WO2024083327A1

WO2024083327A1 - Flooring structure for reducing floor impact sound by using hybrid adhesive and manufacturing method therefor

Info

Publication number: WO2024083327A1
Application number: PCT/EP2022/079104
Authority: WO
Inventors: Jungsoo Kim; Chul-Kyu Kang
Original assignee: Wacker Chemie Ag
Priority date: 2022-10-19
Filing date: 2022-10-19
Publication date: 2024-04-25

Abstract

The present invention relates to a multilayered flooring structure for reducing floor impact sound and a manufacturing method therefor, the multilayered flooring structure comprising: a soft cushion sheet installed on a finishing mortar and having a plurality of perforated holes to be filled with an adhesive composition; a soft adhesive layer filling the perforated holes of the soft cushion sheet and formed on the surface of at least a portion of the soft cushion sheet; and a floor finishing material adhering to the surface of the soft adhesive layer.

Description

FLOORING STRUCTURE FOR REDUCING FLOOR IMPACT SOUND BY

USING HYBRID ADHESIVE AND MANUFACTURING METHOD THEREFOR

Technical Field

The present invention relates to application of an STPE-based hybrid adhesive to a multilayered flooring structure for reducing floor impact sound and, more specifically, to a multilayered flooring structure that reduces floor impact sound and a manufacturing method therefor .

Background Art

Floor impact sounds in multi-unit-housing, especially, apartments , are frequently classified into lightweight and heavyweight impact sounds . Lightweight impact sounds , such as the sound of a chair being dragged, the sound of a spoon falling, and the sound of light footsteps , can be sufficiently absorbed even in existing building structures and cause no problems in people ' s daily life . However, heavyweight impact sounds , such as the sound of children running on the floor and the sound of a heavy obj ect falling on the floor, are transmitted as they are to the floor below . Such noise between floors may cause conflict between residents .

In Korea , such a noise trouble between floors in multi-unit-housing is becoming a serious social problem. Therefore , the Ministry of Land, Infrastructure and Transport of Korea has prepared stricter floor impact sound performance test standards according to the Presidential Decree housing construction standards and the like . Accordingly, a method of reducing floor impact sound is urgently needed to cope with the stricter floor impact sound performance test standards .

Currently, two-component epoxy-based adhesives are mainly used as flooring adhesives in Korea . However, two- component epoxy-based adhesives contain bisphenol A, which is harmful to the human body, and are insufficient in floor impact sound reducing effect due to being rigid in a hard state after adhesion . On the other hand, silicone hybrid-based flooring adhesives do not contain components harmful to the human body and have impact cushioning characteristics due to being rigid in a rubbery state after adhesion, and thus such flooring adhesives can be a solution to reduce floor noise in multi-unit-housing . However, controlling the accuracy in the thickness of coating and the amount of adhesion when applying such adhesives is difficult during construction .

Disclosure of Invention

Technical Problem

An aspect of the present invention is to provide a multilayered flooring structure for reducing floor impact sound.

Another aspect of the present invention is to provide a method for constructing a multilayered flooring structure for reducing floor impact sound .

Solution to Problem

In accordance with an aspect of the present disclosure , there is provided a multilayered flooring structure for reducing floor impact sound, the multilayered flooring structure including : a soft cushion sheet installed on a finishing mortar and having a plurality of perforated holes to be filled with an adhesive composition; a soft adhesive layer filling the perforated holes of the soft cushion sheet and formed on the surface of at least a portion of the soft cushion sheet ; and a floor finishing material adhering to the surface of the soft adhesive layer .

In accordance with another aspect of the present disclosure , there is provided a method for manufacturing a multilayered flooring structure for reducing floor impact sound, the method including : installing a soft cushion sheet on a finishing mortar without separate surface smoothing, the soft cushion sheet having a plurality of perforated holes to be filled with an adhesive composition; forming a soft adhesive layer by filling the perforated holes of the soft cushion sheet with an adhesive composition and coating the adhesive composition on the surface of at least a portion of the soft cushion sheet , followed by curing; and allowing a floor finishing material to adhere to the surface of the soft adhesive layer .

Advantageous Ef fects of Invention

The multilayered flooring structure for reducing floor impact sound according to the present invention leads to leveling of non-unif ormity of the mortar surface by using a perforated soft cushion sheet and has enhanced adhesive strength by forming an STPE-based hybrid adhesive layer with a uniform thickness .

The multilayered flooring structure for reducing floor impact sound according to the present invention can obtain a maximum impact sound reducing ef fect by installing an elastic adhesive layer with a desired thickness .

The multilayered flooring structure for reducing floor impact sound according to the present invention can exhibit an eco-friendly effect of replacing an STPE-based hybrid adhesive with an existing two-component epoxy-based adhesive containing harmful bisphenol A .

The multilayered flooring structure for reducing floor impact sound according to the present invention is a novel flooring structure for reducing noise between floors and can be utilized as an effective flooring structure system in an existing building market .

Brief Description of Drawings

FIG . 1 is a schematic cross-sectional view of a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention .

FIG . 2 shows a construction process for a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention .

FIG . 3 shows , by steps , a specimen preparation procedure for an adhesion test on a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention .

FIG . 4 shows an on-site construction procedure for a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention .

FIG . 5 shows the adhesion test results of a conventional flooring structure .

FIG . 6 shows the adhesion tests results of a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention .

FIG . 7 shows the comparison results of floor impact sound reduction test on a flooring structure constructed using a modified silicone adhesive for reducing floor impact sound according to an embodiment of the present invention and a structure constructed using a conventional epoxy-based adhesive on site .

Best Mode for Carrying out the Invention

Hereinafter, exemplary embodiments of the present invention will be described in detail with reference to the accompanying drawings so that a person with ordinary skill in the art to which the present invention pertains can easily carry out the present invention . The present invention can be implemented in various different forms , and is not limited to the exemplary embodiments described herein .

To clearly describe the present invention, parts irrelevant to the description are omitted, and the same reference numerals will be given to the same or similar constituent elements throughout the specification .

In the drawings , the thicknesses of several layers and regions are enlarged so as to clearly express the layers and the regions . Moreover , in the drawings , the thicknesses of some layers and regions are exaggerated for convenience of explanation .

Hereinafter , the formation of any configuration at "an upper portion ( or a lower portion) " of a base material or "on ( or below ) " of the base material means that any configuration is formed to be brought into contact with an upper surface ( or a lower surface ) of the base material , and does not exclude that another configuration is included between the base material and any configuration formed on ( or below) the base material .

In an embodiment of the present invention, a multilayered flooring structure for reducing floor impact sound includes : a soft cushion sheet installed on a finishing mortar and having a plurality of perforated holes to be filled with an adhesive composition ; a soft adhesive layer filling the perforated holes of the soft cushion sheet and formed on the surface of at least a portion of the soft cushion sheet ; and a floor finishing material adhering to the surface of the soft adhesive layer .

Silicone hybrid-based flooring adhesives have a problem in that the accuracy in the thickness of adhesion and the amount of adhesion are difficult to control .

In a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention, the soft cushion sheet having a plurality of perforated holes to be filled with an adhesive composition is provided between the finishing mortar and the floor finishing material to thereby provide the thickness uniformity of the soft adhesive layer, ensure the accuracy in the amount of adhesion, achieve stronger adhesion between the finishing mortar and the floor finishing material , and show impact cushioning characteristics , thereby reducing impact noise .

FIG . 1 is a schematic cross-sectional view of a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention . Specifically, there is a structure of sequential stacking of : a soft cushion sheet 110 having a plurality of perforated holes 111 on a finishing mortar; a soft adhesive layer 120 filling the perforated holes 111 of the soft cushion sheet 110 and formed on the surface or at least a portion of the soft cushion sheet 110 ; a floor finishing material 30 adhering to a surface of the soft adhesive layer 120 .

The soft cushion sheet 110 may be a soft foam sheet or soft sheet containing, as a main ingredient , at least one selected from the group consisting of polyurethane , PVC, LDPE , LLDPE , HDPE , PP, PET , and synthetic and natural rubbers , but is not limited thereto .

The soft cushion sheet 110 is a plastic foam sheet and can provide the thickness uniformity of an adhesive and control the design quantity .

The density of the soft cushion sheet 110 is 0 . 025- 1 . 2 g/cm³, and preferably 0 . 025-0 . 6 g/cm³, but is not limited thereto .

The thickness of the soft cushion sheet 110 is preferably 0 . 5-30 mm, but is not limited thereto .

The soft cushion sheet 110 is formed with a density and a thickness within the above ranges , thereby maintaining a solid structure to implement excellent durability .

The perforated holes 111 are formed in the soft cushion sheet 110 for direct adhesion between the finishing mortar and the floor finishing material 130 .

The average diameter of the perforated holes 111 may be for example about 3 mm to about 30 mm, and preferably about 5 mm to about 20 mm, but is not limited thereto . The average diameter within the above range can improve adhesiveness between the finishing mortar and the floor finishing material by the filling of the adhesive composition . When the area of the perforated holes is A and the entire sheet area is B , A/B is preferably 1 /2 or greater . If A/B is less than 1 /2 , the contact area between the mortar surface and the flooring material is reduced to result in greatly weakened adhesive strength .

The distance (d) of the perforated holes 111 may be , for example , about 0 . 5 mm to about 10 mm. The distance (d) within the above range can improve the adhesiveness between the finishing mortar and the floor finishing material .

The distance ( d) between the perforated holes 111 means the shortest length among the lengths of straight lines connecting the perforated holes 121 , and for example , may indicate the shortest length among the lengths of straight lines connecting any point constituting the circumference of one perforated hole 121 and any point constituting the circumference of the other perforated hole 121 .

The distance ( d) between the perforated holes 111 may be formed equally within the above range , but is not limited thereto . The distance ( d) may be formed in various combinations within the above range according to the purpose and nature of the invention.

For example, 4,000 to 8,000 perforated holes 114 maybe formed per unit area of 1 m². The number of the perforated holes per unit area within the above range can exhibit high adhesive strength between the finishing mortar and the floor finishing material even though no adhesive layer is formed on the entire surface of the soft cushion sheet 110.

The soft cushion sheet 110 has a Shore A hardness of 5-70 degrees (ISO 868) , and the hardness of the soft cushion sheet is preferably lower than the hardness of the soft adhesive layer 120 in a cured state, but is not limited thereto.

The soft adhesive layer 120 may be a soft-state adhesive layer formed by moisture-curing of an adhesive composition containing a modified silane polymer at room temperature .

The adhesive composition containing the modified silane polymer may form a soft adhesive layer having properties of: a viscosity of 10,000-500,000 CPS before being cured, a Shore A hardness of 10-80 degrees (ISO 868) after being cured into a rubber phase, an adhesive tensile strength of 0.9 or more N/mm² (KS L 1593) , and an elongation of at least 100% (ASTM D 412) .

The adhesive composition may be a silyl-terminated polyether (STPE) -based composition containing a modified silane polymer, a crosslinker, a filler, and other additives .

According to an embodiment of the present invention, the modified silane polymer may be a compound represented by Chemical Formula 1 below.

Y-[ ( CR¹ ₂ ) b— SiR_a ( OR² ) 3-a ]_x (I) , where Y is an x-valent polymer radical bonded via nitrogen, oxygen, sulfur, or carbon, R may be identical or different and is a monovalent, optionally substituted, SiC-bonded hydrocarbon radical, R¹ may be identical or different and is hydrogen atom or a monovalent, optionally substituted hydrocarbon radical, which may be attached to the carbon atom by a nitrogen, phosphorus, oxygen, sulfur or carbonyl group, R² may be identical or different and is hydrogen atom or a monovalent, optionally substituted hydrocarbon radical, X is an integer from 1 to 10, preferably 1, 2, or 3, more preferably 1 or 2, a may be identical or different and is 0, 1, or 2, preferably 0 or 1, and b may be identical or different and is an integer from 1 to 10, preferably 1, 3, or 4, more preferably 1 or 3, more particularly 1.

Examples of radicals R are alkyl radicals, such as the methyl, ethyl, n-propyl, isopropyl, 1-n-butyl, 2-n- butyl, isobutyl, tert-butyl, n-pentyl, isopentyl, neopentyl, tert-pentyl radical; hexyl radicals, such as the n-hexyl radical; heptyl radicals, such as the n-heptyl radical; octyl radicals, such as the n-octyl radical, isooctyl radicals, and the 2 , 2 , 4-trimethylpentyl radical; nonyl radicals, such as the n-nonyl radical; decyl radicals, such as the n-decyl radical; dodecyl radicals, such as the n-dodecyl radical; octadecyl radicals, such as the n-octadecyl radical; cycloalkyl radicals, such as the cyclopentyl, cyclohexyl, cycloheptyl radical and methylcyclohexyl radicals; alkenyl radicals, such as the vinyl, 1-propenyl, and the 2-propenyl radical; aryl radicals, such as the phenyl, naphthyl, anthryl, and phenanthryl radical; alkaryl radicals, such as o- , m-, p- tolyl radicals, xylyl radicals and ethylphenyl radicals; and aralkyl radicals, such as the benzyl radical, the a- and the p-phenylethyl radical.

Examples of substituted radicals R are haloalkyl radicals , such as the 3 , 3 , 3-trif luoro-n-propyl radical , the 2 , 2 , 2 , 2 ' , 2 ^' , 2 ' -hexafluoroisopropyl radical , and the heptafluoroisopropyl radical , and haloaryl radicals , such as the o— , m- , and p-chlorophenyl radical .

Radical R preferably comprises monovalent hydrocarbon radicals which are optionally substituted by halogen atoms and which have 1 to 6 carbon atoms , more preferably alkyl radicals having 1 or 2 carbon atoms , more particularly the methyl radical .

Examples of radicals R¹ are hydrogen atom, the radicals specified for R, and also optionally substituted hydrocarbon radicals bonded to the carbon atom via nitrogen, phosphorus , oxygen, sulfur, carbon, or carbonyl groups .

Preferably R¹ is hydrogen atom and hydrocarbon radicals having 1 to 20 carbon atoms , more particularly hydrogen atom.

Examples of radical R² are hydrogen atom or the examples specified for radical R .

Radical R² is preferably hydrogen atom or alkyl radicals which are optionally substituted by halogen atoms and which have 1 to 10 carbon atoms , more preferably alkyl radicals having 1 to 4 carbon atoms , more particularly the methyl and ethyl radical .

Polymers on which the polymer radical Y is based are to be understood for the purposes of the present invention to be all polymers in which at least 50% , preferably at least 70% , more preferably at least 90% of all the bonds in the main chain are carbon-carbon, carbon-nitrogen, or carbon-oxygen bonds .

Polymer radical Y preferably comprises organic polymer radicals which as polymer chain comprise polyoxyalkylenes , such as polyoxyethylene , polyoxypropylene, polyoxybutylene , polyoxytetramethylene, polyoxyethylene-polyoxypropylene copolymer, and polyoxypropylene-polyoxybutylene copolymer; hydrocarbon polymers, such as polyisobutylene, polyethylene, or polypropylene, and copolymers of polyisobutylenes with isoprene; polyisoprenes; polyurethanes; polyesters, polyamides; polyacrylates; polymetacrylates ; and polycarbonates, and which are bonded preferably via -0- C(=O)-NH-, -NH-C (=0)0-, -NH-C (=0) -NH-, -NR' -C (=0) -NH- , NH-C (=0) -NR' -, -NH-C(=0)-, -C(=O)-NH-, -C (=0) -0- , -0- C(=0)-, -0-C(=0)-0-, -S-C (=0) -NH-, -NH-C (=0) -S-, -C (=0) - S-, -S-C(=O)-, -S-C(=O)-S-, -C(=0)-, -S-, -0-, and -NR' - to the group or groups - [ (CR¹ ₂ )_b-SiR_a (OR²) _3-a] , where R' may be identical or different and has a definition given for R, or is a group -CH (COOR") -CH₂-COOR", in which R" may be identical or different and has a definition specified for R.

Examples of radicals R' are cyclohexyl, cyclopentyl, n-propyl and isopropyl, n-butyl, isobutyl, and tert-butyl, the various sterioisomers of the pentyl radical, hexyl radical, or heptyl radical, and also the phenyl radical.

Radical R' is preferably a group -CH (COOR" ) -CH₂- COOR' ' or an optionally substituted hydrocarbon radical having 1 to 20 carbon atoms, more preferably a linear, branched or cycloalkyl group having 1 to 20 carbon atoms, or an aryl group which has 6 to 20 carbon atoms and is optionally substituted by halogen atoms.

The radicals R' ' are preferably alkyl groups having 1 to 10 carbon atoms, more preferably methyl, ethyl, or propyl radicals.

More preferably radical Y in formula (I) comprises polyurethane radicals and polyoxyalkylene radicals, more particularly polyoxypropylene-containing polyurethane radicals or polyoxypropylene radicals.

The modified silane polymer here may have the groups - [ (CR¹ ₂ )_b-SiR_a (OR²) _3-a] , attached in the manner described, at any desired locations within the polymer, such as, for instance, within the chain and/or terminally, preferably within the chain and terminally, more preferably terminally .

The end groups of the modified silane polymer used in accordance with the invention are preferably groups of the general formulae

-0-C (=0) -NH- (CR¹ ₂)_b ^_SiR_a (OR²) _3-a (III) and

-NH-C (=0) -NR' - (CR¹ ₂)_b-SiR_a (OR²) _3-a (IV) , where the radicals and indices have one of the definitions specified above for them.

In one particularly preferred embodiment of the invention, the modified silane polymer comprises silane- terminated polyethers and silane-terminated polyurethanes, more particularly silane-terminated polypropylene glycols and silane-terminated polyurethanes, in each case with dimethoxymethylsilyl, trimethoxysilyl, diethoxymethylsilyl, or triethoxysilyl end groups that are attached via -O-C (=O) -NH- (CR¹ ₂)_b groups or -NH-C (=0) -NR' - (CR¹ ₂)_b groups, where R' , R¹ and b have one of the definitions specified above.

The average molecular weights M_n of the modified silane polymer is preferably at least 400 g/mol, more preferably a-t least 600 g/mol, more particularly at least 800 g/mol, and preferably not more than 30000 g/mol, more preferably not more than 19,000 g/mol, more particularly not more than 13,000 g/mol.

The viscosity of the modified silane polymer is preferably at least 0.2 Pas, more preferably at least 1 Pas, very preferably at least 5 Pas, and preferably not more than 1000 Pas, more preferably not more than 700 Pas, in each case measured at 20°C.

The modified silane polymer used in accordance with the invention are commercial products or can be prepared by methods that are commonplace within chemistry. The modified silane polymer may be prepared by various, known processes, such as addition reactions, as for example the hydrosilylation, Michael addition, Diels- Alder addition, or reactions between isocyanate- functional compounds with compounds containing isocyanate-reactive groups.

In the case of a first, particularly preferred embodiment of the invention, modified silane polymer comprises, as polymer radicals Y, linear or branched polyoxyalkylene radicals, more preferably polyoxypropylene radicals, whose chain ends are bonded preferably via -O-C(=O)-NH- to the group or groups - [ (CR¹ ₂)_b-SiR_a (OR²) _3-a] , the radicals and indices having one of the definitions stated above. Here, preferably at least 85%, more preferably at least 90%, more particularly at least 95%, of all the chain ends are bonded via -O-C(=O)-NH- to the group - [ (CR¹ ₂)_b-SiR_a (OR² ) _3- _a] . The polyoxyalkylene radicals Y preferably have average molar masses M_n of 4,000 to 30,000 daltons, preferably of 8,000 to 20,000 daltons. Suitable processes for preparing such a modified silane polymer, and also examples of modified silane polymer itself, are also known and are described in publications including EP 1535940 B1 (paragraphs [0005] - [0025] and also inventive examples 1-3 and comparative example 1-4) or EP 1896523 Bl (paragraphs [ 0008 ]-[ 0047 ] ) , which are included in the disclosure content of the present specification. Corresponding silane-terminated polymers are also available commercially, under the name GENIOSIL® STP-E from Wacker Chemie, for example.

In a second, likewise particularly preferred embodiment of the invention, modified silane polymer comprises, as polymer radical Y, linear or branched polyurethane radicals prepared starting preferably from polyether polyols and/or polyester polyols Y1 having an average molar mass of 200 to 20,000 daltons. The polyols used here are more preferably polyether polyols, more particularly polyproyplene glycols, having an average molar mass of 300 to 10,000 daltons, more particularly of 400 to 5,000 daltons. The polyols Y1 may be branched or unbranched. Particularly preferred are unbranched polyols or else polyols having one branching site. Mixtures of branched and unbranched polyols as well may be used.

The modified silane polymer used in accordance with the invention may comprise only one kind of compound of the formula (I) and also mixtures of different kinds of compounds of the formula (I) . In this case the modified silane polymer may comprise exclusively compounds of the formula (I) in which more than 90%, preferably more than 95%, more preferably more than 98% of all of the silyl groups bonded to the polymer radical Y are identical. In that case, however, it is also possible to use a modified silane polymer which comprises, at least in part, compounds of the formula (I) in which different silyl groups are bonded to a polymer radical Y. Lastly, it is also possible as modified silane polymer to use mixtures of different compounds of the formula (I) in which a total of at least 2 different kinds of silyl groups are present, but with all silyl groups bonded to a respective polymer radical Y being identical.

The compositions of the invention preferably comprise modified silane polymer in concentrations of not more than 40 wt%, more preferably not more than 30 wt%, and preferably at least 10 wt%, more preferably at least 15 wt%.

According to an embodiment of the present invention, the adhesive composition may further contain phenyl silicone resin.

The phenyl silicone resin may contain a unit of Chemical Formula II.

R³C (R⁴O) _dR⁵ _eSiO _{(4-c-d-e) /2} ( II) , where R³ may be identical or different and is hydrogen atom, a monovalent, SiC-bonded, optionally substituted aliphatic hydrocarbon radical, or a divalent, optionally substituted, aliphatic hydrocarbon radical which bridges two units of the formula (II) , R⁴ may be identical or different and is hydrogen atom or a monovalent, optionally substituted hydrocarbon radical, R⁵ may be identical or different and is a monovalent, SiC- bonded, optionally substituted aromatic hydrocarbon radical, c is 0, 1, 2, or 3, d is 0, 1, 2, or 3, preferably 0, 1, or 2, more preferably 0 or 1, and e is 0, 1, or 2, preferably 0 or 1, with the proviso that the sum of c+d+e is less than or equal to 3 and in at least 40% of the units of the formula (II) the sum c+e is 0 or 1.

Phenyl silicone resin consists preferably to an extent of at least 90 wt% of units of the formula (II) . With particular preference phenyl silicone resin consists exclusively of units of the formula (II) .

Examples of radicals R³ are the aliphatic examples specified above for R. However, radical R³ may also comprise divalent aliphatic radicals which join two silyl groups of the formula (II) to one another, such as, for example, alkylene radicals having 1 to 10 carbon atoms, such as methylene, ethylene, propylene, or butylene radicals, for instance. One particularly current example of a divalent aliphatic radical is the ethylene radical.

Preferably, however, radical R³ comprises monovalent, SiC-bonded aliphatic hydrocarbon atoms which are optionally substituted by halogen atoms and that have 1 to 18 carbon atoms, more preferably aliphatic hydrocarbon radicals having 1 to 6 carbon atoms, more particularly the methyl radical.

Examples of radical R⁴ are hydrogen atom or the examples specified for radical R.

Radical R⁴ comprises hydrogen atom or alkyl radicals that are optionally substituted by halogen atoms and that have 1 to 10 carbon atoms, more preferably alkyl radicals having 1 to 4 carbon atoms, more particularly the methyl and ethyl radical.

Examples of radicals R⁵ are the aromatic radicals specified above for R.

Radical R⁵ preferably comprises SiC-bonded aromatic hydrocarbon radicals that are optionally substituted by halogen atoms and that have 1 to 18 carbon atoms, such as, for example, ethylphenyl, tolyl, xylyl, chlorophenyl, naphthyl, or styryl radicals, more preferably the phenyl radical .

Preferred for use as phenyl silicone resins are silicone resins in which at least 90% of all radicals R³ are methyl radical, at least 90% of all radicals R⁴ are methyl, ethyl, propyl, or isopropyl radical, and at least 90% of all radicals R⁵ are phenyl radicals.

Preference is given in accordance with the invention to using silicone resins (B) which have at least 20%, more preferably at least 40%, of units of the formula (II) in which c is 0, based in each case on the total number of units of the formula (II) .

One embodiment of the invention uses phenyl silicone resins which, based in each case on the total number of units of the formula (II) , have at least 10%, more preferably at least 20%, and not more than 80%, more preferably not more than 60%, of units of the formula (II) in which c stands for the value 2.

Phenyl silicone resins used with preference are those which, based in each case on the total number of units of the formula (II) , have at least 80%, more preferably at least 95%, of units of the formula (II) in which d stands for the value 0 or 1. Preference is given to using phenyl silicone resins which, based in each case on the total number of units of the formula (II) , have at least 60%, more preferably at least 70%, preferably not more than 99%, more preferably not more than 97%, of units of the formula (II) in which d stands for the value 0.

Employed with more preference as phenyl silicone resins are silicone resins which, based in each case on the total number of units of the formula (II) , have at least 1%, preferably at least 10%, more particularly at least 20% of units of the formula (II) in which e stands for a value other than 0. Phenyl silicone resins can be used which exclusively have units of the formula (II) in which e is other than 0, but more preferably at least 10%, very preferably at least 20%, and preferably not more than 80%, more preferably not more than 60%, of the units of the formula (II) have an e of 0.

Preference is given to using phenyl silicone resins which, based in each case on the total number of units of the formula (II) , have at least 20%, more preferably at least 40%, of units of the formula (II) in which e stands for the value 1. Phenyl silicone resins may be used which exclusively have units of the formula (II) in which e is 1, but more preferably at least 10%, very preferably at least 20%, and preferably not more than 80%, more preferably not more than 60%, of the units of the formula (II) have an e of 0.

Preferably used are phenyl silicone resins which, based in each case on the total number of units of the formula (II) , have at least 50% of units of the formula (II) in which the sum c+e is 0 or 1.

In one particularly preferably embodiment of the invention, phenyl silicone resins are used as component (B) which, based in each case on the total number of units of the formula (II) , have at least 20%, more preferably at least 40%, of units of the formula (II) in which e stands for the value 1 and c stands for the value 0. In this case preferably not more than 70%, more preferably not more than 40%, of all units of the formula (II) have a d other than 0.

In another particularly preferably embodiment of the invention, phenyl silicone resins are resins which, based in each case on the total number of units of formula (II) , have at least 20%, more preferably at least 40%, of units of the formula (II) in which e stands for the value 1 and c stands for the value 0 and which, moreover, have at least 1%, preferably at least 10%, of units of the formula (II) in which c stands for 1 or 2, preferably 2 and e for 0. In this case preferably not more than 70%, more preferably not more than 40%, of all units of the formula (II) have a d other than 0 and at least 1% of all units of the formula (II) have a d of 0.

Examples of the phenyl silicone resins used in accordance with the invention are organopolysiloxane resins which consist substantially, preferably exclusively, of (Q) units of the formulae SiO_4/2, Si(OR⁴)O_3/2, Si(OR⁴)₂O_2/2 and Si (OR⁴) ₃O_1/2, (T) units of the formulae PhSiO_3/2, PhSi (OR⁴) O_2/2 and PhSi (OR⁴) ₂O_1/2, (D) units of the formulae Me₂SiO_2/2 and Me₂Si (OR⁴) O1/2, and also (M) units of the formula Me₃SiO_1/2, where Me is a methyl radical, Ph is a phenyl radical, and R⁴ is hydrogen atom or alkyl radicals that are optionally substituted by halogen atoms and that have 1 to 10 carbon atoms, more preferably hydrogen atom or alkyl radicals having 1 to 4 carbon atoms, with the resin containing preferably 0-2 mol of (Q) units, 0-2 mol of (D) units, and 0-2 mol of (M) units per mol of (T) units.

Preferred examples of the phenyl silicone resins used in accordance with the invention are organopolysiloxane resins which consist substantially, preferably exclusively, of T units of the formulae PhSiO3/2, PhSi (OR⁴) O_2/2, and PhSi (OR⁴) ₂O_1/2 and also D units of the formulae Me₂SiO_2/2, and Me₂Si (OR⁴) O_1/2, where Me is a methyl radical, Ph is a phenyl radical, and R⁴ is hydrogen atom or alkyl radicals that are optionally substituted by halogen atoms and that have 1 to 10 carbon atoms, more preferably hydrogen atom or alkyl radicals having 1 to 4 carbon atoms, with a molar ratio of (T) to (D) units of 0.5 to 2.0.

Further preferred examples of the phenyl silicone resins used in accordance with the invention are organopolysiloxane resins which consist substantially, preferably exclusively, of T units of the formulae PhSiO_3/2, PhSi (OR⁴ )O_2/2 , and PhSi (OR⁴) ₂O_1/2, and also T units of the formulae MeSiO_3/2, MeSi (OR⁴) O_2/2, and MeSi (OR⁴) ₂O_1/2, and also, optionally, D units of the formulae Me₂SiO_2/2 and Me₂Si (OR⁴) O_1/2, where Me is a methyl radical, Ph is a phenyl radical, and R⁴ is hydrogen atom or alkyl radicals that are optionally substituted by halogen atoms and that have 1 to 10 carbon atoms, more preferably hydrogen atom or alkyl radicals having 1 to 4 carbon atoms, with a molar ratio of phenylsilicone to methylsilicone units of 0.5 to 4.0. The amount of D units in these silicone resins is preferably below 10 wt% .

Additionally preferred examples of the phenyl silicone resins used in accordance with the invention are organopolysiloxane resins which consist substantially, preferably exclusively, of T units of the formulae PhSiO_3/2, PhSi (OR⁴ ) O_2/2, and PhSi (OR⁴) ₂O_1/2, where Ph is a phenyl radical and R⁴ is hydrogen atom or alkyl radicals that are optionally substituted by halogen atoms and that have 1 to 10 carbon atoms, more preferably hydrogen atom or alkyl radicals having 1 to 4 carbon atoms. The amount of D units in these silicone resins is preferably below 10 wt%. The phenyl silicone resins used in accordance with the invention preferably possess an average molar mass (number average) M_n of at least 400 g/mol and more preferably of at least 600 g/mol. The average molar mass M_n is preferably not more than 400,000 g/mol, more preferably not more than 100,000 g/mol, more particularly not more than 50,000 g/mol.

The phenyl silicone resins used in accordance with the invention may be either solid or liquid at 23 °C and 1,000 hPa, with phenyl silicone resins preferably being liquid. The phenyl silicone resins preferably possess a viscosity of 10 to 100,000 mPas, preferably of 50 to 50,000 mPas, more particularly of 100 to 20,000 mPas. The phenyl silicone resins preferably possess a polydispersity (M_w/M_n) of not more than 5, more preferably of not more than 3.

The phenyl silicone resins may be used either in pure form or in the form of a solution in a suitable solvent .

Solvents that may be used in this case include substances such as ethers (e.g., diethyl ether, methyl tert-butyl ether, ether derivatives of glycol, THF) , esters (e.g., ethyl acetate, butyl acetate, glycol esters) , hydrocarbons (e.g., pentane, cyclopentane, hexane, cyclohexane, heptane, octane, or else longer- chain, branched and unbranched alkanes) , ketones (e.g., acetone, methyl ethyl ketone) , aromatics (e.g., toluene, xylene, ethylbenzene, chlorobenzene) , or else alcohols (e.g., methanol, ethanol, glycol, propanol, isopropanol, glycerol, butanol, isobutanol, tert-butanol) .

Preference, however, is given to using phenyl silicone resins which are free from organic solvents.

According to an embodiment of the present invention, the crosslinker may be aminosilanes.

Preferably, the amino silanes may be organosilicon compounds containing a unit of Chemical Formula V below.

D_hSi (OR⁷) _gR⁸ _fO_(4-f-g-h)/2 (V) , where R⁷ may be identical or different and denotes hydrogen atom or optionally substituted hydrocarbon radicals, D may be identical or different and denotes a monovalent, SiC-bonded radical containing basic nitrogen, R⁸ may be identical or different and denotes a monovalent, optionally substituted, SiC-bonded organic radical free from basic nitrogen, f is 0, 1, 2, or 3, preferably 1 or 0, g is 0, 1, 2, or 3, preferably 1, 2, or 3, more preferably 2 or 3, and h is 0, 1, 2, 3, or 4, preferably 1, with the proviso that the sum of f+g+h is less than or equal to 4 and there is at least one radical D present per molecule .

In one preferred embodiment of the invention, the compositions of the invention, further to modified silane polymer and phenyl silicone resin, also comprise at least one further aminosilane corresponding to the formula (IX) , especially when modified silane polymer comprises silane- terminated urethanes having end groups of the formula (IV) . It was a surprise that when using modified silane polymer and Phenyl silicone resin which are mutually insoluble or sparingly soluble in the proportions preferred in accordance with the invention, it is possible, by adding aminosilane, to obtain mixtures that are largely homogeneous and preferably wholly homogeneous.

In contrast, those mixtures according to the invention that additionally comprise aminosilanes in the preferred quantities specified below usually, and advantageously, form a homogeneous solution.

The aminosilanes used optionally in accordance with the invention may be not only silanes, i.e., compounds of the formula (V) with f+g+h=4, but also siloxanes, i.e., compounds comprising units of the formula (IX) with f+g+h ≤ 3, with preference being given to silanes.

Examples of optionally substituted hydrocarbon radicals R⁷ are the examples specified for radical R.

The radicals R⁷ are preferably hydrogen atom and hydrocarbon radicals that are optionally substituted by halogen atoms and that have 1 to 18 carbon atoms; more preferably, hydrogen atom and hydrocarbon radicals that have 1 to 10 carbon atoms; more particularly, methyl radical and ethyl radical.

Examples of R⁸ are the examples specified for radical R. Radical R⁸ preferably comprises hydrocarbon radicals that are optionally substituted by halogen atoms and that have 1 to 18 carbon atoms, more preferably hydrocarbon radicals having 1 to 5 carbon atoms, more particularly the methyl radical.

Examples of radicals D are radicals of the formulae H₂N(CH₂)₃-, H₂N (CH₂) ₂NH (CH₂) ₃-, H₂N (CH₂) ₂NH (CH₂) ₂NH (CH₂) ₃-, H₃CNH(CH₂)₃-, C₂H₅NH(CH₂) ₃-, C₃H₇NH (CH₂) ₃-, C₄H₉NH (CH₂) ₃-,

C₅H₁₁NH (CH₂) ₃-, C₆H₁₃NH(CH₂)3-, C₇H₁₅NH (CH₂) ₃-, H₂N(CH₂)₄-, H₂N-

CH₂-CH ( CH3 ) -CH₂- , H₂N(CH₂)₅-, cyclo-C₅H₉NH ( CH₂ ) 3- , cyclo-

C₆H₁₁NH (CH₂) ₃-, phenyl-NH (CH₂) ₃-, (CH₃) ₂N (CH₂) ₃-, (C₂H₅) ₂N (CH₂) ₃-, (C₃H₇) ₂NH (CH₂) ₃-, (C4H9) ₂NH (CH₂) ₃-, ( C₅H₁₁ ) ₂NH ( CH₂ ) 3- , (C₆H₁₃) ₂NH (CH₂) ₃-, (C7H15) ₂NH (CH₂) ₃-,

H₂N(CH₂)-, H₂N (CH₂) ₂NH (CH₂) H₂N (CH₂) ₂NH (CH₂) ₂NH (CH₂)

H3CNH (CH₂) C₂H₅NH(CH₂) C₃H₇NH(CH₂)- C₄H₉NH (CH₂) C5H11NH (CH₂) C₆H₁₃NH (CH₂) C7H15NH (CH₂) - cyclo- C₅H₉NH(CH₂) cyclo-C₆H₁₁NH (CH₂) phenyl-NH (CH₂) - , (CH₃)₂N (CH₂) -, (C₂H₅) ₂N (CH₂) (C₃H₇)₂NH(CH₂)-, (C₄H₉) ₂NH (CH₂) (C₅H₁₁) ₂NH (CH₂) (C₆H₁₃) ₂NH (CH₂) -, (C7H₁₅)₂NH(CH₂)- (CH₃O)₃Si (CH₂)₃NH(CH₂)₃-,

(C₂H₅O) ₃Si (CH₂) ₃NH (CH₂) ₃-, (CH₃O) ₂ (CH₃) Si (CH₂) ₃NH (CH₂) ₃-, and (C₂H₅O) ₂ (CH₃) Si (CH₂) ₃NH (CH₂) ₃-, and also reaction products of the abovementioned primary amino groups with compounds containing epoxide groups or double bonds that are reactive toward primary amino groups. Radical D preferably comprises the H₂N(CH₂)₃-,

H₂N(CH₂)₂NH(CH₂)₃-, and cyclo-CeH₁₁NH (CH₂) ₃- radical .

Examples of the silanes of the formula (IX) that are used optionally in accordance with the invention are H₂N(CH₂)₃- Si(OCH₃)₃, H₂N(CH₂)₃-Si(OC₂H₅)₃, H₂N (CH₂) ₃-Si (OCH₃) ₂CH₃, H₂N (CH₂) ₃-Si (OC₂H₅) ₂CH₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OCH₃) ₃,

H₂N (CH₂) ₂NH (CH₂) ₃-Si (OC₂H₅)₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OCH₃)₂CH₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OC2H5) ₂CH₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OH) ₃, H₂N ( CH₂ ) ₂NH ( CH₂ ) ₃-Si ( OH ) ,₂CH₃ , H₂N ( CH₂ ) ₂NH ( CH₂ ) ₂NH ( CH₂ ) ₃-

Si(OCH₃)₃, H₂N (CH₂) ₂NH (CH₂) 2NH (CH₂) ₃-Si (OC₂H₅) ₃, cyclo- C₆H₁₁NH (CH₂) ₃-Si (OCH₃) ₃, cyclo-CeH₁₁NH (CH₂) ₃-Si (OC₂H₅) ₃, cyclo-C₆H₁₁NH (CH₂) ₃-Si (OCH₃) ₂CH₃, cyclo-C₆H₁₁NH (CH₂) ₃-

Si (OC₂H₅) 2CH₃, cyclo-C₆H₁₁NH (CH₂) ₃-Si (OH) ₃, cyclo- C₆H₁₁NH (CH₂) ₃-Si (OH) ₂CH₃, phenyl-NH (CH₂) ₃-Si (OCH₃) ₃, phenyl- NH (CH₂) ₃-Si (OC₂H₅) ₃, phenyl-NH (CH₂) ₃-Si (OCH₃) ₂CH₃, phenyl- NH (CH₂) ₃-Si (OC₂H₅) ₂CH₃, phenyl-NH (CH₂) ₃-Si (OH) ₃, phenyl- NH (CH₂) ₃-Si (OH) ₂CH₃, HN ( (CH₂) ₃-Si (OCH₃) ₃)₂, HN( (CH₂)₃- Si (OC₂H₅) ₃)₂ HN ( (CH₂) ₃-Si (OCH₃) ₂CH₃) ₂, HN( (CH₂)₃-

Si (OC₂H₅) ₂CH₃) ₂, cyclo-C₆H₁₁NH (CH₂) -Si (OCH₃) ₃, cyclo- C₆H₁₁NH (CH₂) -Si (OC₂H₅) ₃, cyclo-C₆H₁₁NH (CH₂) -Si (OCH₃) ₂CH₃, cyclo-C₆H₁₁NH (CH₂) -Si (OC₂H₅) ₂CH₃, cyclo-C₆H₁₁NH (CH₂) -Si (OH) ₃, cyclo-C₆H₁₁NH (CH₂) -Si (OH) ₂CH₃, phenyl-NH (CH₂) -Si (OCH₃) ₃, phenyl-NH (CH₂) -Si (OC₂H₅) ₃, phenyl-NH (CH₂) -Si (OCH₃) ₂CH₃, phenyl-NH (CH₂) -Si (OC₂H₅) ₂CH₃, phenyl-NH (CH₂) -Si (OH) ₃, and phenyl-NH (CH₂) -Si (OH) ₂CH₃, and also their partial hydrolyzates, with preference being given to H₂N (CH₂) ₂NH (CH₂) ₃-Si (OCH₃) ₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OC₂H₅) ₃, H₂N (CH₂) ₂NH (CH₂) ₃-Si (OCH₃) ₂CH₃, cyclo-C₆H₁₁NH (CH₂) ₃- Si (OCH₃)₃, cyclo-C₆H₁₁NH (CH₂) ₃-Si (OC₂H₅) ₃, and cyclo-

C₆H₁₁NH (CH₂) ₃-Si (OCH₃) ₂CH₃, and also, in each case, their partial hydrolyzates, and particular preference being given to H₂N (CH₂) ₂NH (CH₂) ₃-Si (OCH₃) ₃, H₂N (CH₂) ₂NH (CH₂) ₃- Si (OCH₃)₂CH₃, cyclo-C₆H₁₁NH(CH₂) ₃-Si (OCH₃) ₃, cyclo-

C₆H₁₁NH (CH₂) ₃-Si (OCH₃) ₂CH₃, and also, in each ccaassee,, their partial hydrolyzates .

In the compositions of the invention, the aminosilanes used optionally in accordance with the invention may also take on the function of a curing catalyst or curing cocatalyst .

Furthermore , the aminosilanes used optionally in accordance with the invention may act as adhesion promoters and/or as water scavengers . The aminosilanes used optionally in accordance with the invention are commercial products and/or can be prepared by methods that are commonplace within chemistry . If the compositions of the invention do comprise aminosilanes , the amounts in question are preferably 0 . 1 to 25 parts by weight , more preferably 0 . 5 to 10 parts by weight , in each case based on 100 parts by weight of modified silane polymer . The compositions of the invention do preferably comprise aminosilanes .

The fillers employed in the compositions of the invention may be any desired fillers known to date . Examples of fillers are nonreinforcing fillers , these being fillers having a BET surface area of preferably up to 50 m²/g, such as quartz , diatomerous earth, calcium silicate , zirconium silicate , talc, kaolin, zeolites , metal oxide powders , such as aluminum oxides , titanium oxides , iron oxides , or zinc oxides , and/or their mixed oxides , barium sulfate , calcium carbonate , gypsum, silicon nitride , silicon carbide , boron nitride , glass powders and polymeric powders , such as polyacrylonitrile powders ; reinforcing fillers , these being fillers having a BET surface area of more than 50 m²/g, such as pyrogenically prepared silica , precipitated silica, precipitated chalk, carbon black, such as furnace black and acetylene black, and mixed silicon/aluminum oxides of high BET surface area ; aluminum trihydroxide , fillers in the form of hollow beads , such as ceramic microbeads , examples being those obtainable under the trade name Zeeospheres™ from 3M Deutschland GmbH of Neuss , Germany, elastic polymeric beads , of the kind, for instance , obtainable under the trade name EXPANCEL® from AKZO NOBEL , Expancel , of Sundsvall , Sweden, or glass beads ; fillers in fiber form, such as asbestos and also polymeric fibers . The stated fillers may have been hydrophobized, by treatment for example with organosilanes and/or organosiloxanes or with stearic acid, or by etherification of hydroxyl groups to alkoxy groups .

The fillers optionally employed are preferably calcium carbonate , talc , aluminum trihydroxide , and silica , particular preference being given to aluminum trihydroxide . Preferred calcium carbonate grades are ground or precipitated and have optionally been surface- treated with fatty acids such as stearic acid or salts thereof . The preferred silica is preferably pyrogenic ( fumed) silica .

Fillers optionally employed have a moisture content of preferably below 1 wt% , more preferably below 0 . 5 wt% . I f the compositions of the invention do comprise fillers , the amounts in question are preferably 10 to 1 , 000 parts by weight , more preferably 50 to 500 parts by weight , more particularly 80 to 300 parts by weight , based in each case on 100 parts by weight of modified silane polymer . The compositions of the invention do preferably comprise fillers .

In one particular embodiment of the invention, the compositions of the invention comprise as fillers a combination of a ) silica , more particularly fumed silica , and b ) calcium carbonate , aluminum trihydroxide and/or talc .

If the compositions of the invention do comprise this particular combination of different fillers, they comprise preferably 1 to 80 parts by weight, more preferably 5 to 40 parts by weight, of silica, more particularly fumed silica, and preferably 10 to 500 parts by weight, more preferably 50 to 300 parts by weight, of calcium carbonate, aluminum trihydroxide, talc, or mixtures of these materials, based in each case on 100 parts by weight of modified silane polymer.

The adhesive composition may further contain a catalyst depending on the type of silane polymer.

The catalysts used optionally in the compositions of the invention may be any desired catalyst known to date for compositions that cure by silane condensation. Examples of metal-containing curing catalysts are organotitanium and organotin compounds, examples being titanic esters, such as tetrabutyl titanate, tetrapropyl titanate, tetraisopropyl titanate, and titanium tetraacetylacetonate; tin compounds, such as dibutyltin dilaurate, dibutyltin maleate, dibutyltin diacetate, dibutyltin dioctanoate, dibutyltin acetylacetonate, dibutyltin oxides, and corresponding dioctyltin compounds. Examples of metal-free curing catalysts are basic compounds, such as triethylamine, tributylamine, 1, 4 -diazabi cyclo [2.2.2] octane, 1,5- diazabicyclo [4.3.0] non-5-ene, 1, 8- diazabicyclo [5.4.0] undec-7-ene, N,N-bis- (N, N-dimethyl-2- aminoethyl) methylamine, N, N-dimethylcyclohexylamine, N,N- dimethylphenylamine, and N-ethylmorpholinine .

As catalyst, it is likewise possible to use acidic compounds, such as phosphoric acid and its esters, toluenesulfonic acid, sulfuric acid, nitric acid, or else organic carboxylic acids, e.g., acetic acid and benzoic acid. If the compositions of the invention do comprise catalysts , the amounts involved are preferably 0 . 01 to 20 parts by weight , more preferably 0 . 05 to 5 parts by weight , based in each case on 100 parts by weight of modified silane polymer .

In one embodiment of the invention the catalysts optionally employed are metal-containing curing catalysts , preferably tin-containing catalysts . This embodiment of the invention is especially preferred when modified silane polymer consists wholly or at least partly, in other words to an extent of at least 90 wt% , preferably at least 95 wt% , of compounds of the formula ( I ) in which b is other than 1 .

In the compositions of the invention it is pos sible with preference to do without metal-containing catalysts , and more particularly without catalysts containing tin, when modified silane polymer consists wholly or at least partly, in other words to an extent of at least 10 wt% , preferably at least 20 wt% , of compounds of the formula ( I ) in which b is 1 and R¹ has the definition of hydrogen atom. This embodiment of the invention, without metalcontaining and more particularly without tin-containing catalysts , is particularly preferred .

The adhesive composition may contain other additives . Examples of the other additives may include adhesion promoters , water scavengers , plasticizer, antioxidants , UV stabilizers , fungicides , pigments , adj uvants , and the like , but are not limited thereto .

The adhesion promoters employed optionally in the compositions of the invention may be any desired adhesion promoters that have been described hitherto for systems that cure by silane condensation .

Examples of adhesion promoters are epoxy silanes , such as glycidyloxypropyltrimethoxysilanes , glycidyl oxypropyl -methyldimethoxy si lane , glycidyloxypropyltriethoxysilane , or glycidyloxypropyl- metyhldiethoxysilane , 2- ( 3-triethoxysilylproypl ) maleic anhydride , N- ( 3-trimethoxysilylpropyl ) urea, N- ( 3- triethoxysilylpropyl ) urea, N- ( trimethoxysilylmethyl ) urea, N- (methyldimethoxysilymethyl ) urea , N- ( 3- triethoxysilylmethyl ) urea, N- ( 3- methyldiethoxysilylmethyl ) urea, O-methylcarbamatomethyl- methyldimethoxysilane , O-methylcarbamatomethyl- trimethoxy silane , O-ethylcarbamatomethyl- methyldiethoxysilane , O-ethylcarbamatomethyl- triethoxy silane , 3 -methacryloyloxypropyl- trimethoxy silane , methacryloyloxymethyl-trimethoxysilane , methacryloyl oxymethyl -methyldimethoxy si lane , methacryloyloxymethyl- triethoxy silane , methacryloyloxymethyl-methyldiethoxysilane , 3- acryloyl oxypropyltrimethoxysilane , acryloyloxymethyl- trimethoxysilane , acryloyl oxymethyl - methyldimethoxysilanes , acryloyloxymethyltriethoxysilane , and acryloyloxymethylmethyldiethoxysilane , and also their partial condensates .

If the compositions of the invention do comprise adhesion promoters , the amounts involved are preferably 0 . 5 to 30 parts by weight , more preferably 1 to 10 parts by weight , based in each case on 100 parts by weight of crosslinkable composition .

The water scavengers employed optionally in the compositions of the invention, may be any desired water scavengers described for systems that cure by silane condensation .

Examples of water scavengers are silanes such as vinyltrimethoxysilane , vinyltriethoxysilane , vinylmethyl- dimethoxysilane , O-methylcarbamatomethyl- methyldimethoxysilane, O-methylcarbamatomethyl- trimethoxy silane , O-ethylcarbamatomethyl- methyldi ethoxy si lane , 0- ethyl carbam tome thy 1- triethoxysilane, and/or their partial condensates, and also orthoesters, such as 1, 1, 1-trimethoxyethane, 1,1,1- triethoxyethane , trimethoxymethane, and triethoxymethane.

If the compositions of the invention do comprise water scavengers, the amounts involved are preferably 0.5 to 30 parts by weight, more preferably 1 to 10 parts by weight, based in each case on 100 parts by weight of crosslinkable composition. The compositions of the invention preferably do comprise water scavengers.

The additives employed optionally in the compositions of the invention may be any desired additives known to date and typical for silane-crosslinking systems.

The additives employed optionally in accordance with the invention are preferably antioxidants, UV stabilizers, such as HALS compounds, for example, fungicides, and pigments .

If the compositions of the invention do comprise additives, the amounts involved are preferably 0.01 to 30 parts by weight, more preferably 0.1 to 10 parts by weight, based in each case on 100 parts by weight of constituent (A) . The compositions of the invention do preferably comprise additives.

The adjuvants employed optionally in accordance with the invention are preferably tetraalkoxysilanes, as for example tetraethoxysilane and/or partial condensates thereof, plasticizers, including reactive plasticizers, rheological additives, flame retardants, and organic solvents .

Examples of plasticizers are such as phthalic esters (e.g. , dioctyl phthalate, diisooctyl phthalate, and diundecyl phthalate) , perhydrogenated phthalic esters (e.g. , 1 , 2-cyclohexanedicarboxylic diisononyl esters and 1 , 2-cyclohexanedicarboxylic dioctyl esters) adipic esters (e.g., dioctyl adipate) , benzoic esters, glycol esters, esters of saturated alkanediols (e.g., 2 , 2 , 4-trimethyl- 1, 3-pentanediol monoisobutyrates and 2, 2, 4-trimethyl-l, 3- pentanediol diisobutyrates) , phosphoric esters, sulfonic esters, polyesters, polyethers (e.g., polyethylene glycols and polypropylene glycols with molar masses of preferably 1000 to 10 000 daltons) , polystyrenes, polybutadienes, polyisobutylenes, paraffinic hydrocarbons, and branched hydrocarbons of high molecular mass, with preferably no plasticizers being used.

Examples of reactive plasticizers are those of the formula

R¹⁰ _mSi (OR⁹ ) ₁R¹¹ _kO _{(4-k-1-m) /2} (VI) , in which R⁹ may be identical or different and denotes hydrogen atom or optionally substituted hydrocarbon radicals, R¹⁰ may be identical or different and denotes a monovalent, optionally substituted, SiC-bonded hydrocarbon radical having 3 to 40 carbon atoms, R¹¹ may be identical or different and denotes a monovalent, optionally substituted, SiC-bonded hydrocarbon radical having 1 or 2 carbon atoms, k is 0, 1, 2, or 3, preferably 0 or 1, 1 is 0, 1, 2, or 3, preferably 2 or 3, more preferably 3, and m is 0, 1, 2, 3, or 4, preferably 1, with the proviso that the sum of k+l+m is less than or equal to 4 and there is at least one radical R¹⁰ present per molecule.

Examples of optionally substituted hydrocarbon radicals R⁹ are the examples specified for radical R.

The radicals R⁹ are preferably hydrogen atom and hydrocarbon radicals that are optionally substituted by halogen atoms and that have 1 to 18 carbon atoms; more preferably hydrogen atom and hydrocarbon radicals having 1 to 10 carbon atoms; more particularly, methyl radical and ethyl radical.

Examples of optionally substituted hydrocarbon radicals R¹⁰ are the examples specified for radical R of hydrocarbon radicals having at least 3 carbon atoms .

Radical R¹⁰ preferably has an even number of carbon atoms .

Radical R¹⁰ preferably comprises hydrocarbon radicals having 6 to 40 carbon atoms , more preferably the hexyl , isohexyl , isooctyl , octyl , decyl , dodecyl , tetradecyl , and the hexadecyl radical , very preferably the hexadecyl radical .

Examples of the organosilicon compounds of the formula (VI ) that are optionally employed in accordance with the invention are isooctyltrimethoxysilane , isooctyltriethoxysilane , N-octyltrimethoxysilane , N- octyl triethoxy si lane, decyltrimethoxysilanes , decyltriethoxysilane, dodecyltrimethoxysiloane , dodecyltriethoxysilane , tetradecyltrimethoxysiloane , tetradecyltriethoxysilane , hexadecyltrimethoxysilane , and hexadecyltriethoxysilane . Radical R¹¹ preferably comprises the methyl radical . The organosilicon compounds of the formula (VI ) that are employed optionally in accordance with the invention are commercial products and/or are preparable by methods that are customary within chemistry .

The rheological additives are preferably polyamide waxes , hydrogenated castor oils , or stearates .

Examples of organic solvents are the compounds already identified above as solvents , preferably alcohols .

It is preferred for no organic solvents to be added to the compositions of the invention .

If the compositions of the invention do comprise one or more additives , the amounts involved are in each case preferably 0 . 5 to 200 parts by weight , more preferably 1 to 100 parts by weight , more particularly 2 to 70 parts by weight , based in each case on 100 parts by weight of modified silane polymer . In an embodiment of the present invention, the adhesive composition may contain 8 to 30 wt% of a modified silane polymer, 0 . 5 to 5 wt% of a crosslinker , 0 . 01 to 1 wt% of a catalyst , 5 to 70 wt% of a filler, and 0 . 1 to 30 wt% of other additives .

As a specific example , the adhesive composition may be T3000 (Wacker ) that is commercially available .

The flooring finish material may be a finishing material of a wood flooring, ceramic tiles , plastic tiles , or a vinyl sheet , but is not limited thereto .

The wood flooring may be classified into hardwood flooring, plywood flooring, laminate flooring, and high- pressure laminate flooring and may classified into strip flooring, plank flooring, and parquet flooring, depending on the shape .

Hereinafter, a method for manufacturing a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention is described in detail with reference with FIG . 2 .

The method for manufacturing a multilayered flooring structure for reducing floor impact sound according to an embodiment of the present invention includes : installing a soft cushion sheet on a finishing mortar without separate surface smoothing, the soft cushion sheet having a plurality of perforated holes to be filled with an adhesive composition; forming a soft adhesive layer by filling the perforated holes of the soft cushion sheet with an adhesive composition and coating the adhesive composition on the surface of at least a portion of the soft cushion sheet , followed by curing; and allowing a floor finishing material to adhere to the surface of the soft adhesive layer .

The adhesive composition may contain a modified silane polymer .

The adhesive composition may be a silyl-terminated polyether ( STPE ) -based composition containing a modified silane polymer, a crosslinker, a filler, and other additives . As a specific example , the modified silicone adhesive composition may be T3000 (Wacker ) that is commercially available .

In an embodiment of the present invention, in the coating of the adhesive composition, valleys of 1 mm or higher are preferably formed by using a trowel scraper with grooves of 1-5 mm, but is not limited thereto . In addition to the trowel scraper , a tool such as a roller may be used .

The curing may be moisture curing at room temperature .

Best Mode for Carrying out the Invention

Hereinafter , preferable examples of the present invention will be described in detail with reference to embodiments and examples together with the accompanying drawings such that a person skilled in the art could easily implement the invention . In particular, the technical spirit , core configuration, and action of the present invention are not limited thereto . In addition, the present invention may be implemented in various different forms and is not limited to embodiments and examples set forth herein .

A multilayered flooring structure was implemented by stacking a 2 . 5 mm-thick perforated PE foam sheet on the standard floor structure , forming a T3000 adhesive ( Wacker ) layer, and then allowing a 7 . 5 mm-thick parquet to adhere thereto . In the perforated PE Foam sheet , the average diameter of the perforated holes was about 10 mm, the distance (d) between the perforated holes was about 4 mm, and the number of perforated holes was about 5000 per unit area of Im².

A flooring structure was manufactured by, without stacking of a perforated PE foam sheet , forming a T3000 adhesive (Wacker) layer on the standard floor structure and then allowing a 7 . 5 T parquet (high-pressure laminate flooring) to adhere thereto .

A finishing mortar was the standard floor structure obtained by 4-week curing, and measurement was conducted while the floor adhesion finishing was not applied .

<Test Example 1> Floor impact sound test

The flooring structures of Example 1 and Comparative Example 1 , and Comparative Example 2 were subj ected to a floor impact sound test according to KS F 2810 and KS F 2863 (Bang, Ball , Tap) by a test lab (demonstration experiment lab) of KCL ( Seosan) , and the results are shown in Table 1 below .

In Table 1 below, " (-1 ) " in "41 ( -1 ) " denotes an impact sound reduction effect of 1 dB compared with 42 dB of the comparative example .

TABLE 1

As shown in Table 1 above , as a result of testing in a total of three experiment rooms in the impact ball impact sound test , the structure of Comparative Example 1 including the soft adhesive layer showed a reduction effect of 0-2 dB compared with Comparative Example 2 including no flooring structure , and Example 1 including the flooring structure of the present invention showed a reduction effect of 1 dB in all three experiment rooms . Both Example 1 and Comparative Example 1 included a soft adhesive layer having an impact cushion effect, and thus exhibited a weight impact sound reduction effect . However, Comparative Example 1 did not show a constant result due to poor accuracy in the thickness of coating and the amount of adhesion of an adhesive . However, Example 1 according to the present invention showed a uniform noise reduction effect in all of three experiment rooms .

There was also the same tendency in the tap impact sound test , wherein Example 1 showed a more uniform noise reduction amount compared with Comparative Example 1 . In addition, Example 1 , compared with Comparative Example 1 , showed an improved effect in the total amount of reduction in the tap impact sound test , unlike the impact ball impact sound test .

<Test Example 2> Adhesive strength test

After ceramic ( concrete ) was washed, a perforated PE foam with a sticky surface was placed on one side thereof , and T3000 was applied, and then wooden flooring was constructed . Curing for 4 days was conducted under conditions of a temperature of 20-23 °C and a humidity of 30-50% to prepare a specimen .

The adhesion load was determined by a direct tensile adhesion strength test method according to KS F 3218 , and the adhesive strength is determined by dividing the adhesion load by the cross-sectional area, and the results are shown in FIG. 5.

As a control, a flooring structure, which had been constructed using a conventional epoxy-based adhesive on site in Ulsan, was subjected to an adhesion test, and the results are shown in FIG. 5.

FIG. 5 shows the adhesion test results of a conventional flooring structure. As shown in FIG. 5, the adhesive strength was 1.10-1.30 N/mm², and the peeled shape was not passed in some spots.

FIG. 6 shows the adhesion tests results of a multilayered flooring structure for reducing floor impact sound according to one example of the present invention. As shown in FIG. 6, the adhesive strength was 1.30 N/mm², and the shape was passed in all spots.

<Test Example 3> Comparison of floor impact sound reduction effect compared with epoxy (hard adhesive) flooring adhesive

In order to determine the floor impact sound reduction effect of the flooring structure using the modified silicone adhesive according to the present invention, a floor impact sound test was conducted according to KS F 2810; KS F 2863 (Bang, Ball, Tap) , and the results are shown in Table 8 below.

FIG. 7 shows the comparison results of a floor impact sound reduction test on a flooring structure constructed using a modified silicone adhesive and a structure constructed using a conventional epoxy-based adhesive on site .

In FIG. 7, "Epoxy+6.5 Flooring" denotes a flooring structure using a conventional epoxy flooring adhesive, and "T3000+6.5T Flooring" denotes a flooring structure using a modified silicone adhesive used in order to provide an impact cushion effect in the present invention. As shown in FIG . 7 , the floor structure using the modified silicone adhesive according to the present invention was excellent in a floor impact sound reduction effect compared with the floor structure using the conventional epoxy-based adhesive .

While the present invention is not limited to the described examples and can be applied to various parts , and it would be obvious to a person s killed in the art that various modifications and changes can be made without departing from the spirit and scope of the present invention . Accordingly, such modifications or changes shall be embraced by the scope of the present invention as defined the appended claims .

Claims

1 . A multilayered flooring structure for reducing floor impact sound, the multilayered flooring structure comprising : a soft cushion sheet installed on a finishing mortar and having a plurality of perforated holes to be filled with an adhesive composition; a soft adhesive layer filling the perforated holes of the soft cushion sheet and formed on the surface of at least a portion of the soft cushion sheet ; and allowing a floor finishing material to adhere to the surface of the soft adhesive layer .

2 . The multilayered flooring structure of claim

1 , wherein the soft cushion sheet is a soft foam sheet or soft sheet containing, as a main ingredient , at least one selected from the group consisting of polyurethane, PVC, LDPE, LLDPE, HDPE, PP, PET , and synthetic and natural rubbers .

3 . The multilayered flooring structure of claim 1 , wherein the soft cushion sheet has a density of 0 . 025- 1 . 2 g/cm³ and a thickness of 0 . 5-30 mm.

4 . The multilayered flooring structure of claim 1 , wherein the soft adhesive layer is a soft-state adhesive layer formed by moisture-curing of an adhesive composition containing a modified silane polymer at room temperature .

5 . The multilayered flooring structure of claim 4 , wherein the adhesive composition containing the modified silane polymer forms a soft adhesive layer having properties of : a viscosity of 10 , 000-500 , 000 CPS before being cured, a Shore A hardness of 10-80 degrees (ISO 868) after being cured into a rubber phase, an adhesive tensile strength of 0.9 or more N/mm² (KS L 1593) , and an elongation of at least 100% (ASTM D 412) .

6. The multilayered flooring structure of claim 4, wherein the adhesive composition is a silyl-terminated polyether (STPE) -based composition containing a modified silane polymer, a crosslinker, a filler, and other additives .

7. The multilayered flooring structure of claim 6, wherein the modified silane polymer is a compound represented by Chemical Formula 1 below:

Y- [ (CR¹ ₂)_b-SiR_a(OR²)_3-a]_x (I) , where Y is an x-valent polymer radical bonded via nitrogen, oxygen, sulfur, or carbon, R may be identical or different and is a monovalent, optionally substituted, SiC-bonded hydrocarbon radical, R¹ may be identical or different and is hydrogen atom or a monovalent, optionally substituted hydrocarbon radical, which may be attached to the carbon atom by a nitrogen, phosphorus, oxygen, sulfur or carbonyl group, R² may be identical or different and is hydrogen atom or a monovalent, optionally substituted hydrocarbon radical, X is an integer from 1 to 10, preferably 1, 2, or 3, more preferably 1 or 2, a may be identical or different and is 0, 1, or 2, preferably 0 or 1, and b may be identical or different and is an integer from 1 to 10, preferably 1, 3, or 4, more preferably 1 or 3, more particularly 1.

8. The multilayered flooring structure of claim 4, wherein the adhesive composition further contains a catalyst .

9. The multilayered flooring structure of claim

8 , wherein the adhesive composition contains 8 to 30 wt% of a modified silane polymer, 0 . 5 to 5 wt% of a crosslinker, 0 . 01 to 1 wt% of a catalyst , 5 to 70 wt% of a filler , and 0 . 1 to 30 wt% of other additives .

10 . The multilayered flooring structure of claim 1 , wherein the flooring finish material is a finishing material of a wood flooring, ceramic tiles , plastic tiles , or a vinyl sheet .

11 . The multilayered flooring structure of claim 1 , wherein the hardness of the soft cushion sheet is a Shore A hardness of 5-70 degrees ( ISO 868 ) and lower than the hardness of the soft adhesive layer in a cured state .

12 . A method for manufacturing a multilayered flooring structure for reducing floor impact sound, the method comprising : installing a soft cushion sheet on a finishing mortar without separate surface smoothing, the soft cushion sheet having a plurality of perforated holes to be filled with an adhesive composition; forming a soft adhesive layer by filling the perforated holes of the soft cushion sheet with an adhesive composition and coating the adhesive composition on the surface of at least a portion of the soft cushion sheet , followed by curing; and allowing a floor finishing material to adhere to the surface of the soft adhesive layer .

13 . The method of claim 12 , wherein the adhesive composition is a silyl-terminated polyether ( STPE) -based composition containing a modified silane polymer , a crosslinker, a filler, and other additives.

14. The method of claim 12, wherein the curing is water-curing at room temperature.