187] Preferably, the weight content of the fibers relative to the total weight of the one-component adhesive composition is at most 13 wt.-%, preferably at most 12 wt.-%, more preferably at most 11 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%.

[0188] Preferably, the weight content of the fibers is in the range of 6.0±3.0 wt.-%, preferably 6.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0189] The one-component adhesive composition according to the invention optionally comprises (j) a polyhydroxycarboxylic acid ester which is preferably used as a rheology modifier. Suitable polyhydroxycarboxylates are known to the person skilled in the art and are available, for example, under the trade name R606 and the like are commercially available.

[0190] Preferably, the total weight content of polyhydroxycarboxylic acid esters is at least 0.2 wt.-%, preferably at least 0.3 wt.-%, more preferably at least 0.4 wt.-%, even more preferably at least 0.5 wt.-%, still more preferably at least 0.6 wt.-%, even more preferably at least 0.7 wt.-%, most preferably at least 0.8 wt.-%, and in particular at least 0.9 wt.-%, relative to the total weight of the one-component adhesive composition.

[0191] Preferably, the total weight content of polyhydroxycarboxylic acid esters is at most 5.0 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.0 wt.-%, still more preferably at most 2.0 wt.-%, still more preferably at most 1.6 wt.-%, even more preferably at most 1.4 wt.-%, most preferably at most 1.2 wt.-%, and in particular at most 1.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0192] Preferably, the total weight content of polyhydroxycarboxylic acid esters is in the range of 1.0±0.9 wt.-%, preferably 1.0±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0193] The one-component adhesive composition according to the present invention optionally comprises (k) a polyamide.

[0194] Preferably, the polyamide is a polyamide powder. Suitable polyamide powders are known to the person skilled in the art and are available, for example, under the trade name (Arkema) is commercially available.

[0195] Preferably, the polyamide has the form of particles, flakes, platelets, rods, needles and / or rectangles.

[0196] Preferably, the total weight content of polyamide, relative to the total weight of the one-component adhesive composition, is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%, and in particular at least 5.0 wt.-%.

[0197] Preferably, the total weight content of polyamide is at most 15 wt.-%, preferably at most 12 wt.-%, more preferably at most 11 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0198] Preferably, the total weight content of polyamide is in the range of 5.0±3.0 wt.-%, preferably 5.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0199] The one-component adhesive composition according to the present invention optionally comprises (1) a blowing agent. The blowing agent may be selected from chemical blowing agents, physical blowing agents, preferably expandable thermoplastic microspheres, and mixtures thereof.

[0200] Preferably, the one-component adhesive composition can foam when activated by heat or any other suitable stimulus. Therefore, the material exists in two states, foamable and foamed. Usually, the foamable thermoplastic material becomes a thermosetting material after foaming. In the initial foamable state, the material is usually stable at room temperature. When heated to its activation temperature, due to the activated foaming process, the material undergoes volume expansion, thereby producing the final foaming state of the material. Preferably, a blowing agent (blowing agent) can achieve the foaming process. Under elevated temperature or other activation conditions, the blowing agent decomposes and releases gas. This is usually accompanied by the solidification of the composition, which is designed to undergo solidification at such an elevated temperature.

[0201] Preferably, the blowing agent is a chemical blowing agent, preferably selected from the group consisting of azodicarbonamide, dinitrosopentamethylenetetramine, hydrazides such as 4,4-oxy-bis-(benzenesulfonylhydrazide), trihydrazinotriazine, N,N′-dimethyl-N,N′-dinitrosoterephthalamide, toluenesulfonylhydrazide (TSH), p-toluenesulfonylsemicarbazide (TSSC), 5-phenyltetrazole (5-PT) or NN′-dinitrosopentamethylenetetramine (DNPT); preferably azodicarbonamide. Suitable chemical blowing agents such as azodicarbonamide are known to the person skilled in the art and are available, for example, under the trade name AC7000DB and the like are commercially available.

[0202] In other preferred embodiments, the blowing agent is a physical blowing agent, preferably expandable thermoplastic microspheres. Suitable physical blowing agents such as expandable thermoplastic microspheres are known to those skilled in the art and are available, for example, under the trade name and etc. are commercially available.

[0203] Preferably, the weight content of the blowing agent relative to the total weight of the one-component adhesive composition is at least 0.2 wt.-%, preferably at least 0.3 wt.-%, more preferably at least 0.4 wt.-%, even more preferably at least 0.5 wt.-%, still more preferably at least 0.6 wt.-%, even more preferably at least 0.7 wt.-%, most preferably at least 0.8 wt.-%, and in particular at least 0.9 wt.-%.

[0204] Preferably, the weight content of the blowing agent relative to the total weight of the one-component adhesive composition is at most 5.0 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.0 wt.-%, even more preferably at most 2.0 wt.-%, still more preferably at most 1.6 wt.-%, even more preferably at most 1.4 wt.-%, most preferably at most 1.2 wt.-%, and in particular at most 1.0 wt.-%.

[0205] Preferably, the weight content of the blowing agent is in the range of 1.0±0.9 wt.-%, preferably 1.0±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

[0206] The one-component adhesive composition according to the present invention optionally comprises (m) an impact modifier. For the purpose of this specification, the impact modifier increases durability. Impact modifiers are known to those skilled in the art (see, for example, Berzins A.P. Impact Modifiers, Lutz JT, Grossmann RF Polymer Modifiers and Adhesives (2001), Chapter 8 of Marcel Dekker).

[0207] The functionalized elastomeric adduct impact modifier according to the invention is preferably epoxy-functionalized or carboxyl-functionalized. The elastomeric part may be based on, for example, an acrylonitrile / butadiene copolymer. Functionalized acrylonitrile / butadiene copolymers of this type are available, for example, under the trade name Hypro TM CTBN, CTBNX and ETBN are commercially available.

[0208] Preferably, the impact modifier is selected from the group consisting of functionalized elastomer adducts, preferably elastomer / epoxy adducts, core-shell impact modifiers, and combinations thereof. Suitable impact modifiers are known to those skilled in the art and are available, for example, under the trade name E950,Kane MX257(37 / 63CRS / EPX)、Struktol 3695 and 8001 etc. are commercially available. Particularly suitable modified acrylonitrile / butadiene copolymers are made from (Schill-Seilacher) or (Nanoresins) Those liquid rubbers sold within the product range.

[0209] The core-shell impact modifier according to the present invention generally includes a graft copolymer, which can be characterized as a core-shell copolymer having a rubbery "core", a hard "shell", and swells in a methacrylate and / or acrylate monomer composition but does not dissolve therein. Examples of core-shell copolymers are those in which a hard "shell" monomer such as styrene, acrylonitrile or methyl methacrylate is grafted onto a rubbery "core" made from polymers of butadiene, butyl acrylate, ethyl acrylate and isoprene, etc. One type of core-shell polymer is a methacrylate butadiene styrene (MBS) copolymer made by polymerizing methyl methacrylate in the presence of polybutadiene or a polybutadiene copolymer rubber. Commercial examples of core-shell impact modifiers are ParaloidTM BTA-753, Paraloid 2650A, Paraloid 2691A, E920, Clearstrength XT 100, and Kane AceTM B-564 or Kane AceTM M521.

[0210] In a preferred embodiment, the impact modifier is a core-shell impact modifier selected from the group consisting of: impact modifiers based on butadiene, isoprene, ethylene-propylene and ethylene-butylene in combination with styrene, acrylonitrile and acrylic monomers; acrylonitrile butadiene styrene (ABS) impact modifiers; methacrylate butadiene styrene (MBS) impact modifiers; and MABS impact modifiers.

[0211] In a preferred embodiment, the impact modifier is a (methyl)methacrylate butadiene styrene (MBS) core-shell impact modifier. Thus, the impact modifier is preferably a core-shell copolymer in which a hard "shell" acrylate monomer (preferably (methyl)methacrylate) is grafted onto a rubbery "core" made of butadiene styrene rubber. This type of impact modifier is commercially available (e.g., Kane Ace™ B564, Kane Ace™ M521, Clearstrength™ XT 100, Paraloid 2650A, Paraloid 2691A, E920, Clearstrength XT 100).

[0212] In another preferred embodiment, the impact modifier is a core-shell polybutadiene rubber, which may be dispersed in a liquid bisphenol A epoxy resin (eg, Kane Ace™ MX257).

[0213] In yet another preferred embodiment, the impact modifier is a core-shell impact modifier having an all-acrylic core-shell based on butyl acrylate rubber. Thus, the impact modifier is preferably a core-shell copolymer in which a hard "shell" acrylate monomer (preferably (methyl) methacrylate) is grafted onto a rubbery "core" made of butyl acrylate rubber. This type of first impact modifier is commercially available (e.g., Paraloid™ EXL-2300G, Paraloid EXL-2314, Paraloid EXL 3361).

[0214] Preferably, the one-component adhesive composition according to the invention comprises a first impact modifier and optionally a second impact modifier.

[0215] Preferably, the first impact modifier comprises a methyl methacrylate-butadiene-styrene (MBS) core-shell polymer.

[0216] In a preferred embodiment, the first impact modifier is a solid impact modifier; preferably a solid methyl methacrylate-butadiene-styrene (MBS) core-shell impact modifier.

[0217] Preferably, the weight content of the first impact modifier, preferably a solid first impact modifier, relative to the total weight of the one-component adhesive composition is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%.

[0218] Preferably, the weight content of the first impact modifier, preferably a solid first impact modifier, relative to the total weight of the one-component adhesive composition is at most 22 wt.-%, preferably at most 20 wt.-%, more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, still more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, most preferably at most 10 wt.-%, and in particular at most 9.0 wt.-%.

[0219] Preferably, the weight content of the first impact modifier, preferably a solid first impact modifier, is in the range of 8.0±5.0 wt.-%, preferably 8.0±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0220] In a further preferred embodiment, the first impact modifier is a liquid impact modifier; preferably a methyl methacrylate-butadiene-styrene (MBS) core-shell polymer dispersed in a bisphenol A epoxy resin.

[0221] Preferably, the weight content of the first impact modifier, preferably a liquid first impact modifier, relative to the total weight of the one-component adhesive composition is at least 6.0 wt.-%, preferably at least 8.0 wt.-%, more preferably at least 10 wt.-%, even more preferably at least 12 wt.-%, still more preferably at least 14 wt.-%, even more preferably at least 16 wt.-%, most preferably at least 18 wt.-%, and in particular at least 20 wt.-%.

[0222] Preferably, the weight content of the first impact modifier, preferably a liquid first impact modifier, relative to the total weight of the one-component adhesive composition is at most 36 wt.-%, preferably at most 34 wt.-%, more preferably at most 32 wt.-%, even more preferably at most 30 wt.-%, still more preferably at most 28 wt.-%, even more preferably at most 26 wt.-%, most preferably at most 24 wt.-%, and in particular at most 22 wt.-%.

[0223] Preferably, the weight content of the first impact modifier, preferably a liquid first impact modifier, is in the range of 20±10 wt.-%, preferably 20±5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0224] Preferably, the second impact modifier is an elastomer / epoxy adduct; preferably a nitrile rubber modified epoxy resin; even more preferably a nitrile rubber modified epoxy resin based on bisphenol-A-diglycidyl ether.

[0225] Preferably, the weight content of the second impact modifier relative to the total weight of the one-component adhesive composition is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%.

[0226] Preferably, the weight content of the second impact modifier is at most 22 wt.-%, preferably at most 20 wt.-%, more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, still more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, most preferably at most 10 wt.-%, and in particular at most 9.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0227] Preferably, the weight content of the second impact modifier is in the range of 8.0±5.0 wt.-%, preferably 8.0±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0228] The one-component adhesive composition according to the present invention optionally comprises (n) a toughening agent and / or a flexibilizer. For the purposes of this specification, a toughening agent increases the ability of a material to absorb energy and to deform plastically without breaking. A typical toughening agent is a rubber (elastomer) that can be dispersed as nanoparticles in a polymer matrix to increase the mechanical robustness or toughness of the material. Toughening agents are known to those skilled in the art (see, for example, Bucknall CB (1977) Toughened Plastics, Springer; Keskkula H., Paul DR (1994) Toughening agents for engineering polymers. In: Collyer AA (eds) Rubber Toughened Engineering Plastics. Springer; Arends Ch. (1996) Polymer Toughening, Marcel Dekker). Suitable toughening agents / flexibilizers are known to those skilled in the art and can be found, for example, under the trade name B90 (Eastman) and DY 965CH (Huntsman) are commercially available.

[0229] Preferably, the toughening agent and / or flexibilizer is selected from the group consisting of polyolefins, polyurethanes, polyvinyl acetals, polyvinyl acetates, polyvinyl alcohols, polytetrafluoroethylenes, acrylic resins, polyvinyl chlorides, polyvinylidene chlorides, polystyrenes and combinations thereof; preferably polyurethanes, polyvinyl acetals and combinations thereof.

[0230] Preferably, the toughening and / or flexibilizing agent comprises or consists essentially of a capped polyurethane adduct and / or a polyvinyl acetal resin; preferably a phenol terminated polyurethane adduct and / or a polyvinyl butyral resin.

[0231] Preferred are polyvinyl esters, especially polyvinyl butyral resins such as Resins, especially 90 and Resin.

[0232] Preferably, the total weight content of tougheners and / or flexibilizers, relative to the total weight of the one-component adhesive composition, is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%.

[0233] Preferably, the total weight content of tougheners and / or flexibilizers, relative to the total weight of the one-component adhesive composition, is at most 18 wt.-%, preferably at most 16 wt.-%, more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, still more preferably at most 10 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 8.0 wt.-%, and in particular at most 7.0 wt.-%.

[0234] Preferably, the total weight content of tougheners and / or flexibilizers is in the range of 6.0±4.0 wt.-%, preferably 6.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0235] The one-component adhesive composition according to the present invention optionally comprises (o) a phenoxy resin; preferably a solid phenoxy resin; more preferably a solid phenoxy resin which is a copolymer of bisphenol A and epichlorohydrin.

[0236] Suitable phenoxy resins are known to the person skilled in the art and are available, for example, under the trade names PKHA, PKHB, PKHC, PKHH, PKHJ, PKFE, PKHP, PKHS (InChemRez) or YP-50 was purchased commercially.

[0237] A phenoxy resin may be added to the one-component adhesive composition according to the present invention to adjust the viscosity thereof.

[0238] Preferably, the weight content of the phenoxy resin relative to the total weight of the one-component adhesive composition is at least 3.0 wt.-%, preferably at least 4.0 wt.-%, more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, still more preferably at least 7.0 wt.-%, even more preferably at least 8.0 wt.-%, most preferably at least 9.0 wt.-%, and in particular at least 10 wt.-%.

[0239] Preferably, the weight content of the phenoxy resin relative to the total weight of the one-component adhesive composition is at most 26 wt.-%, preferably at most 24 wt.-%, more preferably at most 22 wt.-%, even more preferably at most 20 wt.-%, still more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, most preferably at most 14 wt.-%, and in particular at most 12 wt.-%.

[0240] Preferably, the weight content of the phenoxy resin is in the range of 10±6.0 wt.-%, preferably 10±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

[0241] The one-component adhesive composition according to the present invention optionally contains (p) a curing accelerator.

[0242] Preferably, the curing accelerator is selected from the group consisting of modified or unmodified urea, imidazole, secondary amine, tertiary amine, quaternary ammonium salt and pyridine; modified urea is preferred. Suitable curing accelerators are known to the person skilled in the art and are available, for example, under the trade name UR 400 was commercially available.

[0243] Preferably, the weight content of the curing accelerator relative to the total weight of the one-component adhesive composition is at least 0.1 wt.-%, preferably at least 0.2 wt.-%, more preferably at least 0.25 wt.-%, even more preferably at least 0.3 wt.-%, still more preferably at least 0.35 wt.-%, even more preferably at least 0.4 wt.-%, most preferably at least 0.45 wt.-%, and in particular at least 0.5 wt.-%.

[0244] Preferably, the weight content of the curing accelerator relative to the total weight of the one-component adhesive composition is at most 2.5 wt.-%, preferably at most 2.0 wt.-%, more preferably at most 1.75 wt.-%, even more preferably at most 1.5 wt.-%, still more preferably at most 1.25 wt.-%, even more preferably at most 1.0 wt.-%, most preferably at most 0.75 wt.-%, and in particular at most 0.5 wt.-%.

[0245] Preferably, the weight content of the curing accelerator is in the range of 0.5±0.4 wt.-%, preferably 0.5±0.2 wt.-%, relative to the total weight of the one-component adhesive composition.

[0246] Preferably, the one-component adhesive composition according to the invention additionally comprises a filler selected from the group consisting of carbonates, borates, oxides, hydroxides, sulfates, titanates, zirconates and mixtures thereof.

[0247] Preferably, the weight content of the additional filler is in the range of 5.0±4.5 wt % relative to the total weight of the one-component adhesive composition.

[0248] Preferably, the additional filler has the form of particles, flakes, platelets, rods, needles and / or rectangles.

[0249] The one-component adhesive composition according to the present invention may include one or more additives (e.g., functional additives) for improving one or more different properties of the composition. As an example, the additive may include an antioxidant, an antiozonant, a UV absorber, an ultraviolet resistant agent, a lubricant, an antistatic agent, a colorant, a flame retardant, a heat stabilizer, a plasticizer, a preservative, a processing aid, a stabilizer, or a combination thereof.

[0250] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises an inosilicate, preferably wollastonite, and a metal oxide, preferably calcium carbonate, wherein the weight content of the inosilicate is greater than the weight content of the metal oxide, preferably in the range of 5:1 to 1.5:1 or 5:1 to 1.5:1.

[0251] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises an inosilicate, preferably wollastonite, and a layered silicate, preferably strontium zinc phosphosilicate, wherein the weight content of the inosilicate is greater than the weight content of the layered silicate, preferably in the range of 15:1 to 2:1 or 15:1 to 2:1.

[0252] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises an inosilicate, preferably wollastonite, and silica, preferably fumed silica, more preferably polydimethylsiloxane-treated fumed silica, wherein the weight content of the inosilicate is greater than the weight content of silica, preferably in the range of 10:1 to 2:1 or 10:1 to 2:1.

[0253] Preferably, the total content of (a) liquid epoxy resin, (b) latent curing agent, (c) silica and (d) metal oxide is at least 40 wt.-%, preferably at least 42.5 wt.-%, more preferably at least 45 wt.-%, even more preferably at least 47.5 wt.-%, still more preferably at least 50 wt.-%, even more preferably at least 52.5 wt.-%, most preferably at least 55 wt.-%, and in particular at least 57.5 wt.-%, relative to the total weight of the composition.

[0254] Preferably, the total content of (a) liquid epoxy resin, (b) latent curing agent, (c) silicon dioxide, (d) metal oxide, (e) optional layered silicate (if present) and (f) optional linear silicate (if present) is at least 50 wt.-%, preferably at least 52.5 wt.-%, more preferably at least 55 wt.-%, even more preferably at least 57.5 wt.-%, still more preferably at least 60 wt.-%, even more preferably at least 62.5 wt.-%, most preferably at least 65 wt.-%, and in particular at least 67.5 wt.-%, relative to the total weight of the composition.

[0255] In a preferred embodiment, the curable one-component adhesive composition according to the invention comprises at least 20 wt.-%, preferably 20 to 60 wt.-%, of a liquid epoxy resin (preferably comprising a liquid epoxy novolac resin or essentially consisting of a liquid epoxy novolac resin, more preferably comprising a liquid epoxy phenol novolac resin or essentially consisting of a liquid epoxy phenol novolac resin), relative to the total weight of the composition; and at least 10 wt.-%, preferably 10 to 25 wt.-% of a chain silicate, preferably wollastonite.

[0256] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises at least 20 wt.-%, preferably 20 to 60 wt.-%, of a liquid epoxy resin (preferably comprising a liquid epoxy novolac resin or essentially consisting of a liquid epoxy novolac resin, more preferably comprising a liquid epoxy phenol novolac resin or essentially consisting of a liquid epoxy phenol novolac resin), relative to the total weight of the composition; at least 10 wt.-%, preferably 10 to 25 wt.-% of a chain silicate, preferably wollastonite; and at least 3.0 wt.-%, preferably 3.0 to 7.0 wt.-% of a metal oxide, preferably calcium oxide.

[0257] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises at least 20 wt.-%, preferably 20 to 60 wt.-% of a liquid epoxy resin (preferably comprising a liquid epoxy novolac resin or essentially consisting of a liquid epoxy novolac resin, more preferably comprising a liquid epoxy phenol novolac resin or essentially consisting of a liquid epoxy phenol novolac resin), relative to the total weight of the composition; at least 10 wt.-%, preferably 10 to 25 wt.-% of a chain silicate, preferably wollastonite; at least 3.0 wt.-%, preferably 3.0 to 7.0 wt.-% of a metal oxide, preferably calcium oxide; and at least 3.0 wt.-%, preferably 3.0 to 7.0 wt.-% of silica, preferably fumed silica, more preferably fumed silica treated with polydimethylsiloxane.

[0258] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises at least 20 wt.-%, preferably 20 to 60 wt.-%, of a liquid epoxy resin (preferably comprising a liquid epoxy novolac resin or essentially consisting of a liquid epoxy novolac resin, more preferably comprising a liquid epoxy phenol novolac resin or essentially consisting of a liquid epoxy phenol novolac resin), relative to the total weight of the composition; at least 10 wt.-%, preferably 10 to 25 wt.-% of a chain silicate, preferably wollastonite; at least 3.0 wt.-%, preferably 3.0 to 7.0 wt.-% of a metal oxide, preferably calcium oxide; and at least 0.5 wt.-%, preferably 0.5 to 5.0 wt.-% of a layered silicate, preferably strontium zinc phosphosilicate.

[0259] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises at least 20 wt.-%, preferably 20 to 60 wt.-%, of a liquid epoxy resin (preferably comprising a liquid epoxy novolac resin or essentially consisting of a liquid epoxy novolac resin, more preferably comprising a liquid epoxy phenol novolac resin or essentially consisting of a liquid epoxy phenol novolac resin), relative to the total weight of the composition; at least 10 wt.-%, preferably 10 to 25 wt.-% of a chain silicate, preferably wollastonite; at least 3.0 wt.-%, preferably 3.0 to 7.0 wt.-% of a metal oxide, preferably calcium oxide; 3.0 to 7.0 wt.-% of silica, preferably fumed silica, more preferably fumed silica treated with polydimethylsiloxane; and at least 0.5 wt.-%, preferably 0.5 to 5.0 wt.-% of a layered silicate, preferably strontium zinc phosphosilicate.

[0260] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises or consists essentially of:

[0261] - (a) a liquid epoxy resin and optionally (g) a reactive diluent, wherein the total weight content of the liquid epoxy resin and the reactive diluent is at least 40 wt.-%, preferably at least 42.5 wt.-%, more preferably at least 45 wt.-%, still more preferably at least 47.5 wt.-%, still more preferably at least 50 wt.-%, even more preferably at least 52.5 wt.-%, most preferably at least 55 wt.-%, and in particular at least 57.5 wt.-%, relative to the total weight of the one-component adhesive composition;

[0262] -(b) latent epoxy curing agent;

[0263] - (c) silicon dioxide;

[0264] - (d) metal oxides;

[0265] - (e) layered silicates and / or (f) chain silicates, wherein the total weight content of layered silicates and / or chain silicates is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition;

[0266] - (m) an impact modifier and / or (n) a toughener and / or a flexibilizer, wherein the total weight content of the impact modifier and / or the toughener and / or the flexibilizer is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition.

[0267] In a preferred embodiment, the curable one-component adhesive composition according to the present invention comprises or consists essentially of:

[0268] - (a) a liquid epoxy resin and optionally (g) a reactive diluent, wherein the total weight content of the liquid epoxy resin and the reactive diluent is at least 40 wt.-%, preferably at least 42.5 wt.-%, more preferably at least 45 wt.-%, still more preferably at least 47.5 wt.-%, still more preferably at least 50 wt.-%, even more preferably at least 52.5 wt.-%, most preferably at least 55 wt.-%, and in particular at least 57.5 wt.-%, relative to the total weight of the one-component adhesive composition;

[0269] -(b) latent epoxy curing agent;

[0270] -(c) silica;

[0271] -(d) metal oxide;

[0272] -(e) phyllosilicate and / or (f) inosilicate, wherein the total weight content of the phyllosilicate and / or inosilicate is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, still more preferably at least 10 wt.-%, yet more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and especially at least 20 wt.-% relative to the total weight of the one-component binder composition; and,

[0273] -(l) blowing agent;

[0274] -(m) impact modifier and / or (n) toughening agent and / or flexibilizer, wherein the total weight content of the impact modifier and / or toughening agent and / or flexibilizer is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, still more preferably at least 10 wt.-%, yet more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and especially at least 20 wt.-% relative to the total weight of the one-component binder composition.

[0275] Preferably, the one-component binder composition according to the invention is thermally curable.

[0276] Preferably, the one-component binder composition according to the invention is pumpable; preferably pumpable with conventional equipment.

[0277] Preferably, the composition is pumpable at a temperature of at least 20 °C, preferably at least 25 °C, more preferably at least 30 °C, still more preferably at least 35 °C, yet more preferably at least 40 °C, even more preferably at least 45 °C, most preferably at least 50 °C, and especially at least 55 °C.

[0278] Preferably, the composition is pumpable at a temperature of at most 105 °C, preferably at most 100 °C, more preferably at most 95 °C, still more preferably at most 90 °C, yet more preferably at most 85 °C, even more preferably at most 80 °C, most preferably at most 75 °C, and especially at most 70 °C.

[0279] Preferably, the composition is pumpable at a temperature in the range of 42 ± 36 °C, preferably 42 ± 18 °C.

[0280] Preferably, the one-component adhesive composition according to the present invention has a viscosity at 25° C. measured according to ASTM D1084-16 of at least 2.0 Pa·s, preferably at least 4.0 Pa·s, more preferably at least 6.0 Pa·s, even more preferably at least 8.0 Pa·s, still more preferably at least 10 Pa·s, even more preferably at least 12 Pa·s, most preferably at least 14 Pa·s, and in particular at least 16 Pa·s.

[0281] Preferably, the viscosity of the composition at 25°C measured according to ASTM D1084-16 is at most 1000 Pa·s, preferably at most 800 Pa·s, more preferably at most 600 Pa·s, still more preferably at most 500 Pa·s, still more preferably at most 400 Pa·s, even more preferably at most 300 Pa·s, most preferably at most 200 Pa·s, and in particular at most 150 Pa·s.

[0282] Preferably, the viscosity of the composition at 25°C measured according to ASTM D1084-16 is at most 120 Pa·s, preferably at most 110 Pa·s, more preferably at most 100 Pa·s, still more preferably at most 90 Pa·s, still more preferably at most 80 Pa·s, even more preferably at most 70 Pa·s, most preferably at most 60 Pa·s, and in particular at most 50 Pa·s.

[0283] Preferably, the viscosity of the composition at 25° C. measured according to ASTM D1084-16 is 100±50 Pa·s, or 150±100 Pa·s, or 150±50 Pa·s, or 200±150 Pa·s, or 200±100 Pa·s, or 200±50 Pa·s, or 250±200 Pa·s, or 250±150 Pa·s, or 250±100 Pa·s, or 250±50 Pa·s, or 300±250 Pa·s, or 300±200 Pa·s, or 300±150 Pa·s, or 300±100 Pa·s, or 300±50 Pa·s, or 350±300 Pa·s, or 350±250 Pa·s, or 350±200 Pa·s. s, or 350±150Pa·s, or 350±100Pa·s, or 350±50Pa·s, or 400±350Pa·s, or 400±300Pa·s, or 400±250Pa·s, or 400±200Pa·s, or 400±150Pa·s, or 400±100Pa·s, or 400±50Pa·s, or 450±400Pa·s, or 450±350Pa·s, or 450±300Pa·s, or 450±250Pa·s, or 450±200Pa·s, or 450±150Pa·s, or 450±100Pa·s, or 450±50Pa·s, or 500±450Pa·s s, or 500±400Pa·s, or 500±350Pa·s, or 500±300Pa·s, or 500±250Pa·s, or 500±200Pa·s, or 500±150Pa·s, or 500±100Pa·s, or 500±50Pa·s, or 550±50Pa·s, or 550±450Pa·s, or 550±400Pa·s, or 550±350Pa·s, or 550±300Pa·s, or 550±250Pa·s, or 550±200Pa·s, or 550±150Pa·s, or 550±100Pa·s, or 550±50Pa·s, or 600±550Pa·s, or 600±500Pa·s, or 600±450Pa·s, or 600±400Pa·s, or 600±350Pa·s, or 600±300Pa·s, or 600±250Pa·s, or 600±200Pa·s, or 600±150Pa·s, or 600±100Pa·s, or 600±50Pa·s, or 650±600Pa·s, or 650±550Pa·s, or 650±500Pa·s, or 650±450Pa·s, or 650±400Pa·s, or 650±350Pa·s, or 650±300Pa·s, or 650±250Pa·s, or 650±200Pa·s,or 650±150Pa·s, or 650±100Pa·s, or 650±50Pa·s, or 700±650Pa·s, or 700±600Pa·s, or 700±550Pa·s, or 700±500Pa·s, or 700±450Pa·s, or 700±400Pa·s, or 700±350Pa·s, or 700±300Pa·s, or 700±250Pa·s, or 700±200Pa·s, or 700±150Pa·s, or 700±100Pa·s, or 700±50Pa·s. ,

[0284] Preferably, the viscosity of the composition at 25 °C as determined according to ASTM D1084-16 is 10 ± 5.0 Pa·s, or 15 ± 10 Pa·s, or 15 ± 5.0 Pa·s, or 20 ± 15 Pa·s, or 20 ± 10 Pa·s, or 20 ± 5.0 Pa·s, or 25 ± 20 Pa·s, or 25 ± 15 Pa·s, or 25 ± 10 Pa·s, or 25 ± 5.0 Pa·s, or 30 ± 25 Pa·s, or 30 ± 20 Pa·s, or 30 ± 15 Pa·s, or 30 ± 10 Pa·s, or 30 ± 5.0 Pa·s, or 35 ± 30 Pa·s, or 35 ± 25 Pa·s, or 35 ± 20 Pa·s, or 35 ± 15 Pa·s, or 35 ± 10 Pa·s, or 35 ± 5.0 Pa·s, or 40 ± 35 Pa·s, or 40 ± 30 Pa·s, or 40 ± 25 Pa·s, or 40 ± 20 Pa·s, or 40 ± 15 Pa·s, or 40 ± 10 Pa·s, or 40 ± 5.0 Pa·s, or 45 ± 40 Pa·s, or 45 ± 35 Pa·s, or 45 ± 30 Pa·s, or 45 ± 25 Pa·s, or 45 ± 20 Pa·s, or 45 ± 15 Pa·s, or 45 ± 10 Pa·s, or 45 ± 5.0 Pa·s, or 50 ± 45 Pa·s, or 50 ± 40 Pa·s, or 50 ± 35 Pa·s, or 50 ± 30 Pa·s, or 50 ± 25 Pa·s, or 50 ± 20 Pa·s, or 50 ± 15 Pa·s, or 50 ± 10 Pa·s, or 50 ± 5.0 Pa·s, or 55 ± 50 Pa·s, or 55 ± 45 Pa·s, or 55 ± 40 Pa·s, or 55 ± 35 Pa·s, or 55 ± 30 Pa·s, or 55 ± 25 Pa·s, or 55 ± 20 Pa·s, or 55 ± 15 Pa·s, or 55 ± 10 Pa·s, or 55 ± 5.0 Pa·s, or 60 ± 55 Pa·s, or 60 ± 50 Pa·s, or 60 ± 45 Pa·s, or 60 ± 40 Pa·s, or 60 ± 35 Pa·s, or 60 ± 30 Pa·s, or 60 ± 25 Pa·s, or 60 ± 20 Pa·s, or 60 ± 15 Pa·s, or 60 ± 10 Pa·s, or 60 ± 5.0 Pa·s, or 65 ± 60 Pa·s, or 65 ± 55 Pa·s, or 65 ± 50 Pa·s, or 65 ± 45 Pa·s, or 65 ± 40 Pa·s, or 65 ± 35 Pa·s, or 65 ± 30 Pa·s, or 65 ± 25 Pa·s, or 65 ± 20 Pa·s, or 65 ± 15 Pa·s, or 65 ± 10 Pa·s, or 65 ± 5.0Pa·s, or 70±65Pa·s, or 70±60Pa·s, or 70±55Pa·s, or 70±50Pa·s, or 70±45Pa·s, or 70±40Pa·s, or 70±35Pa·s, or 70±30Pa·s, or 70±25Pa·s, or 70±20Pa·s, or 70±15Pa·s, or 70±10Pa·s, or 70±5.0Pa·s. .

[0285] Preferably, the one-component adhesive composition according to the invention is wash-off resistant; preferably wash-off resistant according to BMW standard AA-0044 from January 2018. Preferably, the wash-off resistance test involves the following steps:

[0286] (a) Apply beads of the adhesive composition to a substrate having an oil layer (PL3802-39S, 1.5 g / m 2 =0.12g) of hot-dip galvanized steel sheet (DX54D+Z100, 200×40mm), wherein the steel sheet is used as a substrate without a top plate;

[0287] (b) without pre-curing, the sample thus prepared was placed in an immersion fixture and dropped unhindered from a height of 20 cm into a tank filled with room temperature pure water;

[0288] (c) installing the sample into a stirrer in a second tank filled with pure water preheated to 60° C.;

[0289] (d) stirring the sample at 140 rpm (1.47 m / s) for 3 min;

[0290] (e) The sample is removed and visually inspected, wherein the adhesive composition passes the wash-off resistance test when no significant change in the adhesive composition is detected.

[0291] Preferably, the composition is resistant to ageing; preferably resistant to ageing under humid conditions; more preferably resistant to ageing according to PSA D47 1165, preferably PSA D47 1165 (H7).

[0292] Preferably, the one-component adhesive composition according to the invention is thermally expandable.

[0293] Preferably, the composition exhibits a volume expansion at 190°C of at least 10 vol.-%, preferably at least 50 vol.-%, more preferably at least 100 vol.-%, still more preferably at least 150 vol.-%, relative to the volume of the composition before expansion.

[0294] Preferably, the composition exhibits a volume expansion at 190°C of at most 450 vol%, preferably at most 400 vol%, more preferably at most 350 vol%, still more preferably at most 300 vol%, relative to the volume of the composition before expansion.

[0295] Preferably, the composition exhibits a volume expansion at 190° C. in the range of 250±100 vol%, preferably 250±50 vol%, relative to the volume of the composition before expansion.

[0296] Another aspect of the present invention relates to a method for preparing a reinforced structural member, the method comprising the steps of:

[0297] (a) applying the composition according to the present invention as described above to the surface of a structural element;

[0298] (b) curing the applied composition, thereby obtaining a reinforced structural member comprising the composition in a cured state.

[0299] Preferably, step (a) of the process according to the invention involves extrusion.

[0300] Preferably, step (a) of the method according to the invention is performed with the aid of automated means.

[0301] Another aspect of the invention relates to a reinforced structural member comprising a structural element and a composition according to the invention as described above in the cured state.

[0302] Preferably, the reinforcing structural member is a structural panel stiffener.

[0303] Another aspect of the invention relates to the use of a composition according to the invention as described above or a reinforced structural member according to the invention as described above in the manufacture of a vehicle.

[0304] The following examples further illustrate the present invention but should not be construed as limiting its scope.

[0305] A curable one-component adhesive composition was prepared containing the following ingredients in the following weight amounts. The composition was applied to a substrate and tested for wash-off resistance and aging resistance:

[0306]

[0307] As demonstrated by the above comparative data, when the composition comprises a combination of an inosilicate and a metal oxide (Examples 3 and 5), the loss in lap shear (Δ lap shear) is improved even when a relatively low amount of inosilicate is used (Examples 1 and 2 comprise 14.69 wt.-% inosilicate, while Example 5 comprises only 9.79 wt.-% inosilicate).

[0308] The wash-off resistance was tested according to BMW standard AA-0044 from January 2018: Adhesive composition 8 was applied to a substrate having an oil layer (PL3802-39S, 1.5 g / m 2 =0.12g) of hot-dip galvanized steel sheets (DX54D+Z100, 200×40 mm). The adhesive beads were applied to the substrate. The samples had no top plate, only the substrate, on which the material was extruded to a defined thickness related to the final application. The adhesive was not pre-cured. The prepared samples were placed in an immersion fixture and dropped unhindered from a height of 20 cm into a water tank filled with water at room temperature. The samples were then mounted to a stirrer in a second water tank preheated to 60°C. Stirring was performed for 3 minutes at a speed of 140 rpm (1.47 m / s).

[0309] The aging resistance was tested for 3-point bending and lap shear samples using a wet patch test according to PSA D47 1165 (Δ lap shear [%] (after 7 days)). For the lap shear samples, two substrates (HX 420LAD 100) were adhesively bonded to each other with adhesive compositions 1 to 5 with a gap of 4 mm. The curing of the adhesive was carried out at 165°C for 30 minutes. For the 3-point bending samples, a 1.25 mm thick material was bonded to a 0.7 mm thin substrate and cured at 165°C for 30 minutes. For the wet patch, the sample was covered with cotton and then placed in a bag. The same weight of water and cotton was added, and the bag was then sealed and placed in an oven at 70°C for different times. After this step, the sample was placed at -20°C for 2 hours, then kept at room temperature (23°C) to warm up and reach room temperature. The samples were tested at intervals of 2 to 4 hours. Lap shear strength was measured at 23°C according to ASTM method D1002 and 3-point bend was measured at 23°C according to PSA standard D452025 after immersing the test specimens in a wet poultice at 70°C for various times.

Claims

1. A curable one-component adhesive composition comprising: (a) preferably comprises or consists essentially of a liquid glycidyl ether of a bisphenol, a liquid epoxy novolac resin, or a combination thereof; (b) latent epoxy curing agent; (c) silicon dioxide; preferably fumed silicon dioxide; (d) a metal oxide; preferably calcium oxide; and wherein the weight content of the liquid epoxy resin is at least 20 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition; and Optionally, the curable one-component adhesive composition additionally comprises one or more of the following components (e) to (p): (e) layered silicates; preferably clay and / or organophilic layered silicates; (f) inosilicate; preferably wollastonite; (g) a reactive diluent; preferably a glycidyl ether epoxy resin of cashew nut shell liquid; (h) an additional curable epoxy resin; preferably a semi-solid curable epoxy resin; (i) fibers, preferably discontinuous fibers; (j) polyhydroxycarboxylates; (k) polyamides; (l) a blowing agent; preferably azodicarbonamide; (m) impact modifier; (n) toughening agents and / or flexibilizers; (o) a phenoxy resin; preferably a solid phenoxy resin; more preferably a solid phenoxy resin which is a copolymer of bisphenol A and epichlorohydrin; and / or (p) Curing accelerator.

2. The composition according to claim 1, wherein the weight content of the liquid epoxy resin is at least 30 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

3. The composition according to claim 1 or 2, wherein the liquid epoxy resin comprises or consists essentially of composition: Liquid epoxy novolac resin; preferably liquid epoxy phenol novolac resin.

4. A composition according to any one of the preceding claims, wherein the liquid epoxy resin comprises or consists essentially of composition: Liquid bisphenol diglycidyl ether resin; preferably bisphenol A diglycidyl ether resin or bisphenol F diglycidyl ether resin.

5. A composition according to any one of the preceding claims, wherein the liquid epoxy resin comprises or consists essentially of composition: A mixture of a liquid epoxy novolac resin, preferably an epoxy phenol novolac resin, and a liquid bisphenol diglycidyl ether resin, preferably a diglycidyl ether resin of bisphenol A or a diglycidyl ether resin of bisphenol F.

6. The composition of claim 5, wherein the content of the liquid epoxy novolac resin is greater than the content of the liquid bisphenol diglycidyl ether resin.

7. The composition of claim 5, wherein the content of the liquid bisphenol diglycidyl ether resin is greater than the content of the liquid epoxy novolac resin.

8. The composition of claim 5, wherein the content of the liquid epoxy novolac resin is equal to the content of the liquid bisphenol diglycidyl ether resin.

9. The composition according to any one of the preceding claims, wherein the liquid epoxy resin, preferably the liquid epoxy novolac resin and / or the liquid bisphenol diglycidyl ether resin has an epoxy equivalent as determined according to ASTM D1652 in the range of 145 to 200 g / eq, preferably 160 to 185 g / eq, and more preferably 165 to 178 g / eq.

10. The composition according to any one of the preceding claims, wherein the viscosity of the liquid epoxy resin, preferably the liquid epoxy novolac resin and / or the liquid bisphenol diglycidyl ether resin at 25°C measured according to ASTM D2196 is in the range of 14 to 32 Pa·s, preferably 16 to 30 Pa·s, more preferably 18 to 28 Pa·s.

11. The composition according to any one of the preceding claims, wherein the epoxy functionality of the liquid epoxy resin, preferably the liquid epoxy novolac resin and / or the liquid bisphenol diglycidyl ether resin is in the range of 1.3 to 3.9, preferably 1.7 to 3.5, more preferably 2.1 to 3.

1.

12. The composition according to any of the preceding claims, wherein the weight content of the liquid epoxy resin is at least 32 wt.-%, preferably at least 34 wt.-%, more preferably at least 36 wt.-%, even more preferably at least 38 wt.-%, and still more preferably at least 40 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

13. The composition according to any of the preceding claims, wherein the weight content of the liquid epoxy resin is at most 74 wt.-%, preferably at most 70 wt.-%, more preferably at most 66 wt.-%, even more preferably at most 62 wt.-%, still more preferably at most 58 wt.-%, even more preferably at most 52 wt.-%, most preferably at most 48 wt.-%, and in particular at most 44 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

14. The composition according to any of the preceding claims, wherein the weight content of the liquid epoxy resin is in the range of 40±20 wt.-%, preferably 40±10 wt.-%, based on all liquid epoxy resins contained in the composition and relative to the total weight of the one-component adhesive composition.

15. A composition according to any one of the preceding claims, wherein the latent epoxy curing agent is selected from the group consisting of dicyandiamide, aliphatic or aromatic amines or their respective adducts, amidoamines, polyamides, alicyclic amines, anhydrides, polycarboxylic acid polyesters, isocyanates, phenolic resins (preferably selected from phenol or cresol novolac resins, copolymers of phenol terpenes, polyvinylphenol, or bisphenol A formaldehyde copolymers, bishydroxyphenylalkanes), modified and unmodified polyamines or polyamides (preferably selected from triethylenetetramine, diethylenetriamine, tetraethylenepentamine and cyanoguanidine); preferably dicyandiamide.

16. A composition according to any of the preceding claims, wherein the weight content of the latent epoxy curing agent is at least 1.4 wt.-%, preferably at least 1.6 wt.-%, more preferably at least 1.8 wt.-%, even more preferably at least 2.0 wt.-%, still more preferably at least 2.2 wt.-%, even more preferably at least 2.4 wt.-%, most preferably at least 2.6 wt.-%, and in particular at least 2.8 wt.-%, relative to the total weight of the one-component adhesive composition.

17. A composition according to any of the preceding claims, wherein the weight content of the latent epoxy curing agent is at most 4.5 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.8 wt.-%, even more preferably at most 3.6 wt.-%, still more preferably at most 3.4 wt.-%, even more preferably at most 3.2 wt.-%, most preferably at most 3.0 wt.-%, and in particular at most 2.8 wt.-%, relative to the total weight of the one-component adhesive composition.

18. The composition according to any of the preceding claims, wherein the weight content of the latent epoxy curing agent is in the range of 2.8±1.5 wt.-%, preferably 2.8±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

19. The composition according to any one of the preceding claims, wherein the inosilicate has the form of particles, flakes, platelets, rods, needles and / or rectangles; preferably the form of needles.

20. A composition according to any one of the preceding claims, wherein the inosilicate is selected from wollastonite, rhodonite or philadelphite.

21. A composition according to any one of the preceding claims, wherein the inosilicate comprises or consists essentially of composition: Wollastonite; preferably wollastonite needles.

22. The composition according to any one of the preceding claims, wherein the inosilicate has an aspect ratio of at least 2.0, preferably at least 4.0, more preferably at least 6.0, still more preferably at least 8.0, still more preferably at least 10, and even more preferably at least 12.

23. The composition according to any one of the preceding claims, wherein the inosilicate has an aspect ratio of at most 22, preferably at most 20, more preferably at most 18, still more preferably at most 16, still more preferably at most 14, and even more preferably at most 12.

24. A composition according to any one of the preceding claims, wherein the inosilicate has an aspect ratio in the range of 12±5.0, preferably 12±2.

5.

25. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D10 determined by laser diffraction analysis according to ISO 13320 of at least 0.5 μm, preferably at least 1.0 μm, more preferably at least 1.5 μm, still more preferably at least 2.05 μm, still more preferably at least 2.5 μm, even more preferably at least 3.0 μm, most preferably at least 3.5 μm, and in particular at least 4.0 μm.

26. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D10 determined by laser diffraction analysis according to ISO 13320 of at most 12 μm, preferably at most 11 μm, more preferably at most 10 μm, still more preferably at most 9.0 μm, still more preferably at most 8.0 μm, even more preferably at most 7.0 μm, most preferably at most 6.0 μm, and in particular at most 5.0 μm.

27. The composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D10 determined by laser diffraction analysis according to ISO 13320 in the range of 4.0±2.0 μm, preferably 4.0±1.0 μm.

28. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D50 determined by laser diffraction analysis according to ISO 13320 of at least 10 μm, preferably at least 11 μm, more preferably at least 12 μm, still more preferably at least 13 μm, still more preferably at least 14 μm, even more preferably at least 15 μm, most preferably at least 16 μm, and in particular at least 17 μm.

29. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D50 determined by laser diffraction analysis according to ISO 13320 of at most 32 μm, preferably at most 30 μm, more preferably at most 28 μm, still more preferably at most 26 μm, still more preferably at most 24 μm, even more preferably at most 22 μm, most preferably at most 20 μm, and in particular at most 18 μm.

30. The composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D50 determined by laser diffraction analysis according to ISO 13320 in the range of 17±7.0 μm, preferably 17±3.5 μm.

31. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D90 determined by laser diffraction analysis according to ISO 13320 of at least 30 μm, preferably at least 35 μm, more preferably at least 40 μm, still more preferably at least 45 μm, still more preferably at least 50 μm, even more preferably at least 55 μm, most preferably at least 60 μm, and in particular at least 65 μm.

32. A composition according to any one of the preceding claims, wherein the inosilicate has a volume median diameter D90 determined by laser diffraction analysis according to ISO 13320 of at most 120 μm, preferably at most 110 μm, more preferably at most 100 μm, still more preferably at most 90 μm, still more preferably at most 85 μm, even more preferably at most 80 μm, most preferably at most 75 μm, and in particular at most 70 μm.

33. Composition according to any of the preceding claims, wherein the inosilicate has a volume median diameter D90 determined by laser diffraction analysis according to ISO 13320 in the range of 65±30 μm, preferably 65±15 μm.

34. A composition according to any one of the preceding claims, wherein the average length of the inosilicate is at least 30 μm, preferably at least 35 μm, more preferably at least 40 μm, still more preferably at least 45 μm, still more preferably at least 50 μm, even more preferably at least 55 μm, most preferably at least 60 μm, and in particular at least 65 μm.

35. A composition according to any one of the preceding claims, wherein the average length of the chain silicate is at most 105 μm, preferably at most 100 μm, more preferably at most 95 μm, still more preferably at most 90 μm, still more preferably at most 85 μm, even more preferably at most 80 μm, most preferably at most 75 μm, and in particular at most 70 μm.

36. A composition according to any one of the preceding claims, wherein the average length of the inosilicate is in the range of 65±30 μm, preferably 65±15 μm.

37. A composition according to any one of the preceding claims, wherein the average width of the inosilicate is at least 1.0 μm, preferably at least 2.0 μm, more preferably at least 3.0 μm, still more preferably at least 4.0 μm, still more preferably at least 5.0 μm, even more preferably at least 6.0 μm, and most preferably at least 7.0 μm.

38. A composition according to any one of the preceding claims, wherein the average width of the inosilicate is at most 20 μm, preferably at most 18 μm, more preferably at most 16 μm, still more preferably at most 14 μm, still more preferably at most 12 μm, even more preferably at most 10 μm, most preferably at most 9.0 μm, and in particular at most 8.0 μm.

39. A composition according to any one of the preceding claims, wherein the average width of the inosilicate is in the range of 7.0±5.0 μm, preferably 7.0±3.5 μm.

40. A composition according to any of the preceding claims, wherein the weight content of the linear silicate is at least 3.0 wt.-%, preferably at least 4.0 wt.-%, more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, still more preferably at least 7.0 wt.-%, even more preferably at least 8.0 wt.-%, most preferably at least 9.0 wt.-%, and in particular at least 10 wt.-%, relative to the total weight of the one-component adhesive composition.

41. A composition according to any of the preceding claims, wherein the weight content of the linear silicate is at most 30 wt.-%, preferably at most 28 wt.-%, more preferably at most 26 wt.-%, even more preferably at most 24 wt.-%, still more preferably at most 22 wt.-%, even more preferably at most 20 wt.-%, most preferably at most 18 wt.-%, and in particular at most 16 wt.-%, relative to the total weight of the one-component adhesive composition.

42. The composition according to any of the preceding claims, wherein the weight content of the inosilicate is in the range of 15±7.0 wt.-%, preferably 15±3.5 wt.-%, relative to the total weight of the one-component adhesive composition.

43. A composition according to any one of the preceding claims, wherein the metal oxide is selected from the group consisting of CaO, MgO, BaO, K 2 O. Li 2 O、Na 2 O and mixtures thereof; preferably CaO.

44. A composition according to any of the preceding claims, wherein the weight content of the metal oxide is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%, relative to the total weight of the one-component adhesive composition.

45. A composition according to any of the preceding claims, wherein the weight content of the metal oxide is at most 20 wt.-%, preferably at most 18 wt.-%, more preferably at most 16 wt.-%, even more preferably at most 14 wt.-%, still more preferably at most 12 wt.-%, even more preferably at most 10 wt.-%, most preferably at most 8.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

46. ​​The composition according to any of the preceding claims, wherein the weight content of the metal oxide is in the range of 5.0±4.0 wt.-%, preferably 5.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

47. A composition according to any of the preceding claims, wherein the layered silicate has the form of particles, flakes, platelets, rods, needles and / or rectangles.

48. A composition according to any one of the preceding claims, wherein the layered silicate comprises or consists essentially of composition: Organically modified layered silicates; Preference is given to organophilic layered silicates.

49. A composition according to any one of the preceding claims, wherein the layered silicate comprises or consists essentially of composition: Phosphosilicate; preferably zinc phosphosilicate; more preferably organically modified zinc phosphosilicate; still more preferably strontium zinc phosphosilicate.

50. A composition according to any of the preceding claims, wherein the total weight content of the layered silicate is at least 0.5 wt.-%, preferably at least 1.0 wt.-%, more preferably at least 1.5 wt.-%, even more preferably at least 2.0 wt.-%, still more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, most preferably at least 3.5 wt.-%, and in particular at least 4.0 wt.-%, relative to the total weight of the one-component adhesive composition.

51. A composition according to any of the preceding claims, wherein the total weight content of the layered silicate is at most 19 wt.-%, preferably at most 17 wt.-%, more preferably at most 15 wt.-%, even more preferably at most 13 wt.-%, still more preferably at most 11 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

52. The composition according to any of the preceding claims, wherein the total weight content of the layered silicate is in the range of 4.0±3.0 wt.-%, preferably 4.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

53. A composition according to any of the preceding claims, wherein the silica is fumed silica, fused silica, silica gel or quartz; preferably fumed silica; more preferably surface treated fumed silica; even more preferably hydrophobic fumed silica; still more preferably dimethicone treated fumed silica.

54. A composition according to any of the preceding claims, wherein the total weight content of silica is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%, relative to the total weight of the one-component adhesive composition.

55. A composition according to any of the preceding claims, wherein the total weight content of silica is at most 19 wt.-%, preferably at most 17 wt.-%, more preferably at most 15 wt.-%, even more preferably at most 13 wt.-%, still more preferably at most 11 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

56. The composition according to any of the preceding claims, wherein the total weight content of silica is in the range of 5.0±3.0 wt.-%, preferably 5.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

57. A composition according to any one of the preceding claims, wherein the reactive diluent comprises -hydroxy functionality; -aldehyde functionality; -epoxy functionality; -oxazolidine functionality; and / or -lactone functionality; preferably epoxy functionality.

58. The composition of any preceding claim, wherein the reactive diluent is a glycidyl ether epoxy resin.

59. A composition according to any one of the preceding claims, wherein the reactive diluent is selected from phenyl glycidyl ether, alkylphenol monoglycidyl ether, aliphatic monoglycidyl ether, alkylphenol monoglycidyl ether, alkylphenol monoglycidyl ether, 3-glycidyloxypropyl trimethoxysilane, 3-glycidyloxypropyl trimethoxysilane, 3-glycidyloxypropyl methyl dimethoxysilane, 1-(3-glycidyloxypropyl) 1,1,3,3,3-pentamethyldisiloxane, 1,4-butanediol diglycidyl ether, 1,6-hexanediol diglycidyl ether, Glycol diglycidyl ether, 1,4-cyclohexanedimethanol, glycidyl ether of soybean oil, glycidyl ether of linseed oil, glycidyl ether of cashew nut shell liquid, diglycidyl ether of resorcinol, diglycidyl ether of cyclohexanedimethanol, diglycidyl ether of neopentyl glycol, diglycidyl ether of cashew nut shell liquid, triglycidyl ether of trimethylolpropane dipentene, trimethylolpropane triglycidyl ether, glycerol triglycidyl ether, pentaerythritol tetraglycidyl ether and mixtures thereof; preferably glycidyl ether of cashew nut shell liquid, diglycidyl ether of cashew nut shell liquid and mixtures thereof.

60. A composition according to any preceding claim, wherein the reactive diluent has more than one epoxy functional group; preferably two epoxy functional groups.

61. A composition according to any one of the preceding claims, wherein the reactive diluent is a diglycidyl ether of cashew nut shell liquid.

62. The composition according to any one of the preceding claims, wherein the epoxy equivalent of the reactive diluent measured according to ASTM D1652 is in the range of 290 to 450 g / eq, preferably 305 to 435 g / eq, and more preferably 320 to 420 g / eq.

63. The composition according to any one of the preceding claims, wherein the viscosity of the reactive diluent at 25°C measured according to ASTM D2196 is in the range of 0.25 to 12 Pa·s, preferably 0.5 to 6.0 Pa·s, more preferably 1.0 to 3.0 Pa·s.

64. A composition according to any of the preceding claims, wherein the weight content of the reactive diluent is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, still more preferably at least 3.5 wt.-%, even more preferably at least 4.0 wt.-%, most preferably at least 4.5 wt.-%, and in particular at least 5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

65. A composition according to any of the preceding claims, wherein the weight content of the reactive diluent is at most 16 wt.-%, preferably at most 14 wt.-%, more preferably at most 12 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

66. The composition according to any of the preceding claims, wherein the weight content of the reactive diluent is in the range of 5.5±3.0 wt.-%, preferably 5.5±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

67. The composition according to any one of the preceding claims, wherein the additional curable epoxy resin is selected from bisphenol diglycidyl ether resins, epoxy novolac resins, preferably epoxy phenol novolac resins, and combinations thereof.

68. A composition according to any one of the preceding claims, wherein the additional curable epoxy resin comprises or consists essentially of composition: Epoxy novolac resin, preferably epoxy phenol novolac resin; preferably semi-solid epoxy novolac resin, preferably epoxy phenol novolac resin.

69. A composition according to any one of the preceding claims, wherein the additional curable epoxy resin comprises or consists essentially of composition: Bisphenol diglycidyl ether resin; preferably dimer acid modified epoxy resin.

70. The composition according to any of the preceding claims, wherein the additional curable epoxy resin, preferably the epoxy novolac resin, preferably the epoxy phenol novolac resin, has an epoxide equivalent weight determined according to ASTM D1652 in the range of 150 to 210 g / eq, preferably 160 to 200 g / eq, and more preferably 170 to 190 g / eq.

71. The composition according to any one of the preceding claims, wherein the additional curable epoxy resin, preferably the dimer acid-modified epoxy resin, has an epoxy equivalent weight determined according to ASTM D1652 in the range of 400 to 900 g / eq, preferably 500 to 800 g / eq, and more preferably 600 to 700 g / eq.

72. The composition of any preceding claim, wherein the additional curable epoxy resin has a viscosity at 55°C of at least 100 Pa·s, preferably at least 125 Pa·s, more preferably at least 150 Pa·s, as determined according to ASTM D2196.

73. A composition according to any preceding claim, wherein the additional curable epoxy resin has an epoxy functionality in the range of 0.3 to 2.9, preferably 0.7 to 2.5, more preferably 1.1 to 2.

1.

74. A composition according to any of the preceding claims, wherein the weight content of the additional curable epoxy resin is at least 0.5 wt.-%, preferably at least 0.8 wt.-%, more preferably at least 1.1 wt.-%, even more preferably at least 1.4 wt.-%, still more preferably at least 1.7 wt.-%, even more preferably at least 2.0 wt.-%, most preferably at least 2.3 wt.-%, and in particular at least 2.6 wt.-%, relative to the total weight of the one-component adhesive composition.

75. A composition according to any of the preceding claims, wherein the weight content of the additional curable epoxy resin is at most 10 wt.-%, preferably at most 9.0 wt.-%, more preferably at most 8.0 wt.-%, even more preferably at most 7.0 wt.-%, still more preferably at most 6.0 wt.-%, even more preferably at most 5.0 wt.-%, most preferably at most 4.0 wt.-%, and in particular at most 3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

76. The composition according to any of the preceding claims, wherein the weight content of the additional curable epoxy resin is in the range of 2.6±2.0 wt.-%, preferably 2.6±1.0 wt.-%, relative to the total weight of the one-component adhesive composition.

77. The composition of any of the preceding claims, wherein the fibers are in the form of aggregates, hollow materials, chopped materials, or mixtures thereof.

78. A composition according to any one of the preceding claims, wherein the fiber comprises or consists essentially of composition: Inorganic fibers, preferably glass (e.g. E-glass or S-glass) fibers or glass yarns; organic fibers, preferably polymer fibers, more preferably selected from polyamide (e.g. nylon) fibers, polyester fibers, carbon fibers, aramid fibers, polycarbonate fibers, polyethylene fibers, polypropylene fibers, polybutene (e.g. polybutylene terephthalate) fibers, polystyrene fibers, polyurethane fibers; or mixtures thereof.

79. The composition according to any of the preceding claims, wherein the fibers are selected from chopped glass fibers, chopped aramid fibers, aramid pulp, and mixtures thereof; preferably chopped glass fibers.

80. A composition according to any of the preceding claims, wherein the average length of the fibers is at least 0.5 mm, preferably at least 1.0 mm, more preferably at least 1.5 mm, even more preferably at least 2.0 mm, still more preferably at least 2.5 mm, even more preferably at least 3.0 mm, most preferably at least 3.5 mm, and in particular at least 4.0 mm.

81. A composition according to any one of the preceding claims, wherein the average length of the fibers is at most 45 mm, preferably at most 40 mm, more preferably at most 35 mm, still more preferably at most 30 mm, still more preferably at most 25 mm, even more preferably at most 20 mm, most preferably at most 15 mm, and in particular at most 10 mm.

82. A composition according to any one of the preceding claims, wherein the average length of the fibers is in the range of 7.0±6.0 mm, preferably 7.0±3.0 mm.

83. A composition according to any of the preceding claims, wherein the average diameter of the fibers is at least 3.0 μm, preferably at least 4.0 μm, more preferably at least 5.0 μm, still more preferably at least 6.0 μm, still more preferably at least 7.0 μm, even more preferably at least 8.0 μm, most preferably at least 9.0 μm, and in particular at least 10 μm.

84. A composition according to any of the preceding claims, wherein the average diameter of the fibers is at most 45 μm, preferably at most 40 μm, more preferably at most 35 μm, still more preferably at most 30 μm, still more preferably at most 25 μm, even more preferably at most 20 μm, most preferably at most 15 μm, and in particular at most 12 μm.

85. A composition according to any one of the preceding claims, wherein the average diameter of the fibers is in the range of 10±4.0 mm, preferably 10±2.0 mm.

86. A composition according to any of the preceding claims, wherein the weight content of the fibers is at least 1.5 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 2.5 wt.-%, even more preferably at least 3.0 wt.-%, still more preferably at least 3.5 wt.-%, even more preferably at least 4.0 wt.-%, most preferably at least 4.5 wt.-%, and in particular at least 5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

87. A composition according to any of the preceding claims, wherein the weight content of the fibers is at most 13 wt.-%, preferably at most 12 wt.-%, more preferably at most 11 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

88. A composition according to any of the preceding claims, wherein the weight content of the fibers is in the range of 6.0±3.0 wt.-%, preferably 6.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

89. A composition according to any of the preceding claims, wherein the total weight content of the polyhydroxycarboxylic acid ester is at least 0.2 wt.-%, preferably at least 0.3 wt.-%, more preferably at least 0.4 wt.-%, even more preferably at least 0.5 wt.-%, still more preferably at least 0.6 wt.-%, even more preferably at least 0.7 wt.-%, most preferably at least 0.8 wt.-%, and in particular at least 0.9 wt.-%, relative to the total weight of the one-component adhesive composition.

90. A composition according to any of the preceding claims, wherein the total weight content of the polyhydroxycarboxylic acid ester is at most 5.0 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.0 wt.-%, even more preferably at most 2.0 wt.-%, still more preferably at most 1.6 wt.-%, even more preferably at most 1.4 wt.-%, most preferably at most 1.2 wt.-%, and in particular at most 1.0 wt.-%, relative to the total weight of the one-component adhesive composition.

91. A composition according to any of the preceding claims, wherein the total weight content of the polyhydroxycarboxylic acid ester is in the range of 1.0±0.9 wt.-%, preferably 1.0±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

92. The composition of any preceding claim, wherein the polyamide is a polyamide powder.

93. A composition according to any of the preceding claims, wherein the total weight content of the polyamide is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%, relative to the total weight of the one-component adhesive composition.

94. A composition according to any of the preceding claims, wherein the total weight content of the polyamide is at most 15 wt.-%, preferably at most 12 wt.-%, more preferably at most 11 wt.-%, even more preferably at most 10 wt.-%, still more preferably at most 9.0 wt.-%, even more preferably at most 8.0 wt.-%, most preferably at most 7.0 wt.-%, and in particular at most 6.0 wt.-%, relative to the total weight of the one-component adhesive composition.

95. The composition according to any of the preceding claims, wherein the total weight content of the polyamide is in the range of 5.0±3.0 wt.-%, preferably 5.0±1.5 wt.-%, relative to the total weight of the one-component adhesive composition.

96. The composition according to any of the preceding claims, wherein the blowing agent is selected from the group consisting of azodicarbonamide, dinitrosopentamethylenetetramine, hydrazides such as 4,4-oxy-bis-(benzenesulfonylhydrazide), trihydrazinotriazine, N,N′-dimethyl-N,N′-dinitrosoterephthalamide, toluenesulfonylhydrazide (TSH), p-toluenesulfonylsemicarbazide (TSSC), 5-phenyltetrazole (5-PT) or NN′-dinitrosopentamethylenetetramine (DNPT); preferably azodicarbonamide.

97. A composition according to any of the preceding claims, wherein the weight content of the blowing agent is at least 0.2 wt.-%, preferably at least 0.3 wt.-%, more preferably at least 0.4 wt.-%, even more preferably at least 0.5 wt.-%, still more preferably at least 0.6 wt.-%, even more preferably at least 0.7 wt.-%, most preferably at least 0.8 wt.-%, and in particular at least 0.9 wt.-%, relative to the total weight of the one-component adhesive composition.

98. A composition according to any of the preceding claims, wherein the weight content of the blowing agent is at most 5.0 wt.-%, preferably at most 4.0 wt.-%, more preferably at most 3.0 wt.-%, even more preferably at most 2.0 wt.-%, still more preferably at most 1.6 wt.-%, even more preferably at most 1.4 wt.-%, most preferably at most 1.2 wt.-%, and in particular at most 1.0 wt.-%, relative to the total weight of the one-component adhesive composition.

99. The composition according to any of the preceding claims, wherein the weight content of the blowing agent is in the range of 1.0±0.9 wt.-%, preferably 1.0±0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

100. The composition of any of the preceding claims, wherein the impact modifier is selected from the group consisting of elastomer / epoxy adducts, core-shell impact modifiers, and combinations thereof.

101. The composition of any of the preceding claims, comprising a first impact modifier and optionally a second impact modifier.

102. The composition of any of the preceding claims, wherein the first impact modifier comprises a methyl methacrylate-butadiene-styrene (MBS) core-shell polymer.

103. The composition according to any of the preceding claims, wherein the first impact modifier is a solid impact modifier; preferably a solid methyl methacrylate-butadiene-styrene (MBS) core-shell impact modifier.

104. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the solid first impact modifier, relative to the total weight of the one-component adhesive composition is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%.

105. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the solid first impact modifier, relative to the total weight of the one-component adhesive composition is at most 22 wt.-%, preferably at most 20 wt.-%, more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, still more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, most preferably at most 10 wt.-%, and in particular at most 9.0 wt.-%.

106. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the solid first impact modifier, is in the range of 8.0±5.0 wt.-%, preferably 8.0±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

107. The composition of any of the preceding claims, wherein the first impact modifier is a liquid impact modifier; preferably a methyl methacrylate-butadiene-styrene (MBS) core-shell polymer dispersed in a bisphenol A epoxy resin.

108. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the liquid first impact modifier, relative to the total weight of the one-component adhesive composition is at least 6.0 wt.-%, preferably at least 8.0 wt.-%, more preferably at least 10 wt.-%, even more preferably at least 12 wt.-%, still more preferably at least 14 wt.-%, even more preferably at least 16 wt.-%, most preferably at least 18 wt.-%, and in particular at least 20 wt.-%.

109. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the liquid first impact modifier, relative to the total weight of the one-component adhesive composition is at most 36 wt.-%, preferably at most 34 wt.-%, more preferably at most 32 wt.-%, even more preferably at most 30 wt.-%, still more preferably at most 28 wt.-%, even more preferably at most 26 wt.-%, most preferably at most 24 wt.-%, and in particular at most 22 wt.-%.

110. A composition according to any of the preceding claims, wherein the weight content of the first impact modifier, preferably the liquid first impact modifier, is in the range of 20±10 wt.-%, preferably 20±5.0 wt.-%, relative to the total weight of the one-component adhesive composition.

111. A composition according to any of the preceding claims, wherein the second impact modifier is an elastomer / epoxy adduct; preferably a nitrile rubber modified epoxy resin; more preferably a nitrile rubber modified epoxy resin based on bisphenol-A-diglycidyl ether.

112. A composition according to any of the preceding claims, wherein the weight content of the second impact modifier is at least 1.0 wt.-%, preferably at least 2.0 wt.-%, more preferably at least 3.0 wt.-%, even more preferably at least 4.0 wt.-%, still more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, most preferably at least 7.0 wt.-%, and in particular at least 8.0 wt.-%, relative to the total weight of the one-component adhesive composition.

113. A composition according to any of the preceding claims, wherein the weight content of the second impact modifier is at most 22 wt.-%, preferably at most 20 wt.-%, more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, still more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, most preferably at most 10 wt.-%, and in particular at most 9.0 wt.-%, relative to the total weight of the one-component adhesive composition.

114. The composition according to any of the preceding claims, wherein the weight content of the second impact modifier is in the range of 8.0±5.0 wt.-%, preferably 8.0±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

115. A composition according to any of the preceding claims, wherein the toughening and / or flexibilizing agent is selected from the group consisting of polyolefins, polyurethanes, polyvinyl acetals, polyvinyl acetates, polyvinyl alcohols, polytetrafluoroethylenes, acrylic resins, polyvinyl chlorides, polyvinylidene chlorides, polystyrenes, and combinations thereof; preferably polyurethanes, polyvinyl acetals, and combinations thereof.

116. A composition according to any one of the preceding claims, wherein the toughening agent and / or flexibilizing agent comprises or consists essentially of composition: A blocked polyurethane adduct and / or polyvinyl acetal resin; preferably a phenol blocked polyurethane adduct and / or polyvinyl butyral resin.

117. A composition according to any of the preceding claims, wherein the total weight content of the toughener and / or flexibilizer is at least 1.0 wt.-%, preferably at least 1.5 wt.-%, more preferably at least 2.0 wt.-%, even more preferably at least 2.5 wt.-%, still more preferably at least 3.0 wt.-%, even more preferably at least 3.5 wt.-%, most preferably at least 4.0 wt.-%, and in particular at least 4.5 wt.-%, relative to the total weight of the one-component adhesive composition.

118. A composition according to any of the preceding claims, wherein the total weight content of the toughener and / or flexibilizer is at most 18 wt.-%, preferably at most 16 wt.-%, more preferably at most 14 wt.-%, even more preferably at most 12 wt.-%, still more preferably at most 10 wt.-%, even more preferably at most 9.0 wt.-%, most preferably at most 8.0 wt.-%, and in particular at most 7.0 wt.-%, relative to the total weight of the one-component adhesive composition.

119. A composition according to any of the preceding claims, wherein the total weight content of the toughener and / or flexibilizer is in the range of 6.0±4.0 wt.-%, preferably 6.0±2.0 wt.-%, relative to the total weight of the one-component adhesive composition.

120. A composition according to any of the preceding claims, wherein the weight content of the phenoxy resin is at least 3.0 wt.-%, preferably at least 4.0 wt.-%, more preferably at least 5.0 wt.-%, even more preferably at least 6.0 wt.-%, still more preferably at least 7.0 wt.-%, even more preferably at least 8.0 wt.-%, most preferably at least 9.0 wt.-%, and in particular at least 10 wt.-%, relative to the total weight of the one-component adhesive composition.

121. A composition according to any of the preceding claims, wherein the weight content of the phenoxy resin is at most 26 wt.-%, preferably at most 24 wt.-%, more preferably at most 22 wt.-%, even more preferably at most 20 wt.-%, still more preferably at most 18 wt.-%, even more preferably at most 16 wt.-%, most preferably at most 14 wt.-%, and in particular at most 12 wt.-%, relative to the total weight of the one-component adhesive composition.

122. The composition according to any of the preceding claims, wherein the weight content of the phenoxy resin is in the range of 10±6.0 wt.-%, preferably 10±3.0 wt.-%, relative to the total weight of the one-component adhesive composition.

123. The composition according to any one of the preceding claims, wherein the curing accelerator is selected from the group consisting of modified or unmodified ureas, imidazoles, secondary amines, tertiary amines, quaternary ammonium salts and pyridines; preferably modified ureas.

124. A composition according to any of the preceding claims, wherein the weight content of the curing accelerator is at least 0.1 wt.-%, preferably at least 0.2 wt.-%, more preferably at least 0.25 wt.-%, even more preferably at least 0.3 wt.-%, still more preferably at least 0.35 wt.-%, even more preferably at least 0.4 wt.-%, most preferably at least 0.45 wt.-%, and in particular at least 0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

125. A composition according to any of the preceding claims, wherein the weight content of the curing accelerator is at most 2.5 wt.-%, preferably at most 2.0 wt.-%, more preferably at most 1.75 wt.-%, even more preferably at most 1.5 wt.-%, still more preferably at most 1.25 wt.-%, even more preferably at most 1.0 wt.-%, most preferably at most 0.75 wt.-%, and in particular at most 0.5 wt.-%, relative to the total weight of the one-component adhesive composition.

126. The composition according to any of the preceding claims, wherein the weight content of the curing accelerator is in the range of 0.5±0.4 wt.-%, preferably 0.5±0.2 wt.-%, relative to the total weight of the one-component adhesive composition.

127. The composition of any of the preceding claims, additionally comprising a filler selected from the group consisting of carbonates, borates, oxides, hydroxides, sulfates, titanates, zirconates, and mixtures thereof.

128. A composition according to any one of the preceding claims, comprising or consisting essentially of composition: - (a) a liquid epoxy resin and optionally (g) a reactive diluent, wherein the total weight content of the liquid epoxy resin and the reactive diluent is at least 40 wt.-%, preferably at least 42.5 wt.-%, more preferably at least 45 wt.-%, even more preferably at least 47.5 wt.-%, still more preferably at least 50 wt.-%, even more preferably at least 52.5 wt.-%, most preferably at least 55 wt.-%, and in particular at least 57.5 wt.-%, relative to the total weight of the one-component adhesive composition; -(b) latent epoxy curing agent; - (c) silicon dioxide; - (d) metal oxides; - (e) layered silicates and / or (f) chain silicates, wherein the total weight content of the layered silicates and / or chain silicates is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition; - (m) an impact modifier and / or (n) a toughener and / or a flexibilizer, wherein the total weight content of the impact modifier and / or the toughener and / or the flexibilizer is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition.

129. A composition according to any one of the preceding claims, comprising or consisting essentially of composition: - (a) a liquid epoxy resin and optionally (g) a reactive diluent, wherein the total weight content of the liquid epoxy resin and the reactive diluent is at least 40 wt.-%, preferably at least 42.5 wt.-%, more preferably at least 45 wt.-%, even more preferably at least 47.5 wt.-%, still more preferably at least 50 wt.-%, even more preferably at least 52.5 wt.-%, most preferably at least 55 wt.-%, and in particular at least 57.5 wt.-%, relative to the total weight of the one-component adhesive composition; -(b) latent epoxy curing agent; - (c) silicon dioxide; - (d) metal oxides; - (e) layered silicates and / or (f) chain silicates, wherein the total weight content of the layered silicates and / or chain silicates is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition; - (l) a blowing agent; -(m) an impact modifier and / or (n) a toughener and / or a flexibilizer, wherein the total weight content of the impact modifier and / or the toughener and / or the flexibilizer is at least 2.5 wt.-%, preferably at least 5 wt.-%, more preferably at least 7.5 wt.-%, even more preferably at least 10 wt.-%, still more preferably at least 12.5 wt.-%, even more preferably at least 15 wt.-%, most preferably at least 17.5 wt.-%, and in particular at least 20 wt.-%, relative to the total weight of the one-component adhesive composition.

130. A composition according to any preceding claim which is heat curable.

131. A composition according to any preceding claim which is pumpable.

132. A composition according to any of the preceding claims, wherein the composition is pumpable at a temperature of at least 20°C, preferably at least 25°C, more preferably at least 30°C, even more preferably at least 35°C, still more preferably at least 40°C, even more preferably at least 45°C, most preferably at least 50°C, and in particular at least 55°C.

133. A composition according to any of the preceding claims, wherein the composition is pumpable at a temperature of at most 105°C, preferably at most 100°C, more preferably at most 95°C, even more preferably at most 90°C, still more preferably at most 85°C, even more preferably at most 80°C, most preferably at most 75°C, and in particular at most 70°C.

134. A composition according to any preceding claim, wherein the composition is pumpable at a temperature in the range of 42±36°C, preferably 42±18°C.

135. A composition according to any of the preceding claims, having a viscosity at 25°C measured according to ASTM D1084-16 of at least 2.0 Pa·s, preferably at least 4.0 Pa·s, more preferably at least 6.0 Pa·s, even more preferably at least 8.0 Pa·s, still more preferably at least 10 Pa·s, even more preferably at least 12 Pa·s, most preferably at least 14 Pa·s, and in particular at least 16 Pa·s.

136. A composition according to any of the preceding claims, having a viscosity at 25°C of at most 120 Pa·s, preferably at most 110 Pa·s, more preferably at most 100 Pa·s, still more preferably at most 90 Pa·s, still more preferably at most 80 Pa·s, even more preferably at most 70 Pa·s, most preferably at most 60 Pa·s, and in particular at most 50 Pa·s, measured according to ASTM D1084-16.

137. The composition according to any of the preceding claims, having a viscosity at 25°C measured according to ASTM D1084-16 of 10±5.0 Pa·s, or 15±10 Pa·s, or 15±5.0 Pa·s, or 20±15 Pa·s, or 20±10 Pa·s, or 20±5.0 Pa·s, or 25±20 Pa·s, or 25±15 Pa·s, or 25±10 Pa·s, or 25±5.0 Pa·s, or 30±25 Pa·s, or 30±20 Pa·s, or 30±15 Pa·s, or 30±10 Pa·s, or 30±5.0 Pa·s, or 35±30 Pa·s, or 35±25 Pa·s, or 35±20 Pa·s. s, or 35±15Pa·s, or 35±10Pa·s, or 35±5.0Pa·s, or 40±35Pa·s, or 40±30Pa·s, or 40±25Pa·s, or 40±20Pa·s, or 40±15Pa·s, or 40±10Pa·s, or 40±5.0Pa·s, or 45±40Pa·s, or 45±35Pa·s, or 45±30Pa·s, or 45±25Pa·s, or 45±20Pa·s, or 45±15Pa·s, or 45±10Pa·s, or 45±5.0Pa·s, or 50±45Pa·s, or 50±40Pa·s a·s, or 50±35Pa·s, or 50±30Pa·s, or 50±25Pa·s, or 50±20Pa·s, or 50±15Pa·s, or 50±10Pa·s, or 50±5.0Pa·s, or 55±50Pa·s, or 55±45Pa·s, or 55±40Pa·s, or 55±35Pa·s, or 55±30Pa·s, or 55±25Pa·s, or 55±20Pa·s, or 55±15Pa·s, or 55±10Pa·s, or 55±5.0Pa·s, or 60±55Pa·s, or 60±50Pa·s, or 60±45 Pa·s, or 60±40Pa·s, or 60±35Pa·s, or 60±30Pa·s, or 60±25Pa·s, or 60±20Pa·s, or 60±15Pa·s, or 60±10Pa·s, or 60±5.0Pa·s, or 65±60Pa·s, or 65±55Pa·s, or 65±50Pa·s, or 65±45Pa·s, or 65±40Pa·s, or 65±35Pa·s, or 65±30Pa·s, or 65±25Pa·s, or 65±20Pa·s, or 65±15Pa·s, or 65±10Pa·s, or 65±5.0Pa·s, or 70±65Pa·s, or 70±60Pa·s, or 70±55Pa·s, or 70±50Pa·s, or 70±45Pa·s, or 70±40Pa·s, or 70±35Pa·s, or 70±30Pa·s, or 70±25Pa·s, or 70±20Pa·s, or 70±15Pa·s, or 70±10Pa·s, or 70±5.0Pa·s. .

138. A composition according to any of the preceding claims, which is wash-off resistant; preferably wash-off resistant according to BMW standard AA-0044 from January 2018.

139. The composition according to any of the preceding claims, which is resistant to ageing; preferably resistant to ageing under humid conditions; more preferably resistant to ageing according to PSA D47 1165, preferably PSA D47 1165 (H7).

140. A composition according to any preceding claim which is thermally expandable.

141. A composition according to any of the preceding claims, which exhibits a volume expansion of at least 10 vol.-%, preferably at least 50 vol.-%, more preferably at least 100 vol.-%, even more preferably at least 150 vol.-% at 190°C, relative to the volume of the composition before expansion.

142. The composition according to any of the preceding claims, which exhibits a volume expansion at 190°C of at most 450 vol.-%, preferably at most 400 vol.-%, more preferably at most 350 vol.-%, still more preferably at most 300 vol.-%, relative to the volume of the composition before expansion.

143. The composition according to any of the preceding claims, which exhibits a volume expansion at 190°C in the range of 250±100 vol.-%, preferably 250±50 vol.-%, relative to the volume of the composition before expansion.

144. A method for preparing a reinforced structural member, the method comprising the steps of: (a) applying a composition according to any one of the preceding claims onto the surface of a structural element; (b) curing the applied composition to obtain a reinforced structural member comprising the composition in a cured state.

145. The method of claim 144, wherein step (a) involves extrusion.

146. A method according to claim 144 or 145, wherein step (a) is performed with the aid of an automated device.

147. A reinforced structural member comprising a structural element and the composition of any one of claims 1-143 in a cured state.

148. The reinforced structural member of claim 147 which is a structural panel reinforcement.

149. Use of a composition according to any one of claims 1 to 143 or a reinforced structural member according to claim 147 or 148 in the manufacture of a vehicle.

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