Non-Silicone Thermal Interface Materials

Abstract

The thermally conductive composition includes a non-silicone polymeric resin that is curable in place along the heat dissipation pathway. The composition exhibits low density for particular use in weight-sensitive applications requiring a thermal conductivity of at least 1.5 W / m·K.

Description

[Technical field]

[0001] The present invention relates generally to thermally conductive materials, and more particularly to non-silicone polymer-based thermal interface materials that can be dispensed as a liquid and cured in situ into a relatively low density, thermally conductive coating. [Background technology]

[0002] Thermally conductive materials, for example, are widely employed as interfaces between heat-generating electronic components and heat sinks, allowing the transfer of excess thermal energy from the electronic components to the thermally coupled heat sink. Numerous such thermal interface designs and materials have been implemented, with the best performance being achieved when gaps between the thermal interface and the respective heat transfer surfaces are substantially avoided, promoting conductive heat transfer from the electronic components to the heat sink. Thus, the thermal interface material preferably mechanically conforms to the somewhat uneven heat transfer surfaces of the respective components. Thus, key physical properties of high performance thermal interface materials are flexibility and low hardness. For dispensable materials, it is even more important that the thermal interface be able to wet the heat transfer surfaces, and provide adequate adhesion and cohesion to avoid delamination and maintain the interface shape and function over the expected service life. Thus, dispensable thermal interface materials may be designed with a yield stress to avoid significant spreading after dispensing, or without a yield stress to allow maximum flow and penetration into the surface. The curing behavior of the material can be tailored to avoid particle settling and provide sufficient pre-curing time for rework and handling.

[0003] Electric vehicles (EVs) rely on their on-board battery systems to operate. To meet customer needs, the battery systems installed in EVs must be able to produce high power output and be recharged in a short time. These characteristics require the battery system to carry a large current, which generates a lot of heat. Therefore, dissipating heat from the battery system during charge / discharge cycles has become an important aspect of battery system design. To maintain a safe battery operating temperature, thermal interface materials have been used to dissipate excess heat.

[0004] Improved battery performance is driving the demand for higher thermal conductivity for thermal interface materials. Traditionally, thermal conductivity has been achieved by increasing the loading of conductive fillers. However, highly loaded materials tend to be highly viscous, resulting in slower dispensing speeds and limiting production throughput. In addition, highly loaded materials exhibit high density due to the relatively high density of thermally conductive filler particles. The increased weight of the thermal interface material can reduce vehicle performance. Highly loaded thermal materials also tend to exhibit significant abrasiveness, which can damage dispensing equipment.

[0005] Silicone oils and resins are widely used in thermal interface materials because of their low viscosity and high thermal stability. However, because silicone oils have low surface tension, they tend to "bleed out" from the intended application location, which can cause them to spread on the substrate and affect adjacent surfaces. For example, silicone thermal materials can inhibit the paintability of a surface by undesirably spreading from the intended location. In addition, most silicone resins contain volatile cyclic silicone oligomers that can affect the function of other components, such as optical sensors.

[0006] Several non-silicone materials have been proposed and implemented in thermal interface applications. However, it has been difficult to design non-silicone systems that exhibit the right combination of temperature stability, pre-cure viscosity, and cured hardness. The development of silyl-modified polymers has shown promise due to their desirable mechanical properties, such as low hardness, high service temperature, and versatility. The use of these and other non-silicone polymers in thermal interface applications has traditionally been achieved with well-known thermally conductive particulate fillers, such as aluminum nitride, silicon carbide, aluminum, alumina trihydrate, and boron nitride. Each of these filler materials suffers from drawbacks, such as high cost, high abrasiveness, and low hydrolytic stability, limiting their use in certain applications. Summary of the Invention [Problem to be solved by the invention]

[0007] It is therefore an object of the present invention to provide a thermally conductive material that exhibits properties useful in weight-sensitive applications, such as low density.

[0008] It is another object of the present invention to provide a low density thermally conductive material formed from a one-part or two-part composition that can be dispensed via conventional dispensing equipment. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0009] In accordance with the present invention, low density, high thermal conductivity materials can be formed from compositions that exhibit a suitable viscosity for dispensing as a curable liquid coating via conventional liquid dispensing equipment. The compositions achieve these properties while also exhibiting reduced abrasiveness in non-silicone formulations. The compositions generally include three main components: a non-silicone polymer resin, a diluent compatible with the non-silicone polymer resin, and a thermally conductive particulate filler incorporated therein. The material before curing exhibits a liquid, dispensable viscosity and can be cured to form a soft solid with high thermal conductivity. The specific formulation of the thermally conductive filler incorporating graphite particles allows the material to have a viscosity of 2.4 g / cm. 3It is possible to show a density of less than 100 nm.

[0010] In one embodiment, the thermally conductive composition comprises a liquid diluent having a viscosity of less than 500 cP at 25° C., a silyl-modified non-silicone polymeric resin soluble in the diluent, and a particulate filler comprising 30-70 weight percent graphite particles having an average particle size of 15 μm to 150 μm and the remaining weight percent non-graphite particles having an average particle size less than 33% of the average particle size of the graphite. The thermally conductive composition has a mass of 2.4 g / cm 3 It exhibits a density of less than 1.5 W / m K and a thermal conductivity of at least 1.5 W / m K.

[0011] The silyl-modified non-silicone polymeric resin may be condensation curable and the composition may include a catalyst effective to promote condensation curing of the silyl-modified non-silicone polymeric resin. The silyl-modified non-silicone polymeric resin may include alkoxysilane end groups.

[0012] The composition is -1 and may be curable at or above ambient temperature from a viscosity of less than 1000 Pa·s at 25°C to a cured hardness of 20 Shore 00 to 80 Shore A.

[0013] The graphite particles may be coated with pyrolytic pitch carbon. The non-graphite particles may be selected from boron nitride, aluminum nitride, alumina, alumina trihydrate, aluminum, silicon carbide, silicon, silica, silicates, magnesium oxide, magnesium hydroxide, zinc oxide, and mixtures thereof. At least a portion of the non-graphite particles may be surface treated with an alkyl compound having 3 to 12 carbon atoms.

[0014] The non-graphitic particles may have an average particle size of less than 10 μm, and the particle sizes may be distributed in a multimodal distribution having a first peak between 0.1 and 1 μm and a second peak between 1 and 10 μm.

[0015] The thermal interface resin composition may be formed from a two-part composition including a first part having a diluent having a viscosity of less than 500 cP at 25°C and a non-silicone polymeric resin soluble in the diluent, and a second part having a catalyst effective to promote a condensation cure reaction of water and the non-silicone polymeric resin. At least one of the first and second parts includes graphite particles having an average particle size of 15 μm to 150 μm and non-graphite particles having an average particle size of less than 10 μm. The two-part composition, when the first and second parts are mixed at or above ambient temperature, has a hardness of 20 Shore 00 to 80 Shore A, a thermal conductivity of at least 1.5 W / m·K, and a viscosity of 2.4 g / cm. 3 It is possible to cure to a thermal interface having a density less than 1000 .mu.m.

[0016] The non-silicone polymeric resin may contain alkoxysilane end groups and may constitute 10 to 35 weight percent of the composition.

[0017] The graphitic and non-graphitic particles together define a particulate filler composition in which the graphitic particles comprise 30-70% by weight.

[0018] The catalyst may include an organometallic compound and a moisture scavenger may be included in the first part of the composition.

[0019] The battery system includes a battery and a thermally conductive composition thermally coupled to the battery. The thermally conductive composition includes a liquid diluent having a viscosity of less than 500 cP at 25° C., a silyl-modified non-silicone polymeric resin soluble in the diluent, and a particulate filler including 30-70% by weight of graphite particles having an average particle size of 15 μm to 150 μm and the remaining weight % of non-graphite particles having an average particle size less than 33% of the average particle size of the graphite. The thermally conductive composition has a mass of 2.4 g / cm. 3 It exhibits a density of less than 1.5 W / m K and a thermal conductivity of at least 1.5 W / m K.

[0020] The thermally conductive composition can be cured to a hardness of 20 Shore A to 80 Shore A and has a hardness of 2.2 g / cm 3It may exhibit a density of less than 100 nm.

[0021] DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS The above-listed objects and advantages, together with other objects, features, and advancements represented by the present invention, are presented herein with respect to specific embodiments, however, it is recognized that other embodiments and aspects of the present invention are within the purview of those skilled in the art.

[0022] The thermally conductive composition of the present invention may be formed as a coating on a surface or self-supporting substrate for placement along a heat dissipation path to remove excess heat from heat-generating electronic components, typically such as the battery system of an electric vehicle. The thermally conductive composition is preferably non-silicone and is filled with thermally conductive particles to achieve the desired thermal conductivity, typically at least 1.5 W / m·K. The composition preferably exhibits sufficient flexibility and cohesion to provide a stable interface.

[0023] The thermally conductive composition is preferably dispenseable via conventional liquid dispensing equipment and then hardens to a soft solid. In some embodiments, the composition can be first separated into two or more parts and dispensed from at least two separate containers to separate the reactive silyl-modified polymer resin from reaction catalysts and water until the time when hardening of the material is desired. The composition of the present invention is hardened in situ after dispensing by silyl hydrolysis and condensation. In other embodiments, the composition may be stored in and dispensed from a single container, optionally in the presence of a reaction inhibitor or in the absence of moisture to prevent premature hardening of the silyl-modified polymer resin.

[0024] This composition has a density of 2.4 g / cm 3 The thermal interface material of the present invention includes a composite blend of thermally conductive fillers that provide the thermally conductive material with a unique set of properties, including a density less than 0.01 g / mol / g, which allows for lightweight assemblies using the thermal interface material of the present invention.

[0025] resin A variety of silyl-modified resins may be used in the matrix of the present invention. Condensation-curable silyl-modified resins preferably participate in a hydrolysis-condensation cure pathway at ambient temperature or higher. The resin is preferably non-silicone, and the composition contains no more than trace amounts of silicone. In some embodiments, the composition does not contain silicone. In some embodiments, the non-silicone resin is substantially free of -Si-O- units in the polymer therein. In other embodiments, the non-silicone resin excludes polysiloxane resins, and does not have repeating -Si-O- units therein.

[0026] As used herein, the silyl-modified reactive polymer resin is present in the range of about 5 to about 50 weight percent of the total composition; in some embodiments, the composition comprises a range of about 10 to about 40 weight percent of the silyl-modified reactive polymer resin; in some embodiments, the composition comprises a range of 15 to 35 weight percent of the silyl-modified reactive polymer resin; in some embodiments, the composition comprises a range of 18 to 28 weight percent of the silyl-modified reactive polymer resin.

[0027] Examples of suitable resins for the reactive resin of the present invention include reactive polymer resins having at least one silyl reactive functional group that includes at least one bond that can be activated with water. Exemplary silyl reactive functional groups include alkoxysilanes, acetoxysilanes, and ketoximesilanes.

[0028] The reactive polymer resin can be any non-silicone polymer that can participate in silyl hydrolysis reaction.For example, the reactive polymer resin can be selected from a wide range of polymers as polymer systems with reactive silyl groups, such as silyl-modified reactive polymers.The silyl-modified reactive polymer preferably has a non-silicone backbone to limit or avoid silicone release when heated, such as when used in electronic devices.Preferably, the silyl-modified reactive polymer has a flexible backbone to reduce elastic modulus and glass transition temperature.Preferably, the silyl-modified reactive polymer has a flexible backbone of polyether, polyester, polyurethane, polyacrylate, polyisoprene, polybutadiene, polystyrene-butadiene, polyisobutylene or polybutylene-isoprene.

[0029] Silyl-modified reactive polymers can be obtained by reacting a polymer with at least one ethylenically unsaturated silane in the presence of a radical initiator, and the ethylenically unsaturated silane has at least one hydrolyzable group on silicon atom.For example, the silyl-modified reactive polymer can be a dimethoxysilane-modified polymer, a trimethoxysilane-modified polymer, or a triethoxysilane-modified polymer.For example, the silyl-modified reactive polymer can include silane-modified polyether, polyester, polyurethane, polyacrylate, polyisoprene, polybutadiene, polystyrene-butadiene, or polybutylene-isoprene.

[0030] The ethylenically unsaturated silane may be selected from the group consisting of vinyltrimethoxysilane, vinyltriethoxysilane, vinyldimethoxymethylsilane, vinyldiethoxymethylsilane, trans-β-methylacrylic acid trimethoxysilylmethyl ester, and trans-β-methylacrylic acid trimethoxysilylpropyl ester.

[0031] The silyl-modified reactive polymer preferably contains silyl groups with at least one hydrolyzable group on the silicon atom in statistical distribution, for example, a polymer having the general formula:

[0032] [ka] where R is a monovalent to tetravalent polymer radical, R 1 , R 2 , R 3 are each independently an alkyl or alkoxy group having 1 to 8 carbon atoms, A is a carboxy, carbamate, amide, carbonate, ureido, urethane, sulfonate group, an oxygen atom or a covalent bond, and x=1 to 8 and n=1 to 4. In some embodiments, R does not include any -Si-O- units.

[0033] The silyl-modified reactive polymer can also be obtained by reacting a polymer having a hydroxyl group with an alkoxysilane having an isocyanate group. For example, the silyl-modified reactive polymer can be a dimethoxysilane-modified polyurethane polymer, a trimethoxysilane-modified polyurethane polymer, or a triethoxysilane-modified polyurethane polymer. Furthermore, the silyl-modified reactive polymer can be represented by the average general formula:

[0034] [ka] In the formula, R is a monovalent to tetravalent polymer residue, and the residue R 1 , R 2 and R 3 at most one third of the radicals are independently alkyl radicals having 1 to 4 carbon atoms, and the residues R 1 , R 2 and R 3 At least one-quarter of the radicals R are independently ethoxy residues, and the remaining radicals R 1 , R 2 and R 3 are each independently a methoxy radical, and n=1 to 4. In some embodiments, R does not contain any -Si-O- units.

[0035] Silyl-modified reactive polymers are available, for example, as dimethoxysilane-modified MS polymers with a polyether backbone and XMAP™ polymers with a polyacrylate backbone from Kaneka Belgium NV, trimethoxysilane-modified ST polymers from Evonik, triethoxysilane-modified Tegopac™ polymers from Evonik, silane-modified Desmoseal™ polymers from Covestro, or di- or tri-methoxysilane-modified Geniosil™ polymers from Wacker.

[0036] Diluent The compositions of the present invention preferably contain a diluent to adjust the viscosity of the dispensed composition, especially under shear, and to maintain flexibility / softness properties when the composition is in the cured state. The cured compositions exhibit a relatively low modulus or hardness of less than 80 Shore A, which relieves stress during electronic component assembly and promotes compatibility of thermal materials with the respective contact surfaces of the electronic components.

[0037] The diluents useful in the compositions of the present invention are those that are effective in promoting the flowability of the aggregates that make up the composition. The diluents of the present invention may be compatible with, and preferably a solvent for, the selected non-silicone resin, and preferably a low volatility liquid that reduces the overall viscosity of the composition before curing so that the composition is easily dispenseable through a liquid dispensing device. Thus, the diluent may exhibit a viscosity of less than 500 cP at 25°C. In another embodiment, the diluent may exhibit a viscosity of less than 250 cP at 25°C. In a further embodiment, the diluent may exhibit a viscosity of less than 100 cP at 25°C. Preferably, the diluent exhibits a viscosity of 1 to 50 cP at 25°C.

[0038] The diluent is preferably added to the composition in an amount suitable to properly adjust the viscosity for dispensability before curing and softness after curing. In some embodiments, the diluent may comprise about 1-50 weight percent of the composition. In some embodiments, the diluent may comprise about 1-20 weight percent of the composition. In some embodiments, the diluent may comprise about 5-10 weight percent of the composition. The diluent may preferably be present at less than 20 weight percent of the composition.

[0039] Examples of diluents include benzoates, oleates, ricinoleates, phthalates, trimellitates, teraphthalates, adipates, sebacates, azelates, maleates, citrates, epoxidized vegetable oils, organic sulfates, organic phosphates, glycols and polyethers, ether esters, polyolefins, and combinations thereof.

[0040] Thermally Conductive Particles The selection of thermally conductive particulate filler is important to achieve the desired properties of the present invention, including low density, high thermal conductivity, low abrasion, high dispensability, form stability and cure flexibility. Applicants have surprisingly found that blends of graphitic and non-graphitic particles within critical ranges of average particle size, relative average particle size, and relative loading concentration can produce a composite with a viscosity of 2.4 g / cm. 3 It has been found that by using the above-mentioned method, it is possible to achieve a highly thermally conductive composition exhibiting a density of less than 2.4 g / cm. Prior art compositions require high loading concentrations of relatively high density thermally conductive particles, resulting in an overall material density of 2.4 g / cm. 3 It is theorized that the relatively large graphite particles may reduce the abrasiveness of the dispensable composition while maintaining a high degree of thermal conductivity.

[0041] The thermally conductive filler composition included in the material of the present invention includes both graphitic and non-graphitic particles. The filler composition includes 30% to 70% by weight of graphitic particles; in some embodiments, the filler composition includes 40% to 60% by weight of graphitic particles. The graphitic particles preferably have an average particle size (d50 The graphite particles may be selected from natural graphite, synthetic graphite, and graphite coated with pyrolytic pitch carbon.

[0042] The remaining weight percent (balance) of the filler composition is non-graphite particles. Non-graphite particles useful in the present invention include boron nitride, aluminum nitride, alumina, alumina trihydrate, aluminum, silicon carbide, silicon, silica, silicates, magnesium oxide, magnesium hydroxide, zinc oxide, and mixtures thereof. In some embodiments, the non-graphite particles may be surface treated with an alkyl compound having 3 to 12 carbon atoms for compatibility with the polymer resin. Surface treatment agents include alkoxysilanes, fatty acid compounds.

[0043] The non-graphite particles preferably have an average particle size (d 50 In some embodiments, the non-graphitic particles have an average particle size (d 50 ) is less than 10 μm; in some embodiments, the average particle size of the non-graphitic particles (d 50 ) is less than 5 μm. The non-graphitic particles may be present in a multimodal particle size distribution. As used herein, the term "multimodal" size distribution refers to a distribution having multiple concentration peaks (maxima) of particle sizes. In some embodiments, the bimodal particle size distribution of the non-graphitic particles includes a first concentration peak between 0.1 μm and 1 μm and a second concentration peak between 1 μm and 10 μm.

[0044] The compositions of the invention desirably exhibit a thermal conductivity of at least 1.5 W / m K, more preferably at least 2 W / m K, and even more preferably at least 2.5 W / m K. The compositions of the invention also preferably have a thermal conductivity of at least 2.4 g / cm 3 less than 2.2 g / cm 3 It shows a density of less than .

[0045] The selection of graphite and non-graphite thermally conductive particles also determines the abrasion of the overall composition. The abrasion of the composition can be evaluated by a slurry abrasion test according to ASTM G75. It has been found that compositions of the present invention incorporating critical ranges of graphite and non-graphite particles exhibit desirable low abrasion with less than 3 mg of aluminum metal loss per 6 hours of abrasion testing in a slurry test. This low abrasion allows the dispensing device to be maintained over long periods of use.

[0046] Reaction catalyst Reaction catalysts may be used to further accelerate the hydrolysis-condensation cure reaction of the silyl-modified reactive resin. Examples of reaction catalysts useful in the compositions of the present invention include organotin, organozinc and organotitanium compounds (collectively referred to herein as "organometallic catalysts") that accelerate the moisture cure of the silyl-modified reactive resin.

[0047] The reaction catalyst used in the compositions of the present invention is present in the range of about 0 to about 1 weight percent of the reaction catalyst. In some embodiments, the composition includes a range of 0.1 to about 0.5 weight percent of the reaction catalyst. In some embodiments, the composition includes less than 0.5 weight percent of the reaction catalyst, more preferably less than 0.3 weight percent of the reaction catalyst. As used herein, a concentration of "less than" a particular amount may include zero.

[0048] The thermally conductive compositions of the present invention are preferably curable in the presence of water at or above ambient temperature (moisture curable). Depending on the application, moisture may be available from the ambient environment or from water provided in the reactants. Preferably, the amount of water required in the composition itself is small so as not to interfere with the functional properties of the thermal material. In some embodiments, water is present in the compositions of the present invention in the range of 0-2 weight percent of the composition. In some embodiments, the composition comprises water in the range of 0.1-1 weight percent. In some embodiments, the composition comprises water in the range of less than 2 weight percent, more preferably less than 1 weight percent.

[0049] As used herein, the term "ambient temperature" is intended to mean the temperature of the environment in which the reaction occurs, within a temperature range of 15 to 30°C, preferably 25°C. The thermally conductive composition is curable at ambient temperature within 72 hours, preferably within 24 hours. The thermally conductive composition may also be curable at elevated temperatures. As used herein, the term "curable" is intended to mean that the composition is capable of reacting under appropriate conditions and the reaction product has an irreversible solid form.

[0050] Water Scavenger The composition of the present invention preferably contains a water scavenger to prevent the reaction of resin-containing components before dispensing so as to extend shelf life.The water scavenger may be, for example, alkyltrimethoxysilane, oxazolidine, zeolite powder, p-toluenesulfonyl isocyanate, oxocalcium, and ethyl orthoformate.The water scavenger is preferably vinyltrimethoxysilane.If there is too much water scavenger in the composition, curing will be slow.The water scavenger may be present in an amount of more than about 0.05% by weight and less than about 5% by weight, for example about 0.5% by weight, of the composition.

[0051] Optional Additives In accordance with some embodiments of the present invention, the compositions described herein may further comprise one or more additives selected from fillers, stabilizers, antioxidants, adhesion promoters, solvents, pigments, wetting agents, dispersants, flame retardants, extenders, and corrosion inhibitors. In other embodiments, the compositions may be free of any or all of the additives.

[0052] characteristics The curable composition of the present invention is preferably curable at ambient temperature or above, for example at 25° C. or above. The curable composition is preferably curable within 1 s at 25° C. -1 and more preferably has a viscosity of less than 1000 Pa·s as measured by a parallel plate rheometer at a shear rate of 1 s at 25°C. -1The curable composition preferably exhibits a dispensing rate of at least 100 g / min, more preferably at least 200 g / min, through a 3.175 mm orifice under a pressure of 90 psi at 25° C. After curing of the polymeric resin, the composition preferably exhibits a hardness of 20 Shore 00 to 80 Shore A, as measured by a durometer at 25° C. EXAMPLES

[0053] The examples described herein provide exemplary compositions, which are not intended to be limiting of the various compositions contemplated by the present invention.

[0054] Example 1 Compositions 1-1 through 1-6 in Tables 1a and 1b below represent examples of single component formulations.

[0055] [Table 1a]

[0056] [Table 1b]

[0057] Example 2 Compositions 2-1 and 2-2 in Table 2A below represent examples of two-component formulations, with the first part of each formulation designated as part "A" and the second part of each formulation designated as part "B."

[0058] [Table 2A]

[0059] The properties of the cured compositions of Example 2 after mixing parts A and B for each of Compositions 2-1 and 2-1 are shown below in Table 2B.

[0060] [Table 2B]

[0061] Example 3 Compositions 3-1, 3-2, and 3-3 represent control formulations that do not have the thermally conductive filler blend of the present invention. Although the control formulations exhibit good thermal conductivity, their densities are inadequate for the intended applications of the present invention.

[0062] [Table 3]

[0063] Example 4 Compositions 4-1 and 4-2 represent formulations consistent with the present invention, while compositions 4-3, 4-4, and 4-5 represent prior art thermally conductive particle blends containing relatively large non-graphitic particle sizes. As shown in Table 4 below, compositions 4-1 and 4-2 exhibit significantly reduced abrasiveness compared to compositions 4-3, 4-4, and 4-5. Abrasiveness was tested in a Miller Slurry Abrasive Tester in accordance with ASTM G75. The material was diluted with an equal amount of diluent (the same oil was used for all compositions in this Example 4) to form a slurry. Aluminum abrasive blocks were used to measure metal loss after 6 hours of abrasion.

[0064] [Table 4]

Claims

1. A thermally conductive composition, comprising: 1 s －１ and a liquid diluent having a viscosity of less than 500 cP at 25°C; A silyl-modified non-silicone polymer resin soluble in the diluent; and A particulate filler comprising: (i) 30 to 70% by weight of graphite particles having an average particle size of 15 μm to 150 μm; and (ii) The remaining non-graphite particles having an average particle size of less than 33% of the average particle size of the graphite, and The heat-conductive composition has a density of less than 2.4 g / cm ３ and a heat conductivity of at least 1.5 W / m·K, and is a heat-conductive composition.

2. The thermally conductive composition according to claim 1, wherein the silyl-modified non-silicone polymer is condensation curable and optionally contains a catalyst effective to promote the condensation curing of the silyl-modified non-silicone polymer.

3. The silyl-modified non-silicone polymer contains alkoxysilane end groups; and / or The silyl-modified non-silicone polymer does not contain -Si-O- units; and / or The thermally conductive composition according to claim 1 or 2, wherein the silyl-modified non-silicone polymer is a two-part composition.

4. The composition has a viscosity of 1 s －１ and is curable at 25°C from a viscosity of less than 1000 Pa·s at 25°C to a cured hardness of 20 Shore 00 to 80 Shore A. The thermally conductive composition according to claim 1 or 2.

5. The thermally conductive composition according to claim 1 or 2, wherein the graphite particles are coated with pyrolytic pitch carbon.

6. The thermally conductive composition according to claim 1 or 2, wherein the non-graphite particles are selected from boron nitride, aluminum nitride, alumina, alumina trihydrate, aluminum, silicon carbide, silicon, silica, silicate, magnesium oxide, magnesium hydroxide, zinc oxide, and mixtures thereof.

7. The thermally conductive composition according to claim 1 or 2, wherein at least a portion of the non-graphite particles are surface-treated with an alkyl compound having 3 to 12 carbon atoms.

8. The thermally conductive composition according to claim 1 or 2, wherein the non-graphite particles have an average particle size of less than 10 μm.

9. The thermally conductive composition according to claim 1 or 2, wherein the non-graphite particles have a multimodal particle size distribution.

10. The thermally conductive composition according to claim 9, wherein the multimodal particle size distribution includes a first peak between 0.1 μm and 1 μm and a second peak between 1 μm and 10 μm.

11. A cured reaction product of the thermally conductive composition according to claim 1 or 2.

12. A battery; and A battery system comprising the thermally conductive composition according to claim 1 or 2 thermally coupled to the battery.

13. The battery system according to claim 12, wherein the thermally conductive composition is cured to a hardness of 20 Shore 00 to 80 Shore A.

14. The battery system according to claim 12, wherein the thermally conductive composition has a density of less than 2.2 g / cm ３ 3.

15. A thermal interface formed from a two-part composition, A first part comprising a diluent having a viscosity of less than 500 cP at 25°C and a non-silicone polymer resin soluble in the diluent; and A second part comprising water and a catalyst effective to promote the condensation curing reaction of the non-silicone polymer resin comprising At least one of the first part and the second part comprises graphite particles having an average particle size of 15 μm to 150 μm and non-graphite particles having an average particle size of less than 10 μm, The two-part composition cures when the first part and the second part are mixed at a temperature above ambient temperature, and forms a thermal interface having a hardness of 20 Shore 00 to 80 Shore A, a thermal conductivity of at least 1.5 W / m·K, and a density of less than 2.4 g / cm ３ 3, a thermal interface.

16. The thermal interface according to claim 15, wherein the non-silicone polymer is a silyl-modified polymer containing alkoxysilane end groups.

17. The thermal interface according to claim 15 or 16, wherein the diluent and the non-silicone polymer together constitute an organic resin composition, and the non-silicone polymer constitutes 10 to 35% by weight of the organic resin composition.

18. The thermal interface according to claim 15 or 16, wherein the graphite particles and the non-graphite particles together constitute a particulate filler composition in which the graphite particles account for 30 to 70% by weight.

19. The thermal interface according to claim 15 or 16, wherein the catalyst comprises an organometallic compound.

20. The thermal interface according to claim 15 or 16, wherein the first part contains a moisture scavenger.

21. Use of the thermally conductive composition according to claim 1 as a thermal interface material.