WO2022084394A1

WO2022084394A1 - Composite article

Info

Publication number: WO2022084394A1
Application number: PCT/EP2021/079103
Authority: WO
Inventors: Elias Ruda Shakour; Yeonsuk Roh
Original assignee: Basf Se
Priority date: 2020-10-22
Filing date: 2021-10-20
Publication date: 2022-04-28

Abstract

A composite article (P) comprising at least one coversheet (A); at least one composite (B) comprising at least one reinforcing structure (B1) and at least one aerogel (B2); and at least one binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet.

Description

COMPOSITE ARTICLE

FIELD OF THE INVENTION

The presently claimed invention is directed to a composite article (P) comprising at least one coversheet (A); at least one composite (B) comprising at least one reinforcing structure (B1 ) and at least one aer- ogel(B2); and at least one binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet.

BACKGROUND OF THE INVENTION

Structurally rigid composites are a desirable material for many industries such as the construction and the automotive industry due to their light weight and higher strength, in comparison to other materials. Panel constructions are shaped parts which are used as structural reinforcement for automotives.

These composites and the process for producing them are well-known in the state of the art. Additionally, honeycomb sandwich panels have also been extensively used in the automotive industry. Honeycomb sandwich panels comprise of two thin and hard surface sheets bonded to a thick and lightweight honeycomb structured core. Although, the honeycomb structure provides for good mechanical properties, it has limited applicability, even though it has reduced heat conduction, due to the its flammability and also difficult to mold into desired shape.

Thus, the object of the presently claimed invention is to provide a composite article that could provide structural rigidity; thus, it could be molded into desired share, along with superior flame retardancy and reduced heat conduction. It also further object of the presently claimed invention that the composite article displays improved Noise Vibration and Harshness (NVH) testing data as this could be used in automotive industry.

SUMMARY OF THE INVENTION

Surprisingly, it was found that the composite article (P) according to presently claimed invention not only provided desired thermal insulation, flame retardancy but also structural rigidity, thus the composite article (P) could be moulded in any desired shape as per the requirement. This, composite article (P) according presently claimed invention also displayed excellent NVH data along with bone fire test results.

Accordingly, the first aspects of the presently claimed invention is directed a composite article (P) comprising: i. at least one coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1 ) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet.

Second aspects of the presently claimed invention is directed to a process for preparing a composite article (P) comprising the steps of: i. providing at least one composite (B);

II. providing at least one coversheet (A); ill. covering at least a part of the composite (B) with the cover sheet (A); and iv. spraying at least one binder composition onto the coversheet(A) to form a pre-impregnated blank, and v. compression moulding of the pre-impregnated blank.

The third aspects of the presently claimed invention is directed to the use of the composite article (P) as a thermal insulator.

The fourth aspects of the presently claimed invention is directed to the use of the composite article (P) as non-combustible or combustible product.

The fifth aspects of the presently claimed invention is directed to the use of the composite article (P) as an automotive part.

The sixth aspects of the presently claimed invention is directed to the use of the composite article (P) is to develop a 3-dimensional semi structural or a 3-dimesional structural framework.

The seventh aspects of the presently claimed invention is directed to an article comprising the composite article (P).

The seventh aspects of the presently claimed invention is directed to an automotive part comprising the composite article (P).

DESCRIPTION OF THE DRAWINGS

FIG. 1 illustrates the fabrication process of the composite (B) wherein a gel precursor 11 is added to a reinforcing batting 12 in some constraining mold type structure 10.

FIG. 2 shows an aerogel composite 20 is formed with an inorganic or organic batting/sheet 21 and an aerogel matrix of composite (B).

FIG. 3 shows a gel precursor mixed with microfiber material being cast into a continuous lofty fiber batting material to generate the composite (B) as illustrated in FIG. 4. FIG. 3 shows three layers of laminate consisting of a layer of lofty fiber batting 32, a fine copper mesh 31 , and a second layer of lofty fiber batting 32.

FIG. 4 shows another three layers of laminate, a layer of lofty fiber batting 42, a woven carbon fiber textile 41 , and a second layer of fiber batting 42. While these laminates are shown to be symmetric, this is preferred and not mandatory.

FIG. 5 is an exploded partial view of an aerogel composite (B)showing the composite reinforced both on a macro level with a fiber batting and on a micro level with individual filaments.

FIG. 6 is an exploded view of composite (B). consisting of a layer of fiber batting 61 , a layer of silicon carbide felt 62, a fine copper mesh 63, a layer of silicon carbide felt 62, and a layer of fiber batting 61 .

Fig. 7 shows alignment of coversheets and composite (B) prior to addition of binder composition. The composite (B)(72), herein Slentex® is used, is placed in between two coversheets (71).

Fig. 8 shows composite article (P) having two cover sheets laminated with binder in A-B-A fashion.

Fig. 9 shows the temperature attained while performing the bonfire test over a period of 20 minutes. Bonfire test performed in accordance to a method as described in presently claimed invention.

Fig. 10a is the top part of the composite article (P) after exposing to bonfire test for 20 minutes. Fig. 10b is the bottom part of the composite article (P) after exposing to bonfire test for 20 minutes.

DETAILED DESCRIPTION

Before the present compositions and formulations of the presently claimed invention are described, it is to be understood that this invention is not limited to particular compositions and formulations described, since such compositions and formulation may, of course, vary. It is also to be understood that the terminology used herein is not intended to be limiting, since the scope of the presently claimed invention will be limited only by the appended claims.

If hereinafter a group is defined to comprise at least a certain number of embodiments, this is meant to also encompass a group which preferably consists of these embodiments only. Furthermore, the terms 'first', 'second', 'third' or 'a', 'b', 'c', etc. and the like in the description and in the claims, are used for distinguishing between similar elements and not necessarily for describing a sequential or chronological order. It is to be understood that the terms so used are interchangeable under appropriate circumstances and that the embodiments of the presently claimed invention described herein are capable of operation in other sequences than described or illustrated herein. In case the terms 'first', 'second', 'third' or '(A)', '(B)' and '(C)' or '(a)', '(b)', '(c)', '(d)', 'i', 'ii' etc. relate to steps of a method or use or assay there is no time or time interval coherence between the steps, that is, the steps may be carried out simultaneously or there may be time intervals of seconds, minutes, hours, days, weeks, months or even years between such steps, unless otherwise indicated in the application as set forth herein above or below.

Furthermore, the ranges defined throughout the specification include the end values as well i.e. a range of 1 to 10 implies that both 1 and 10 are included in the range. For the avoidance of doubt, applicant shall be entitled to any equivalents according to applicable law.

In the following passages, different aspects of the presently claimed invention are defined in more detail. Each aspect so defined may be combined with any other aspect or aspects unless clearly indicated to the contrary. In particular, any feature indicated as being preferred or advantageous may be combined with any other feature or features indicated as being preferred or advantageous.

Reference throughout this specification to 'one embodiment' or 'an embodiment' means that a particular feature, structure or characteristic described in connection with the embodiment is included in at least one embodiment of the presently claimed invention. Thus, appearances of the phrases 'in one embodiment' or 'in an embodiment' in various places throughout this specification are not necessarily all referring to the same embodiment.

Furthermore, the particular features, structures or characteristics may be combined in any suitable manner, as would be apparent to a person skilled in the art from this disclosure, in one or more embodiments. Furthermore, while some embodiments described herein include some, but not other features included in other embodiments, combinations of features of different embodiments are meant to be within the scope of the presently claimed invention, and form different embodiments, as would be understood by those in the art. For example, in the appended claims, any of the claimed embodiments can be used in any combination.

In a first embodiment, the presently claimed invention is directed to a composite article (P) comprising: i. at least one coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1 ) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1 ) comprises a lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet; more preferably the composite article (P) comprises: i. at least two coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1 ) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/organic sheet/inorganic sheet; even more preferably, the composite article (P) comprises: i. at least two coversheet (A); ii. at least one composite (B) comprising at least one reinforcing structure (B1) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/organic/ inorganic sheet; and the binder (C) is selected from an organic binder, inorganic binder or combination thereof; most preferably, the composite article (P) comprises: i. at least two coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting sheet and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/organic/ inorganic sheet; and the binder (C) is a polyurethane resin composition; and in particular the composite article (P) comprises: i. at least two coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1) and at least one aerogel(B2); and ill. at least one polyurethane resin binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting sheet and a continuous aerogel (B2) through said batting; and the polyurethane resin composition comprises:

(a) at least one isocyanate, and

(b) at least one isocyanate reactive component, wherein (a) and (b) are present at an isocyanate index in the range of 100 to 180.

In another preferred embodiment, the composite article (P) comprises at least two coversheets (A).

In another preferred embodiment, the composite (B) is sandwiched between the two coversheets (A).

In another preferred embodiment, the coversheet(s) is having a thickness in the range of 0.1 mm to 10 mm; more preferably the coversheet(s) is having a thickness in the range of 0.3 mm to 8 mm; even more preferably the coversheet(s) is having a thickness in the range of 0.5 mm to 6 mm; most preferably the coversheet(s) is having a thickness in the range of 0.8 mm to 6 mm; and in particular the coversheet(s) is having a thickness in the range of 1 mm to 5 mm;

In another preferred embodiment, the coversheet is selected from fiber mat, thermosetting sheet, or thermoplastic sheet. In another preferred embodiment, the fiber mat is a sheet comprising fiberglass, carbon fiber, natural fiber, mineral wool, basalt, ceramic or any combination thereof.

In another preferred embodiment, the thermosetting coversheet is selected from polyurea sheet or polyurethane sheet; more preferably the thermosetting coversheet is polyurethane sheet.

In another preferred embodiment, the thermoplastic coversheet is selected from nylon, polyester, thermoplastic reinforced tapes or thermoplastic paper including thermoplastic reinforced tape.

In another preferred embodiment, the composite (B) comprises at least one reinforcing structure (B1 ) and at least one aerogel(B2).

In another preferred embodiment, the aerogels are a class of materials formed by removing a mobile interstitial solvent phase from the pores of a gel structure supported by an open-celled polymeric material at a temperature and pressure above the solvent critical point. By keeping the solvent phase above the critical pressure and temperature during the entire solvent extraction process, strong capillary forces generated by liquid evaporation from very small pores that cause shrinkage and pore collapse are not realized. Aerogels typically have low bulk densities preferably in the range of 0.03 to 0.3 g/cc, very high surface areas generally in the range of 400 to 1 ,000 m²/g and higher, preferably in the range of 700 to 1000 m²/g), high porosity > 95% , preferably > 97%, and relatively large pore volume > 3.8 mL/g, preferably about > 3.9 mL/g. The combination of these properties in an amorphous structure gives the lowest thermal conductivity values 9 to 16 mW/m.K at 37 °C. and 1 atmosphere of pressure for any coherent solid material.

The composite (B) of the present invention comprises two phases. The first is a low-density aerogel and the second is a reinforcing phase.

In another preferred embodiment, the aerogel (B2) comprises selected from inorganic or organic gel forming materials or any combinations thereof.

In another preferred embodiment, the inorganic gel is selected from oxides of zirconia, yttria, hafnia, alumina, titania, ceria, silica, or any combination thereof.

In another preferred embodiment, the aerogel matrix of the composite (B) can be organic, inorganic, or a mixture thereof. The wet gels used to prepare the aerogels may be prepared by any of the gel-forming techniques that are well-known to those trained in the art: examples include adjusting the pH and/or temperature of a dilute metal oxide sol to a point where gelation occurs (R. K. Iler, Colloid Chemistry of Silica and Silicates, 1954, chapter 6; R. K. Iler, The Chemistry of Silica, 1979, chapter s, C. J. Brinker and G. W. Scherer, Sol-Gel Science, 1990, chapters 2 and 3). Suitable materials for forming inorganic aerogels are oxides of most of the metals that can form oxides, such as silicon, aluminum, titanium, zirconium, hafnium, yttrium, vanadium, and the like. Particularly preferred are gels formed primarily from alcohol solutions of hydrolyzed silicate esters due to their ready availability and low cost (alcogel).

In another preferred embodiment, the organic aerogels can be made from polyacrylates, polystyrenes, polyacrylonitriles, polyurethanes, polyimides, polyfurfural alcohol, phenol furfuryl alcohol, melamine formaldehydes, resorcinol formaldehydes, cresol formaldehyde, phenol formaldehyde, polyvinyl alcohol dialdehyde, polycyanurates, polyacrylamides, various epoxies, agar, agarose, and the like (see for instance C. S. Ashley, C. J. Brinker and D. M. Smith, Journal of Non-Crystalline Solids, volume 285, 2001). However, as insulating articles at high temperatures in oxygen-containing atmospheres, these materials can burn away and are thus not preferred for this invention.

In another preferred embodiment, the inorganic aerogel is formed by the hydrolysis and condensation of an appropriate metal alkoxide.

In another preferred embodiment, the metal alkoxides are those having about 1 to 6 carbon atoms, more preferably from 1-4 carbon atoms, in each alkyl group.

In another preferred embodiment, the metal alkoxides are selected from tetraethoxysilane (TEOS), tetramethoxysilane (TMOS), tetra-n-propoxysilane, aluminum isopropoxide, aluminum sec-butoxide, cerium isopropoxide, hafnium tert-butoxide, magnesium aluminum isopropoxide, yttrium isopropoxide, titanium isopropoxide, zirconium isopropoxide or any combination thereof.

In another preferred embodiment, the silica precursors such as tetraethoxysilane (TEOS), tetramethoxysilane (TMOS), tetra-n-propoxysilane, 1 ,1 ,1-trimethyl-N-(trimethylsilyl)-silanamine these materials can be partially hydrolyzed and stabilized at low pH as polymers of polysilicic acid esters such as polydiethoxysiloxane (PDEOS). These materials are commercially available in alcohol solution (for example Silbond® 40, 40% silica content, Silbond Corporation). Pre-polymerized silica precursors are especially preferred for the aerogel composite (B).

In another preferred embodiment, the suitable materials for use in forming the aerogels at lower temperature are the non-refractory metal alkoxides that form oxides such as silicon and magnesium as well as mixtures thereof. For higher temperature applications, suitable alkoxides are generally refractory metal alkoxides which form oxides such as zirconia, yttria, hafnia, alumina, titania, ceria, and the like. The mixtures of non-refractory metals with refractory metals, such as silicon and/or magnesium with aluminum, may also be used. An advantage of using more than one metal oxide matrix material for the aerogel structure is an enhancement of IR opacification, achieved by providing chemical functional groups that absorb radiation at a wider range of wavelengths.

In another preferred embodiment, the reinforcing phase consists primarily of a lofty fibrous material, preferably a combination of the lofty batting and one or more fibrous materials of significantly different thickness, length, and/or aspect ratio. A preferred combination of a two fibrous material system is produced when a short, high aspect ratio microfiber (one fibrous material) dispersed throughout an aerogel matrix that penetrates a continuous lofty fiber batting (the second fibrous material).

In another preferred embodiment, the lofty batting is defined as a fibrous material that shows the properties of bulk and some resilience (with or without full bulk recovery). The preferred form is a soft web of this material. The batting preferably refers to layers or sheets of a fibrous material.

In another preferred embodiment, the reinforcing fibrous material used in the composite (B) is one or more layers of a lofty fibrous batting. The use of a lofty batting reinforcement minimizes the volume of unsupported aerogel while avoiding substantial degradation of the thermal performance of the aerogel. While generally a “batting” is a product resulting from carding or Garnetting fiber to form a soft web of fiber in sheet form, “batting” also includes webs in non-sheet form, e.g. the Primaloft® products from Albany International, provided that they are sufficiently open to be “lofty.” Batting commonly refers to a fibrous material commonly used for lining quilts or for stuffing or packaging or as a blanket of thermal insulation. Suitable fibers for producing the batting are relatively fine, generally having deniers < 15, preferably deniers < 10. The softness of the web is a byproduct of the relatively fine, multi-directionally oriented fibers that are used to make the fiber web.

In another preferred embodiment, the batting is “lofty” for purposes of presently claimed invention if it contains sufficiently few individual filaments (or fibers) that it does not significantly alter the thermal properties of the composite (B) as compared to a non-reinforced aerogel body of the same material. Generally, this would mean that upon looking at a cross-section of a final aerogel composite, the cross- sectional area of the fibers > 10% of the total surface area of that cross section, preferably > 8%, and most preferably > 5%. In another preferred embodiment, the cross-sectional area of the fibers is in the range of 0.1 > 10% of the total surface area of that cross section; more preferably the cross-sectional area of the fibers is in the range of 0.5 > 8 % of the total surface area of that cross section, even more preferably the cross-sectional area of the fibers is in the range of 0.5 > 6 % of the total surface area of that cross section; and most preferably the cross-sectional area of the fibers is in the range of 1 > 5 % of the total surface area of that cross section.

In another preferred embodiment, the lofty fibrous batting is made from fibers having a diameter in the range of 0.1 to 100 pm., more preferably 0.1 to 80 pm, 0.5 to 70 pm, most preferably 1 to 60 pm, and in particular 5 to 50 pm.

In another preferred embodiment, the lofty batting preferably has a thermal conductivity < 50 mW/m.K at room temperature and pressure to facilitate the formation of the low thermal conductivity aerogel composites.

Another way of determining if a batting is sufficiently lofty to be within the scope of this invention is to evaluate its compressibility and resilience. In another preferred embodiment, the lofty batting is one that (i) is compressible by at least 50% of its natural thickness, preferably at least 65%, most preferably at least 75%, and in particular preferably at least 80 % and (ii) is sufficiently resilient that after compression for a few seconds it will return to at least 70% of its original thickness, preferably at least 75%, and most preferably at least 80%. By this definition a lofty batting is one that can be compressed to remove the air (bulk) yet spring back to substantially its original size and shape. For example, a Holofil™ batting may be compressed from its original 1.5" thickness to a minimum of about 0.2" and spring back to its original thickness once the load is removed. This batting can be considered to contain 1.3" of air (bulk) and 0.2" of fiber. It is compressible by 87% and returns to essentially 100% of its original thickness. Fiberglass batting used may be compressed to a similar extent and springs back to about 80% of its original thickness but does that quite slowly.

In another preferred embodiment, the batting retains at least 50% of its thickness after the gel forming liquid is poured in.

In another preferred embodiment, the fiber reinforcements used in composite (B) that tend to run along the z axis, (in the direction of the heat flow) will significantly increase the thermal conductivity of the resulting composite by acting as thermal conduits. A batting that has highly aligned (straight) fibers, particularly in the x-y horizontal plane is stiffer than a typical lofty batting of the same density with bent or crimped fibers running in all three axes. In order to minimize heat flow in the z direction the batting should have low heat flow along the z axis (in the direction of the heat flow). Thus, a suitable batting has a high enough quantity of fibers oriented along the z axis to maintain loft, yet not so great a quantity that the insulating properties of the resulting composite are compromised by these fibers. The fibers along the z axis may be of a different material, preferably one with lower thermal conductivity than those in the x and y axes. The z axis fibers may also be made more circuitous, so that they present a more tortuous path for heat conduction than do the fibers in the x-y direction. The same fiber materials and methods may be used throughout the batting in an attempt to minimize thermal conduction in all axes, but in many insulating applications, however, it is heat flow in a specific direction that is being addressed, and using such materials and methods may compromise the flexibility of the resulting composite. In another preferred embodiment, the ideal lofty batting is one with fine, crimped fibers, evenly dispersed throughout the composite(B).

In another preferred embodiment, the composite (B) further comprises microfiber.

While the composite (B) produced with a lofty batting is flexible, durable, has a low thermal conductivity and has a good resistance to sintering, the performance of the aerogel composite may be substantially enhanced by incorporating randomly distributer microfibers into the composite, particularly microfibers that will help resist sintering while increasing durability and decreasing dusting. The effect of microfiber on the performance of a composite will depend on a number of variables, such as fiber alignment, diameter, length, aspect ratio (fiber length/fiber diameter), strength, modulus, strain to failure, coefficient of thermal expansion, and the strength of the interface between the fiber and the matrix. The microfibers are incorporated into the composite by dispersing them in the gel precursor liquid and then using that liquid to infiltrate the lofty batting.

In another preferred embodiment, aspect ratio of the microfiber is defined as the ratio of microfiber length to microfiber diameter.

In another preferred embodiment, the microfibers have the diameter in the range from 0.1 to 100 pm, have high aspect ratios L/d > 5, preferably L/d>100, and are relatively uniformly distributed throughout the composite(B). Since higher aspect ratios improve composite performance, the longest microfibers possible are desired. However, the length of the fibers used herein is constrained to avoid or at least minimize any filtration by the chosen lofty batting has when a microfiber-containing gel precursor is infused into the batting. The microfibers should be short enough to minimize filtration by the lofty batting and long enough to have the maximum possible effect on the thermal and mechanical performance of the composite(B). The microfibers preferably have a thermal conductivity of < 200 mW/m.K to facilitate the formation of low thermal conductivity aerogel composites.

In another preferred embodiment, the lofty fibrous batting are microfibers fibers evenly dispersed throughout the composite.

When the microfibers are dispersed in a sol, they often will rapidly settle. To overcome this problem, a suspension or dispersion agent that will not deleteriously affect the gel formation should be added to the sol. In another preferred embodiment, the suspension/dispersion agents include solutions of high molecular weight block copolymers with pigment affinic groups (Disperbyk-184 and 192 from BYK- Chemie), and the like. The agents need to be effective during at least the period of time between the dispersion of the microfiber in the gel precursor and the gelation of the sol.

The quantity, type, and/or size and aspect ratio of the microfibers used within a specific aerogel composite may be varied to meet specific tasks. For example, an application may involve insulating regions of different temperatures using a continuous aerogel composite; the composite may be made such that more microfibers will be present in the areas of the composite (B) that will contact the higher temperature regions. Similarly, different microfibers (e.g. different material, different aspect ratio, size) may be incorporated in such areas for best insulation performance. Such microfiber modification may be accomplished by using a variety of suspension agents and/or microfibers to cause the microfibers to settle into the composite at different rates and thus in different locations.

In another preferred embodiment, the suitable fibrous materials for forming both the lofty batting and the microfibers include any fiber-forming material selected from fiberglass, quartz, polyester (PET), polyethylene, polypropylene, polybenzimidazole (PBI), polyphenylenebenzo-bisoxasole (PBO), polyetherether ketone (PEEK), polyarylate, polyacrylate, polytetrafluoroethylene (PTFE), poly-metaphenylene diamine (Nomex), poly-paraphenylene terephthalamide (Kevlar), ultra-high molecular weight polyethylene (UHMWPE) e.g. Spectra™, novoloid resins (Kynol), polyacrylonitrile (PAN), PAN/carbon, carbon fibers or any combination thereof.

In another preferred embodiment, the same fibrous material may be used in both the batting and the microfibers for the preparation of the composite (B).

In another preferred embodiment, a combination of different fibrous materials may be utilized in both the batting and the microfibers for the preparation of the composite (B). In another preferred embodiment, one such combination is a lofty fiberglass batting with carbon microfibers distributed throughout.

In another preferred embodiment, the combination of batting and microfiber reinforcement has been found to enhance sintering resistance. This may be accomplished by incorporating microfibers of a suitable material, e.g. carbon filaments, within the gel precursor (generally in combination with a suitable non-reactive dispersing agent) prior to pouring the gel precursor onto the fibrous batting. FIG. 5 is an exploded view of such an aerogel composite where the composite is reinforced on both a macro level with a fibrous batting 51 and on a micro level with carbon fiber filaments 52. When dispersed in a silica matrix, carbon microfibers provide a combination of IR opacification and microscale strengthening that give a non-refractory metal oxide such as silica greatly improved thermal and mechanical performance at higher temperatures relative to non-strengthened and opacified silica.

In another embodiment of this invention, the lofty reinforcing fibrous batting is used in the form of a multi-layer laminate as shown in FIGS. 3, 4, and 6. In addition to including fibrous material batting, the laminates may include layers of materials which will help provide specific characteristics to the final composite (B) structure. For example, the inclusion of a metal layer in the x-y plane, such as a copper mesh, can improve x-y thermal and/or electrical conductivity, RFI-EMI attenuation, the ability to anchor the composite (B) to a support structure, and/or provide additional physical strength. While any metal can be used to produce the metal mesh, copper and stainless steel are currently preferred. Suitable meshes will be made from wires having diameters ranging from about 0.001 to 0.1 inches, preferably about 0.01 to 0.05, and the wire spacing may range from as tight as a window screen to 0.3 inches. When the additional layer is of a high (>1 W/m.K) thermal conductivity material such as a carbon fiber, silicon carbide, or a metal, the resulting composite (B) has been found to exhibit a significantly enhanced ability to rapidly dissipate heat throughout the x-y plane of a multilayer composite, further improving the durability of the composite under a high heat load.

FIG. 3 shows three layers of laminate consisting of a layer of lofty fiber batting 32, a fine copper mesh 31 , and a second layer of lofty fiber batting 32. FIG. 4 shows another three layers of laminate, a layer of lofty fiber batting 42, a woven carbon fiber textile 41 , and a second layer of fiber batting 42. While these laminates are shown to be symmetric, this is preferred and not mandatory.

FIG. 6 is an exploded view of a laminate consisting of a layer of fiber batting 61 , a layer of silicon carbide felt 62, a fine copper mesh 63, a layer of silicon carbide felt 62, and a layer of fiber batting 61 . In another preferred embodiment, the lofty fibrous batting consists essentially of fibers having a thermal conductivity < 50 mW/m.K as determined according to ASTM C 177.

In another preferred embodiment, the lofty fibrous batting consists essentially of fibers having a thermal conductivity < 50 mW/m.K, more preferably thermal conductivity < 45 mW/m.K, even more preferably thermal conductivity < 40 mW/m.K, most preferably thermal conductivity < 30 mW/m.K, and in particular thermal conductivity < 20 mW/m.K, as determined according to ASTM C 177.

In another preferred embodiment, the composite (B) comprises at least one dopant (B3).

In another preferred embodiment, the dopant (B3) is selected from carbon black, titania, iron oxides, silicon carbide, molybdenum silicide, manganese oxides, or polydialkylsiloxanes wherein the alkyl groups contain 1 to 4 carbon atoms.

In another preferred embodiment, the dopant is present in an amount of 1 to 20% by weight of the total weight of the composite (B), more preferably the dopant is present in an amount of 1 to 15% by weight of the total weight of the composite (B), most preferably the dopant is present in an amount of 2 to 12% by weight of the total weight of the composite (B), and in particular the dopant is present in an amount of 5 to 10% by weight of the total weight of the composite (B).

In another preferred embodiment, the reinforced aerogel composition has a density at 20 °C in the range of 0.15 and 0.40 g/cm³; more preferably a density at 20 °C in the range of 0.15 and 0.35 g/cm³; and most preferably a density at 20 °C in the range of 0.20 and 0.35 g/cm³.

In another preferred embodiment, the composite (B) comprises at least one reinforcing structure (B1 ) and at least one aerogel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet; more preferably the composite (B) comprises at least one reinforcing structure (B1) and at least one aerogel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and/ or microfiber and a continuous aerogel (B2) through said batting/sheet/mi- crofiber, wherein he microfiber dispersed throughout the aerogel (B2); most preferably the composite (B) comprises at least one reinforcing structure (B1 ) and at least one aerogel(B2); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting and/or microfiber and a continuous aerogel (B2) through said batting/microfiber, wherein the microfiber dispersed throughout the aerogel (B2); and in particular the composite (B) comprises at least one reinforcing structure (B1 ) and at least one aero- gel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and microfiber and a continuous aerogel (B2) through said batting/ microfiber, wherein the microfiber dispersed throughout the aerogel (B2). In another preferred embodiment, the composite (B) comprises at least one reinforcing structure (B1 ) and a silica aerogel(B2); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and a continuous silica aerogel (B2) through said batting/sheet; more preferably the composite (B) comprises at least one reinforcing structure (B1 ) and a silica aero- gel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and/ or microfiber; and a continuous silica aerogel (B2) through said bat- ting/sheet/microfiber, wherein the microfiber is dispersed throughout the silica aerogel (B2), wherein the lofty fibrous batting and the microfiber are same or different; most preferably the composite (B) comprises at least one reinforcing structure (B1) and a silica aero- gel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or microfiber; and a continuous silica aerogel (B2) through said batting/microfiber, wherein the microfiber dispersed throughout the silica aerogel (B2)and the lofty fibrous batting and the microfiber are same or different; and in particular the composite (B) comprises at least one reinforcing structure (B1 ) and a silica aerogel(B2); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting and microfiber; and a continuous silica aerogel (B2) through said batting/ microfiber, wherein the microfiber dispersed throughout the silica aerogel (B2)and the lofty fibrous batting and the microfiber are same or different.

In another preferred embodiment, the composite (B) comprises at least one reinforcing structure (B1 ) and a silica aerogel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting, microfiber and an organic or an inorganic sheet; wherein the organic sheet is selected from thermosetting or thermoplastic sheet and the inorganic sheet is a metal sheet; more preferably the composite (B) comprises at least one reinforcing structure (B1 ) and a silica aero- gel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting, microfiber and an inorganic sheet; wherein the inorganic sheet is a metal sheet; and most preferably the composite (B) comprises at least one reinforcing structure (B1) and a silica aerogel(B2); wherein the reinforcing structure (B1) comprises lofty fibrous batting, microfiber and a metal sheet.

In another preferred embodiment, the binder (C) is selected from an organic binder, inorganic binder or combination thereof.

In another preferred embodiment, the organic binder is a polyurethane resin composition.

In another preferred embodiment, the polyurethane resin composition comprises:

(a) at least one isocyanate, and

(b) at least one isocyanate reactive component, wherein (a) and (b) are present at an isocyanate index in the range of 100 to 180.; more preferably the polyurethane resin composition comprises: (a) at least one isocyanate, and

(b) at least one isocyanate reactive component, wherein (a) and (b) are present at an isocyanate index in the range of 110 to 170; and most preferably the polyurethane resin composition comprises:

(a) at least one isocyanate, and

(b) at least one isocyanate reactive component elected from polyamine or polyol, wherein (a) and (b) are present at an isocyanate index in the range of 120 to 160.

In another preferred embodiment, the isocyanate index is in the range of 120 to 160.

In another preferred embodiment, the isocyanate is aromatic isocyanate or an aliphatic isocyanate.

In another preferred embodiment, the isocyanate comprises at least one aromatic isocyanate selected from toluene diisocyanate; polymeric toluene diisocyanate, polymeric toluene diisocyanate, polymeric methylene diphenyl diisocyanate; 1 ,5-naphthalene diisocyanate; methylene diphenyl diisocyanate; polymeric methylene diphenyl diisocyanate; m-phenylene diisocyanate; 1 ,5-naphthalene diisocyanate; 4- chloro-1 ; 3-phenylene diisocyanate; 2,4,6-toluylene tri isocyanate, 1 ,3-diisopropylphenylene-2,4-diiso- cyanate; 1-methyl-3,5-diethylphenylene-2,4-diisocyanate; 1 ,3,5-triethylphenylene-2,4-diisocyanate;

1 .3.5-triisoproply-phenylene-2,4-diisocyanate; 3,3'-diethyl-bisphenyl-4,4'-diisocyanate; 3,5,3',5'-tetrae- thyl-diphenylmethane-4,4'-diisocyanate; 3,5,3',5'-tetraisopropyldiphenylmethane-4,4'-diisocyanate; 1- ethyl-4-ethoxy-phenyl-2,5-diisocyanate; 1 ,3,5-triethyl benzene-2,4,6-triisocyanate; 1-ethyl-3,5-diisopro- pyl benzene-2,4,6-triisocyanate, tolidine diisocyanate, 1 ,3,5-triisopropyl benzene-2,4,6-triisocyanate or mixtures thereof; more preferably the aromatic isocyanate is selected from toluene diisocyanate; polymeric toluene diisocyanate, methylene diphenyl diisocyanate; polymeric methylene diphenyl diisocyanate, m-phenylene diisocyanate; 1 ,5-naphthalene diisocyanate; 4-chloro-1 ; 3-phenylene diisocyanate;

2.4.6-toluylene triisocyanate, 1 ,3-diisopropylphenylene-2,4-diisocyanate, 1-methyl-3,5-dieth- ylphenylene-2,4-diisocyanate or mixture thereof; even more preferably the aromatic isocyanate is selected from toluene diisocyanate; polymeric toluene diisocyanate, methylene diphenyl diisocyanate; polymeric methylene diphenyl diisocyanate, m-phenylene diisocyanate and 1 ,5-naphthalene diisocyanate or a combination thereof; most preferably the aromatic isocyanate is selected from toluene diisocyanate; polymeric toluene diisocyanate, methylene diphenyl diisocyanate and polymeric methylene diphenyl diisocyanate, and in particular the aromatic isocyanate comprises methylene diphenyl diisocyanate and/or polymeric methylene diphenyl diisocyanate or mixtures thereof.

In another preferred embodiment, the aromatic isocyanate selected from methylene diphenyl diisocyanate, polymeric methylene diphenyl diisocyanate or combination thereof.

In another preferred embodiment, the methylene diphenyl diisocyanate is available in three different isomeric forms, namely 2,2'-methylene diphenyl diisocyanate (2,2'-MDI), 2,4'-methylene diphenyl diisocyanate (2,4'-MDI) and 4,4'-methylene diphenyl diisocyanate (4,4'-MDI). Methylene diphenyl diisocyanate can be classified into monomeric methylene diphenyl diisocyanate and polymeric methylene di- phenyl diisocyanate referred to as technical methylene diphenyl diisocyanate. Polymeric methylene diphenyl diisocyanate includes oligomeric species and methylene diphenyl diisocyanate isomers. Thus, polymeric methylene diphenyl diisocyanate may contain a single methylene diphenyl diisocyanate isomer or isomer mixtures of two or three methylene diphenyl diisocyanate isomers, the balance being oligomeric species. Polymeric methylene diphenyl diisocyanate tends to have isocyanate functionalities of higher than 2. The composite article according to isomeric ratio as well as the amount of oligomeric species can vary in wide ranges in these products. For instance, polymeric methylene diphenyl diisocyanate may typically contain 30 wt.-% to 80 wt.-% of methylene diphenyl diisocyanate isomers, the balance being said oligomeric species. The methylene diphenyl diisocyanate isomers are often a mixture of 4,4'-methylene diphenyl diisocyanate, 2,4'-methylene diphenyl diisocyanate and very low levels of 2,2'-methylene di-phenyl diisocyanate.

In addition, reaction products of polyisocyanates with polyhydric polyols and their mixtures with other diisocyanates and polyisocyanates can also be used.

In another preferred embodiment, the isocyanate comprises a polymeric methylene diphenyl diisocyanate. Commercially available isocyanates available under the tradename, such as, but not limited to, Lupranat® from BASF can also be used for the purpose of the present invention.

In another preferred embodiment, the aliphatic isocyanate selected from isophorone diisocyanate, pro- pylene-1 ,2-diisocyanate, propylene-1 ,3-diisocyanate, butylene-1 ,2-diisocyanate, butylene-1 ,3-diisocy- anate, hexamethylene-1 ,6-diisocyanate, 2-methylpentamethylene-1 ,5-diisocyanate, 2-ethylbutylene- 1 ,4-diisocyanate, 1 ,5-pentamethylene diisocyanate, ethyl ester l-lysine triisocyanate, 1 ,6,11-triisocya- natoundecane, (2,4,6-trioxotriazine-1 ,3,5(2h,4h,6h)-triyl)tris(hexamethylene) isocyanate, methyl-2,6- diisocyanate caproate, octamethlyene-1 ,8-diisocyanate, 2,4,4-trimethylhexamethylene-1 ,6-diisocya- nate, nonamethylene diisocyanate, 2,2,4-trimethylhexamethylene-1 ,6-diisocyanate, decamethylene- 1 ,10-diisocyanate, 2,11-diisocyanato-dodecane, triphenylmethane-4,4’,4”-triisocyanate, toluene-2,4,6- triyl triisocyanate, tris(isocyanatohexyl)biuret, trimethylcyclohexyl] triisocyanate, 2,4,4'-triisocyanato-di- cyclohexylmethane, 2,2,-methylene-bis(cyclohexyl isocyanate), 3,3'-methylene-bis(cyclohexyl isocyanate), 4,4'-methylene-bis(cyclohexyl isocyanate), 4,4'-ethylene-bis(cyclohexyl isocyanate), 4,4'-propyl- ene-bis-(cyclohexyl isocyanate), bis(paraisocyano-cyclohexyl)sulfide, bis(para-isocyanato-cyclo- hexyl)sulfone, bis(para-isocyano-cyclohexyl)ether, bis(para-isocyanato-cyclohexyl)diethyl silane, bis(para-isocyanato-cyclohexyl)diphenyl silane, bis(para-isocyanato-cyclohexyl)ethyl phosphine oxide, bis(para-isocyanato-cyclohexyl)phenyl phosphine oxide, bis(para-isocyanato-cyclohexyl)N-phenyl amine, bis(para-isocyanato-cyclohexyl)N-methyl amine,3,3-diisocyanato adamantane, 3,3-diisocyano biadamantane, 3,3-diiso-cyanatoethyl-1'-biadamantane, 1 ,2-bis (3-isocyanato-propoxy)ethane, 2,2-di- methyl propylene diisocyanate, 3-methoxy hexamethylene-1 ,6-diisocyanate, 2,5-dimethyl heptamethylene diisocyanate, 5-methyl nonamethylene-1 ,9-diisocyanate, 1 ,4-diisocyanato cyclohexane, 1 ,2- diisocyanato octadecane, 2,5-diisocyanato-1 ,3,4-oxadiazole, OCN(CH2)3O(CH2)2O(CH2)3NCO and OCN(CH2)3N(CH3)(CH2)3NCO or polymeric forms of diisocyanates.; more preferably the aliphatic isocyanate selected from isophorone diisocyanate, propylene-1 ,2-diisocyanate, propylene-1 ,3- diisocyanate, butylene-1 ,2-diisocyanate, butylene-1 ,3-diisocyanate, hexamethylene-1 ,6-diisocyanate, 2-methylpentamethylene-1 ,5-diisocyanate1 ,5-pentamethylene diisocyanate, 1 ,6,11-triisocya- natoundecane, methyl-2,6-diisocyanate caproate, octamethlyene-1 ,8-diisocyanate, 2,4,4-trimethylhex- amethylene-1 ,6-diisocyanate, nonamethylene diisocyanate, 2,2,4-trimethylhexamethylene-1 ,6-diisocy- anate, decamethylene-1 ,10-diisocyanate, 2,11-diisocyanato-dodecane or polymeric forms of diisocyanates; and most preferably the aliphatic isocyanate selected from isophorone diisocyanate, hexameth- ylene-1 ,6-diisocyanate, 2-methylpentamethylene-1 ,5-diisocyanate, 1 ,5-pentamethylene diisocyanate, 1 octamethlyene-1 ,8-diisocyanate, 2,4,4-trimethylhexamethylene-1 ,6-diisocyanate, nonamethylene diisocyanate, 2,2,4-trimethylhexamethylene-1 ,6-diisocyanate, decamethylene-1 ,10-diisocyanate, 2,11- diisocyanato-dodecane and polymeric forms of diisocyanates or mixtures thereof.

In another preferred embodiment, the isocyanate reactive component is a polyol having an average functionality in the range of 2.0 to 8.0.

In another preferred embodiment, the polyol has hydroxyl number in the range of 15 mg KOH/g to 1800 mg KOH/g as determined according to the standard acetic anhydride method.

In one embodiment, the compounds being reactive towards isocyanate and having a molecular weight of 400 g/mol or more are compounds having hydroxyl groups, also referred to as polyol. Suitable polyols have an average functionality preferably in the range of 2.0 to 8.0, or in the range of 2.0 to 6.5, or in the range of 2.5 to 6.5 and the hydroxyl number preferably in the range of 15 mg KOH/g to 1800 mg KOH/g, or more preferably in the range of 15 mg KOH/g to 1500 mg KOH/g, and most preferably in the range of 100 mg KOH/g to 1500 mg KOH/g, and in particular the hydroxyl number in the range of 500 to 1200 mg KOH/g. The compounds that are reactive towards isocyanate can be present in the polyurethane resin composition in amounts preferably in the range of 1 wt.-% to 99 wt.-%, based on the total weight of the polyurethane resin composition.

In one embodiment, the polyols are selected from polyether polyols, polyester polyols, polyether-ester polyols or a combination thereof.

In another embodiment, the polyol comprises polyether polyols. In yet another embodiment, the polyol comprises a mixture of polyether polyols and polyester polyols.

In another preferred embodiment, the polyether polyols, according to the invention, have an average functionality in the range of 2.0 to 8.0, more preferably in the range of 2.5 to 6.5, most preferably in the range of 2.5 to 5.5, and the hydroxyl number in the range of 15 mg KOH/g to 1500 mg KOH/g, more preferably in the range of 100 mg KOH/g to 1500 mg KOH/g, and most preferably in the range of 250 mg KOH/g to 1000 mg KOH/g.

In another embodiment, the polyether polyols are obtainable by known methods, for example by anionic polymerization with alkali metal hydroxides, e.g., sodium hydroxide or potassium hydroxide, or alkali metal alkoxides, e.g., sodium methoxide, sodium ethoxide, potassium ethoxide or potassium isopropox- ide, as catalysts and by adding at least one amine-containing starter molecule, or by cationic polymerization with Lewis acids, such as antimony pentachloride, boron fluoride etherate and so on, or fuller’s earth, as catalysts from one or more alkylene oxides having 2 to 4 carbon atoms in the alkylene moiety.

Starter molecules are generally selected such that their average functionality is preferably in the range of 2.0 to 8.0, and most preferably in the range of 3.0 to 8.0. Optionally, a mixture of suitable starter molecules is used.

Starter molecules for polyether polyols include amine containing and hydroxyl-containing starter molecules. Suitable amine containing starter molecules include, for example, aliphatic and aromatic diamines such as ethylenediamine, propylenediamine, butylenediamine, hexamethylenediamine, phenylenediamines, toluenediamine, diaminodiphenylmethane and isomers thereof.

Other suitable starter molecules further include alkanolamines, e.g. ethanolamine, N-methylethanola- mine and N-ethylethanolamine, dialkanolamines, e.g., diethanolamine, N-methyldiethanolamine and N- ethyldiethanolamine, and trialkanolamines, e.g., triethanolamine, and ammonia.

Suitable amine containing starter molecules are selected from ethylenediamine, phenylenediamines, toluenediamine or isomers thereof. In one embodiment, it is ethylenediamine.

Hydroxyl-containing starter molecules are selected from sugars, sugar alcohols, for e.g. glucose, mannitol, sucrose, pentaerythritol, sorbitol; polyhydric phenols, resols, e.g., oligomeric condensation products formed from phenol and formaldehyde, trimethylolpropane, glycerol, glycols such as ethylene glycol, propylene glycol and their condensation products such as polyethylene glycols and polypropylene glycols, e.g., diethylene glycol, triethylene glycol, dipropylene glycol, and water or a combination thereof.

Suitable hydroxyl containing starter molecules are selected from sugar and sugar alcohols such as sucrose, sorbitol, glycerol, pentaerythritol, trimethylolpropane or mixtures thereof. In some embodiments the hydroxyl containing starter molecules are selected from sucrose, glycerol, pentaerythritol or trimethylolpropane.

Suitable alkylene oxides having 2 to 4 carbon atoms are, for example, ethylene oxide, propylene oxide, tetrahydrofuran, 1 ,2-butylene oxide, 2,3-butylene oxide and styrene oxide. Alkylene oxides can be used singly, alternatingly in succession or as mixtures. In one embodiment, the alkylene oxides are propylene oxide and/or ethylene oxide. In some embodiments, the alkylene oxides are mixtures of ethylene oxide and propylene oxide that comprise more than 50 wt.-% of propylene oxide. In another preferred embodiment, the amount of the polyether polyols is in the range of 1 wt.-% to 99 wt.-%, based on the total weight of the polyurethane resin composition, more preferably in the range of 20 wt.-% to 99 wt.-%, and most preferably the range of 40 wt.-% to 99 wt.-%.

In another preferred embodiment, the suitable polyester polyols have an average functionality in the range of 2.0 to 6.0, more preferably in the range of 2.0 to 5.0, and most preferably in the range of 2.0 to 4.0 and a hydroxyl number in the range of 30 mg KOH/g to 250 mg KOH/g, and most preferably in the range of 100 mg KOH/g to 200 mg KOH/g.

In another preferred embodiment, the polyester polyols are based on the reaction product of carboxylic acids or anhydrides with hydroxy group containing compounds. Suitable carboxylic acids or anhydrides have preferably from 2 to 20 carbon atoms, or from 4 to 18 carbon atoms, for example succinic acid, glutaric acid, adipic acid, suberic acid, azelaic acid, sebacic acid, decanedicarboxylic acid, maleic acid, fumaric acid, phthalic acid, isophthalic acid, terephthalic acid, oleic acid, phthalic anhydride. Particularly comprising of phthalic acid, isophthalic acid, terephthalic acid, oleic acid and phthalic anhydride or a combination thereof.

Suitable hydroxyl containing compounds are selected from ethanol, ethylene glycol, propylene-1 ,2-gly- col, propylene-1 ,3-glycol, butyl-ene-1 ,4-glycol, butylene-2,3-glycol, hexane-1 ,6-diol, octane-1 ,8-diol, neopentyl glycol, cyclohexane dimethanol (1 ,4-bis-hydroxy-methylcyclohexane), 2-methyl-propane-

1 .3-diol, glycerol, trimethylolpropane, hex-ane-1 ,2,6-triol, butane -1 ,2, 4-triol, trimethylolethane, pentaerythritol, quinitol, mannitol, sorbitol, methyl glycoside, diethylene glycol, triethylene glycol, tetraethylene glycol, polyethylene glycol, dipropylene glycol, polypropylene glycol, polyethylene-propylene glycol, dibutylene glycol or polybutylene glycol. In one embodiment, the hydroxyl containing compound is selected from ethylene glycol, propylene-1 , 2-glycol, propylene-1 ,3-glycol, butyl-ene-1 ,4-glycol, butylene-

2.3-glycol, hexane-1 ,6-diol, octane-1 ,8-diol, neopentyl glycol, cyclohexane dimethanol (1 ,4-bis-hy- droxy-methylcyclohexane), 2-methyl-propane-1 ,3-diol, glycerol, trimethylolpropane, hexane-1 , 2, 6-triol, butane -1 ,2, 4-triol, trimethylolethane, pentaerythritol, quinitol, mannitol, sorbitol, methyl glycoside or diethylene glycol. In another embodiment, the hydroxyl containing compound is selected from ethylene glycol, propylene-1 , 2-glycol, propylene-1 ,3-glycol, butyl-ene-1 ,4-glycol, butylene-2,3-glycol, hexane- 1 ,6-diol, octane-1 ,8-diol, neopentyl glycol or diethylene glycol. In still another embodiment, the hydroxyl containing compound is selected from hexane-1 , 6-diol, neopentyl glycol or diethylene glycol.

Suitable polyether-ester polyols have a hydroxyl number in the range of 100 mg KOH/g to 460 mg KOH/g, more preferably in the range of 150 mg KOH/g to 450 mg KOH/g, most preferably in the range of 250 mg KOH/g to 430 mg KOH/g and in any of these embodiments may have an average functionality in the range of 2.3 to 5.0, and most preferably in the range of 3.5 to 4.7.

Such polyether-ester polyols are obtainable as a reaction product of i) at least one hydroxyl-containing starter molecule; ii) of one or more fatty acids, fatty acid monoesters or mixtures thereof; iii) of one or more alkylene oxides having 2 to 4 carbon atoms. The starter molecules of component I) are generally selected such that the average functionality of component i) is preferably 3.8 to 4.8, or from 4.0 to 4.7, or even from 4.2 to 4.6. Optionally, a mixture of suitable starter molecules is used.

Suitable hydroxyl-containing starter molecules of component i) are selected from sugars, sugar alcohols (glucose, mannitol, sucrose, pentaerythritol, sorbitol), polyhydric phenols, resols, e.g., oligomeric condensation products formed from phenol and formaldehyde, trimethylolpropane, glycerol, glycols such as ethylene glycol, propylene glycol and their condensation products such as polyethylene glycols and polypropylene glycols, e.g., diethylene glycol, triethylene glycol, dipropylene glycol, and water or a combination thereof.

In another preferred embodiment, the hydroxyl-containing starter molecules of component i) are selected from sugars and sugar alcohols such as sucrose and sorbitol, glycerol, and mixtures of said sugars and/or sugar alcohols with glycerol, water and/or glycols such as, for example, diethylene glycol, dipropylene glycol or combination thereof.

Said fatty acid or fatty acid monoester ii) is selected from polyhydroxy fatty acids, ricinoleic acid, hy- droxyl-modified oils, hydroxyl-modified fatty acids and fatty acid esters based in myristoleic acid, palmitoleic acid, oleic acid, stearic acid, palmitic acid, vaccenic acid, petroselic acid, gadoleic acid, erucic acid, nervonic acid, linoleic acid, a- and g-linolenic acid, stearidonic acid, arachidonic acid, timnodonic acid, clupanodonic acid and cervonic acid or a combination thereof. Fatty acids can be used as purely fatty acids. In this regard, preference is given to using fatty acid methyl esters such as, for example, biodiesel or methyl oleate.

Biodiesel is to be understood as meaning fatty acid methyl esters within the meaning of the EN 14214 standard from 2010. Principal constituents of biodiesel, which is generally produced from rapeseed oil, soybean oil or palm oil, are methyl esters of saturated Cw to C fatty acids and methyl esters of mono- or polyunsaturated Cis fatty acids such as oleic acid, linoleic acid and linolenic acid.

Suitable alkylene oxides iii) having 2 to 4 carbon atoms are, for example, ethylene oxide, propylene oxide, tetrahydrofuran, 1 ,2-butylene oxide, 2,3-butylene oxide and/or styrene oxide. Alkylene oxides can be used singly, alternatingly in succession or as mixtures.

In another preferred embodiment, the alkylene oxides comprise propylene oxide and ethylene oxide. In another preferred embodiment, the alkylene oxide is a mixture of ethylene oxide and propylene oxide comprising more than 50 wt.-% of propylene oxide. In another embodiment, the alkylene oxide comprises purely propylene oxide.

In another preferred embodiment, suitable chain extenders and/or cross linkers can also be present in the polyurethane resin composition, as described hereinabove. The addition of bifunctional chain extenders, trifunctional and higher-functional cross linkers or, if appropriate, mixtures thereof might be added. Chain extenders and/or cross linkers used are preferably alkanol amines and in particular diols and/or triols having molecular weights preferably in in the range of 60 g/mol to 300 g/mol. Suitable amounts of these chain extenders and/or cross linkers can be added and are known to the person skilled in the art. For instance, chain extenders and/or cross linkers can be present in an amount up to 99 wt.-%, or up to 20 wt.-%, based on the total weight of the polyurethane resin composition.

In another embodiment, commercially available compounds that are reactive towards isocyanate can also be employed, for e.g. Sovermol®, Pluracol® and Quadrol® from BASF.

In another preferred embodiment, the isocyanate reactive component is a polyether polyol.

In another preferred embodiment, the polyurethane resin composition comprises a chain extender and/or cross linker having a molecular weight in the range of 49 g/mol to 399 g/mol.

In another preferred embodiment, the polyurethane resin composition further comprises catalysts, additives and fillers.

In another preferred embodiment, the additives is selected from pigments, dyes, surfactants, graphite, graphene, flame retardants, hindered amine light stabilizers, ultraviolet light absorbers, stabilizers, defoamers, internal release agents, desiccants, blowing agents, curing agents, fire class additive and anti-static agents or a combination thereof.

In another preferred embodiment, the fire class additive is selected from the group consisting of clay materials, magnesium hydroxide, alumina trihydrate (“ATH”), metal carbonates or combination thereof.

In another preferred embodiment, the polyurethane resin composition, as described hereinabove, further comprises catalysts and additives.

Suitable catalysts for the polyurethane resin composition are well known to the person skilled in the art. For instance, tertiary amine and phosphine compounds, metal catalysts such as chelates of the em- bodimentsvarious metals, acidic metal salts of strong acids; strong bases, alcoholates and phenolates of various metals, salts of organic acids with a variety of metals, organometallic derivatives of tetravalent tin, trivalent and pentavalent As, Sb and Bi and metal carbonyls of iron and cobalt and mixtures thereof can be used as catalysts.

Suitable tertiary amines include, such as triethylamine, tributylamine, N-methylmorpholine, N-ethylmor- pholine, N,N, N', N'-tetramethylethylenediamine, pentamethyl-diethylenetriamine and higher homologues (as described in, for example, DE-A 2,624,527 and 2,624,528), 1 ,4-diazabicyclo(2.2.2)octane, N-methyl-N'-dimethyl-aminoethylpiperazine, bis-(dimethylaminoalkyl)piperazines, tris(dimethyla- minopropyl)hexahydro-1 ,3,5-triazin, N,N-dimethylbenzylamine, N,N-dimethylcyclohexylamine, N,N- diethyl-benzylamine, bis-(N,N-diethylaminoethyl) adipate, N,N,N',N'-tetramethyl-1 ,3-butanediamine, N,N-dimethyl-p-phenylethylamine, 1 ,2-dimethylimidazole, 2-methylimidazole, monocyclic and bicyclic amines together with bis-(dialkylamino)alkyl ethers, such as 2, 2-bis-(dimethylaminoethyl)ether. Triazine compounds, such as, but not limited to 33, wherein, tris(dimethylaminopropyl)hexahydro-1 ,3,5-triazin can also be used.

Suitable metal catalysts include metal salts and organometallics comprising tin-, titanium-, zirconium-, hafnium , bismuth-, zinc-, aluminium- and iron compounds, such as tin organic compounds, preferably tin alkyls, such as dimethyltin or diethyltin, or tin organic compounds based on aliphatic carboxylic acids, preferably tin diacetate, tin dilaurate, dibutyl tin diacetate, dibutyl tin dilaurate, bismuth compounds, such as bismuth alkyls or related compounds, or iron compounds, preferably iron-(ll)-acetylacetonate or metal salts of carboxylic acids, such as tin-ll-isooctoate, tin dioctoate, titanium acid esters or bismuth- (lll)-neodecanoate or a combination thereof.

The catalysts, as described hereinabove, can be present in amounts preferably up to 20 wt.-% based on the total weight of the polyurethane resin composition.

In another preferred embodiment, the additives is selected from pigments, dyes, surfactants, graphite, graphene, flame retardants, hindered amine light stabilizers, ultraviolet light absorbers, stabilizers, defoamers, internal release agents, desiccants, blowing agents, curing agents, fire class additive, antistatic agents or a combination thereof. Further details regarding additives can be found, for example, in the Kunststoffhandbuch, Volume 7, “Polyurethane” Carl-Hanser-Verlag Munich, 1st edition, 19662nd edition, 1983 and 3rd edition, 1993. Suitable amounts of these additives are well known to the person skilled in the art. However, for instance, the additives can be present in amounts up to 20 wt.-% based on the total weight of the polyurethane resin composition.

In another preferred embodiment, the polyurethane resin composition, as described hereinabove, can also comprise a reinforcing agent. Suitable reinforcing agents refer to fillers in the present context.

Suitable fillers include, such as, but not limited to, silicatic minerals, examples being finely ground quartzes, phyllosilicates, such as antigorite, serpentine, hornblendes, amphibols, chrysotile, and talc; metal oxides, such as kaolin, aluminum oxides, aluminium hydroxides, magnesium hydroxides, hydromagnesite, titanium oxides and iron oxides, metal salts such as chalk, heavy spar and inorganic pigments, such as cadmium sulfide, zinc sulfide, and also glass and others. Preference is given to using kaolin (china clay), finely ground quartzes, aluminum silicate, and coprecipitates of barium sulfate and aluminum silicate.

Suitable fillers have an average particle diameter in the range of 0.1 pm to 500 pm, more preferably uin the range of 1 pm to 100 pm, and most preferably in the range of 1 pm to 10 pm. Diameter in this context, in the case of non-spherical particles, refers to their extent along the shortest axis in space. Suitable amounts of the fillers can be present in the polyurethane resin composition which are known to the person skilled in the art. For instance, fillers can be present in an amount up to 50 wt.-%, based on the total weight of the polyurethane resin composition.

In another preferred embodiment, the composite (B) has thermal conductivity of < 30 mW/m.K according to ASTM C 177 standard at a temperature of 37.5° C., in an ambient environment, at atmospheric pressure, and at a compression load of about 2 psi.

In another preferred embodiment, the composite article (P) has a thickness in the range of 1 mm to 50 mm; more preferably the composite article (P) has a thickness in the range of 5 mm to 45 mm; even more preferably the composite article (P) has a thickness in the range of 5 mm to 40 mm; most preferably the composite article (P) has a thickness in the range of 10 mm to 40 mm; and in particular the composite article (P) has a thickness in the range of 10 mm to 30 mm.

In another preferred embodiment, the coversheet has an area weight in the range of 100 g/m² to 1500 g/m².

In another preferred embodiment, the composite article (P) comprises: i. at least two coversheets(A); and

II. at least one composite (B); wherein the composite (B) is sandwiched between two coversheets with a layer structure A-B-A.

In another preferred embodiment, the composite article (P) comprises: i. at least three coversheets(A); and

II. at least two composite (B); wherein the composite (B) is sandwiched between two coversheets with a layer structure A-B-A-B-A; and binder component (C) is present in bet been the interface of A and B and/or over the A as a layer/sheet.

In another embodiment, presently claimed invention is directed to a process for preparing a composite product comprising the steps of: i. providing at least one composite (B);

II. providing at least one coversheet (A); ill. covering at least a part of the composite (B) with the cover sheet (A); and iv. spraying a binder composition onto the coversheet(A) to form a pre-impregnated blank, and v. compression moulding of the pre-impregnated blank.

In another preferred embodiment, the binder composition (C) forms a layer/film over the cover sheet(A).

In another preferred embodiment, the binder composition is polyurethane resin composition.

In another preferred embodiment, the polyurethane forms a layer/film over the cover sheet(A).

In another embodiment, the said binder composition (C) is sprayed onto the cover sheet (A) to form a film/layer over the coversheet. In another embodiment, the said binder composition (C) film is prepared from the polyurethane resin composition which is sprayed onto the cover sheet. In the present context, the term “polyurethane film” refers to the atomized polyurethane resin composition which, when sprayed onto the coversheet, binds itself to the cover sheet and has no thickness of its own. That is, to say, that the binder layer formed/ polyurethane film does not exists as a separate layer onto the cover sheet. Also, the term “atomized” herein refers to the particles or droplets of the polyurethane resin composition obtained from suitable spraying means, such as but not limited to a nozzle or an atomizer.

In another preferred embodiment, the binder composition forms a film on the coversheet(A); and resulting in a pre-impregnated blank.

In another preferred embodiment, the above described process is a spray transfer molding process. Spraying of the polyurethane resin composition onto the at least one cover sheet can be carried out using suitable means well known to the person skilled in the art. However, the isocyanate and the component reactive towards isocyanate can be mixed in a mixing device to obtain a reactive mixture before spraying it onto the at least one cover sheet as the polyurethane composition to obtain the preimpregnated blank. Suitable mixing device for this purpose are preferably a mixing head or a static mixer.

In another preferred embodiment, a reaction mixture is obtained by feeding at least two streams into the mixing device, wherein:

(i) a first stream comprises at least one isocyanate component, and

(ii) a second stream comprises at least one polyol component, wherein at least one of the catalysts, the additive and the filler is present in at least one of (i) and (ii).

Suitable temperatures for processing the reaction mixture are well known to the person skilled in the art. In one embodiment, the first stream and the second stream, independent of each other, can be premixed in suitable mixing means, such as, but not limited to, a static mixer.

The mixing device can be a low pressure or high-pressure mixing device comprising: i. pumps to feed the streams, ii. a high-pressure mixing head in which the streams, as described hereinabove, are mixed, iii. a first feed line fitted to the high-pressure mixing head through which the first stream is introduced into the mixing head, and iv. a second feed line fitted to the high-pressure mixing head through which the second stream is introduced into the mixing head.

Optionally, the mixing device, as described hereinabove, can further comprise at least one measurement and control unit for establishing the pressures of each feed lines in the mixing head. Also, the term “low pressure” here refers to a pressure in the range of 0.1 MPa to 5 MPa, while the term “high pressure” refers to pressure above 5 MPa.

In one embodiment, the reaction mixture is passed from the mixing head into the mixing device. A solid/gas mixture can be added through additional inlets. By “solid”, it is referred to the fillers, as described hereinabove, which are in a solid state of matter.

The reaction mixture obtained from the mixing device is fed to the spraying means. Suitable spraying means include, but are not limited to, spray heads. In one embodiment, the spray head for spraying the polyurethane resin composition comprises at least one polyurethane spray jet. The polyurethane spray jet essentially consists of fine particles or droplets of the polyurethane resin composition, i.e. of the reaction mixture, preferably dispersed in the gas stream. Such a polyurethane spray jet can be obtained in different ways, for example, by atomizing a liquid jet of the reaction mixture of the polyurethane resin composition by a gas stream introduced into it, or by the ejection of a liquid jet of the reaction mixture from a corresponding nozzle or atomizer. By the term “liquid jet of the reaction mixture”, it is referred to the fluid jet of the reaction mixture of the polyurethane resin composition that is not yet in the form of fine reaction mixture droplets dispersed in a gas stream, i.e. especially in a liquid viscous phase. Thus, in particular, such a “liquid jet of the reaction mixture” does not mean a polyurethane spray jet, as described above. Such methods are described, for example in, DE 10 2005 048 874 A1 , DE 101 61 600 A1 , WO 2007/073825 A2, US 3,107,057 A and DE 1 202 977 B.

Alternatively, a solid containing gas stream can also be employed instead of the gas stream, as described hereinabove. The solid-containing gas stream can be prepared by passing the gas stream through solid-containing metering cells of a cellular wheel sluice. By the flushing of the cellular spaces, the solid is dragged along by the pressurized air stream and transported to the mixing head as a solid/air or solid/gas mixture. To avoid pulsation, the channel inside the metering sluice must be designed with a diameter that excludes positive overlap. This embodiment further ensures that a quantitatively unchanged air flow rate for spraying the reaction mixture is available even when the cellular wheel sluice metering is turned off of its revolutions per minute is changed, and thus spraying can be effected alternatively without or with variable filler quantities. As a particular advantage of such a cellular wheel sluice, the solid proportion in the pre-impregnated blank to be prepared can be variably adjusted. The polyurethane spray jet, as described hereinabove, impinges on a spray area oscillating with an adjustable amplitude of less than 500 mm. By the term “spray area”, it is referred to the target area of the at least one cover sheet.

During the spraying, the at least one cover sheet optionally is wetted with the polyurethane resin composition. In one embodiment, spraying of the polyurethane resin composition is done on both the sides of the at least one cover sheet. In one embodiment, spraying of the polyurethane resin composition is done at least one side of the both cover sheet, if the combination is A-B-A fashion and the site of polyurethane spray is away from composite (B).

Handling of the at least one cover sheet can be either manually or automatically. By the term “automatically”, it is referred to the handling of the at least one cover sheet via a human interface, for instance, using industrial robots. In a preferred embodiment, an industrial robot that has preferably 6 axes and is especially tailored for production facilities using flexible robot-controller automation is employed. The robot is operated by means of a process software incorporated into a control cabinet. The control is suitable for communicating with external control systems. The robot can be equipped with a highly developed dual port safety system, the functions of which are continuously monitored. In case of a failure or malfunction, the electric supply of the motors can be switched off and brakes activated. Furthermore, the movement of each axes can be limited by software functions. In a preferred embodiment, the robot is driven via brushless three phase servomotors with brakes on all axes.

The pre-impregnated blank obtained is subsequently compression moulded , for example, in a heated compression molding tool and is compressed in accordance with the required geometry and hardened. Subsequently, it is optionally possible, while the composite article (P) is left in the compression molding tool, for a contour cut, that is to say, coarse cutting to shape, to be performed around the tool or around the tool geometry.

In another preferred embodiment, it is also possible, if necessary, the composite article (P) to be cooled or thermally stabilized in the compression molding tool or outside the compression molding tool, preferably cooled or thermally stabilized in a further tool, in particular in a workpiece cooling device.

In accordance with the embodiments, “thermally stabilized” is to be understood to mean that the composite article (P) assumes a temperature below the previous conversion temperature in order to attain a stable state.

In another embodiment, tempering of the composite, that is to say a temperature process, in order for distortions to be compensated and/or the level of cross-linking of the materials to be increased, is performed in a further tool or in a further device. For example, it may be provided that, for cooling, the composite article (P) is merely placed on a frame or by way of one side on a surface. Use may however also be made of a closed cooling device which surrounds the composite around the full circumference and in which the temperature can be regulated. In another preferred embodiment, the cooling can be followed by trimming of the outer contour, or cutting to shape of the side regions/edges, in accordance with the required contour and optionally also a chip-removing machining process, such as, for example, milling of the outer contour and milling and drilling for inserts and other similar recesses in the composite article construction.

Another aspect of the present invention relates to the use of the composite article (P), as described hereinabove, as an automotive part. In an embodiment, the automotive parts are selected from lower sound shield, acoustical belly pan, aero shield, splash shield, underbody panel, chassis shield, door module, or high temperature shield.

In another embodiment, the high temperature shileds are a battery cover, battery top, firewall, near exhaust parts

In another embodiment, presently claimed invention is directed to the use of the composite article (P) as thermal insulator.

In another embodiment, presently claimed invention is directed to the use of the composite article (P) as non-combustible or combustible product.

In another embodiment, presently claimed invention is directed to the use of the composite article (P) as an automotive part.

In another embodiment, presently claimed invention is directed to the use of the composite article (P) as a battery case.

In another embodiment, presently claimed invention is directed to the use of the composite article (P) to develop a 3-dimensional semi structural or a 3-dimesional structural framework.

In another embodiment, presently claimed invention is directed to an article comprising the composite article (P).

In another embodiment, presently claimed invention is directed to an automotive part comprising the composite article (P).

The thermal conductivity in the presently invention is determined according to ASTM C 177.

The hydroxy number in the presently invention is determined according to the standard acetic anhydride method.

The compressive strength in the presently invention is determined according to ASTM C165. The present invention is illustrated in more detail by the following embodiments and combinations of embodiments which result from the corresponding dependency references and links:

1 . A composite article (P) comprising: i. at least one coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1 ) and aleast one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1 ) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet.

2. The composite article according to embodiment 1 , wherein the composite article (P) comprises at least two coversheets (A).

3. The composite article according to any one of the embodiments 1 to 2, wherein the composite (B) is sandwiched between the two coversheets (A).

4. The composite article according to any one of the embodiments 1 to 3, wherein the coversheet is having a thickness in the range of 0.1 mm to 10 mm.

5. The composite article according to any one of the embodiments 1 to 4, wherein the coversheet is selected from fiber mat, thermosetting sheet, or thermoplastic sheet.

6. The composite article according to any one of the embodiments 1 to 5, wherein the fiber mat comprises fiberglass, carbon fiber, natural fiber, mineral wool, basalt, ceramic materials or any combination of one or more of the aforementioned.

7. The composite article according to embodiment 5, wherein the thermosetting coversheet is a polyurethane sheet.

8. The composite article according to embodiment 1 , wherein the lofty fibrous batting consists essentially of fibers having a thermal conductivity < 50 mW/m.K ASTM C177.

9. The composite article according to embodiment 8, wherein the lofty fibrous batting is made from fibers having a diameter in the range of 0.1 to 100 pm.

10. The composite article according to any one of the preceding embodiments wherein the composite (B) further comprises microfibers. 11 . The composite article according to embodiment 1 , wherein the aerogel (B2) is selected from inorganic or organic gel materials or any combinations thereof.

12. The composite article according to embodiment 11 , wherein the inorganic gel material is selected from oxides of zirconia, yttria, hafnia, alumina, titania, ceria, silica, or any combination thereof.

13. The composite article according to embodiment 12, wherein the organic gel forming material is selected from polyacrylates, polystyrenes, polyacrylonitriles, polyurethanes, polyimides, polyfurfural alcohol, phenol furfuryl alcohol, melamine formaldehydes, resorcinol formaldehydes, cresol formaldehyde, phenol formaldehyde, polyvinyl alcohol dialdehyde, polycyanurates, polyacrylamides, various epoxies, agar, agarose, or any combination thereof.

14. The composite article according to any one of the preceding embodiments, wherein the composite (B) comprises at least one dopant (B3).

15. The composite article according to embodiment 14, wherein the dopant (B3) is selected from carbon black, titania, iron oxides, silicon carbide, molybdenum silicide, manganese oxides, polydialkylsiloxanes wherein the alkyl groups contain 1 to 4 carbon atoms, or any combination thereof.

16. The composite article according to any of the embodiments 14 to 15, wherein the dopant is present in an amount of about 1 to 20% by weight based on the total weight of the composite

(B).

17. The composite article according to any one of the preceding embodiments, wherein the composite (B) has a density at 20 °C in the range of 0.15 and 0.40 g/cm³.

18. The composite article according to any one of the preceding embodiments, wherein the binder

(C) is selected from an organic binder, inorganic binder or any combination thereof.

19. The composite article according to embodiment 18, wherein the organic binder is a polyurethane resin composition.

20. The composite article according to embodiment 19, wherein the polyurethane resin composition comprises:

(a) an isocyanate, and

(b) an isocyanate reactive component, wherein (a) and (b) are present at an isocyanate index in the range of 100 to 180. The composite article according to embodiment 20, wherein the isocyanate index is in the range of 120 to 160. The composite article according to any of the embodiments 20 to 21 , wherein the isocyanate is an aromatic isocyanate or an aliphatic isocyanate. The composite article according to embodiments 22, wherein the aromatic isocyanate is selected from toluene diisocyanate; polymeric toluene diisocyanate, polymeric toluene diisocyanate, polymeric methylene diphenyl diisocyanate; 1 ,5-naphthalene diisocyanate; methylene diphenyl diisocyanate; polymeric methylene diphenyl diisocyanate; m-phenylene diisocyanate; 1 ,5-naphthalene diisocyanate; 4-chloro-1 ; 3-phenylene diisocyanate; 2,4,6-toluylene triisocyanate, 1 ,3-diisopropylphenylene-2,4-diisocyanate; 1-methyl-3,5-diethylphenylene-2,4-diisocya- nate; 1 ,3,5-triethylphenylene-2,4-diisocyanate; 1 ,3,5-triisoproply-phenylene-2,4-diisocyanate; 3,3'-diethyl-bisphenyl-4,4'-diisocyanate; 3,5,3',5'-tetraethyl-diphenylmethane-4,4'-diisocyanate; 3,5,3',5'-tetraisopropyldiphenylmethane-4,4'-diisocyanate; 1-ethyl-4-ethoxy-phenyl-2,5-diisocy- anate; 1 ,3,5-triethyl benzene-2,4,6-triisocyanate; 1-ethyl-3,5-diisopropyl benzene-2,4,6-triisocy- anate, tolidine diisocyanate, 1 ,3,5-triisopropyl benzene-2,4,6-triisocyanate or mixtures thereof The composite article according to embodiment 23, wherein the aromatic isocyanate is selected from methylene diphenyl diisocyanate, polymeric methylene diphenyl diisocyanate or combination thereof. The composite article according to embodiment 22, wherein the aliphatic isocyanate is selected from isophorone diisocyanate, propylene-1 ,2-diisocyanate, propylene-1 ,3-diisocyanate, butyl- ene-1 ,2-diisocyanate, butylene-1 ,3-diisocyanate, hexamethylene-1 ,6-diisocyanate, 2- methylpentamethylene-1 ,5-diisocyanate, 2-ethylbutylene-1 ,4-diisocyanate, 1 ,5-pentameth- ylene diisocyanate, ethyl ester l-lysine triisocyanate, 1 ,6,11-triisocyanatoundecane, (2,4,6-tri- oxotriazine-1 ,3,5(2h,4h,6h)-triyl)tris(hexamethylene) isocyanate, methyl-2,6-diisocyanate caproate, octamethlyene-1 ,8-diisocyanate, 2,4,4-trimethylhexamethylene-1 ,6-diisocyanate, nonamethylene diisocyanate, 2, 2, 4-trimethylhexamethylene-1 ,6-diisocyanate, decamethylene- 1 ,10-diisocyanate, 2,11-diisocyanato-dodecane, triphenylmethane-4,4’,4”-triisocyanate, tolu- ene-2,4,6-triyl triisocyanate, tris(isocyanatohexyl)biuret, tri methylcyclohexyl] triisocyanate, 2,4,4'-triisocyanato-dicyclohexylmethane, 2,2,-methylene-bis(cyclohexyl isocyanate), 3,3'- methylene-bis(cyclohexyl isocyanate), 4,4'-methylene-bis(cyclohexyl isocyanate), 4,4'-eth- ylene-bis(cyclohexyl isocyanate), 4,4'-propylene-bis-(cyclohexyl isocyanate), bis(paraisocyano- cyclohexyl)sulfide, bis(para-isocyanato-cyclohexyl)sulfone, bis(para-isocyano-cyclohexyl)ether, bis(para-isocyanato-cyclohexyl)diethyl silane, bis(para-isocyanato-cyclohexyl)diphenyl silane, bis(para-isocyanato-cyclohexyl)ethyl phosphine oxide, bis(para-isocyanato-cyclohexyl)phenyl phosphine oxide, bis(para-isocyanato-cyclohexyl)N-phenyl amine, bis(para-isocyanato-cyclo- hexyl)N-methyl amine,3,3-diisocyanato adamantane, 3,3-diisocyano biadamantane, 3,3-diiso- cyanatoethyl-1'-biadamantane, 1 ,2-bis (3-isocyanato-propoxy)ethane, 2,2-dimethyl propylene diisocyanate, 3-methoxy hexamethylene-1 ,6-diisocyanate, 2,5-dimethyl heptamethylene diisocyanate, 5-methyl nonamethylene-1 ,9-diisocyanate, 1 ,4-diisocyanato cyclohexane, 1 ,2-diisocy- anato octadecane, 2,5-diisocyanato-1 ,3,4-oxadiazole, OCN(CH2)3O(CH2)2O(CH2)3NCO, OCN(CH2)3N(CH3)(CH2)3NCO, polymeric forms of diisocyanates or mixtures thereof.

26. The composite article according to embodiment 20, wherein the isocyanate reactive component is a polyol having an average functionality in the range of 2.0 to 8.0.

27. The composite article according to embodiment 26, wherein the polyol has a hydroxyl number in the range of 15 mg KOH/g to 1800 mg KOH/g as determined according to the standard acetic anhydride method.

28. The composite article according to any one of the embodiments 26 to 27, wherein the polyol is a polyether polyol.

29. The composite article according to any one of the embodiments 19 to 28, wherein the polyurethane resin composition comprises a chain extender and/or cross linker having a molecular weight in the range of 49 g/mol to 399 g/mol.

30. The composite article according to any one of the embodiments 19 to 29, wherein the polyurethane resin composition further comprises catalysts, additives and fillers.

31. The composite article according to embodiment 30, wherein the additives are selected from pigments, dyes, surfactants, graphite, graphene, flame retardants, hindered amine light stabilizers, ultraviolet light absorbers, stabilizers, defoamers, internal release agents, desiccants, blowing agents, curing agents, fire class additive and anti-static agents or a combination thereof.

32. The composite article according to embodiment 31 , wherein the fire class additive is selected from the group consisting of clay materials, magnesium hydroxide, alumina trihydrate (“ATH”), metal carbonates and mixtures of two or more of the aforementioned.

33. The composite article according to any one of the embodiments 1 to 32, wherein the composite (B) has a thermal conductivity of < 30 mW/m.K according to ASTM C 177 standard at a temperature of 37.5° C., in an ambient environment, at atmospheric pressure, and at a compression load of about 2 psi.

34. The composite article according to any one of the embodiments 1 to 33, wherein the composite article (P) has a thickness in the range of 1 mm to 50 mm.

35. The composite article according to any one of the embodiments 1 to 34, wherein the coversheet has an area weight in the range of 100 g/m² to 1500 g/m². 36. The composite article according to any one of the embodiments 1 to 35 wherein the composite article comprises: i. at least two coversheets(A); and

II. at least one composite (B); wherein the composite (B) is sandwiched between two coversheets with a layer structure A- B-A.

37. A process for preparing a composite article (P) comprising the steps of: i. providing at least one composite (B);

38. The process according to embodiment 37, wherein the binder composition is a polyurethane resin composition.

39. The method according to any one of the embodiments 37 to 38, wherein the binder composition forms a film on the coversheet(A); and resulting in a pre-impregnated blank

40. The process according to any one of the embodiments 38 to 39, wherein the polyurethane resin composition is high pressure atomized.

41 . The process according to any one of the embodiments 37 to 40, wherein the process is a spray transfer moulding process.

42. Use of the composite article (P) according to any one of the embodiments 1 to 36 as thermal insulator.

43. Use of the composite article (P) according to any one of the embodiments 1 to 36 as non-com- bustible or combustible product.

44. Use of the composite article (P) according to any one of the embodiments 1 to 36 as an automotive part.

45. Use of the composite article (P) according to any one of the embodiments 1 to 36 as part of a 3-dimensional semi structural or a 3-dimesional structural framework.

46. An article comprising the composite article (P) according to any one of the embodiments 1 to 36. 47. An automotive part comprising the composite article (P) according to any one of the embodiments 1 to 36. EXAMPLES

Materials:

Preparation of composite (B)is known in the art, e.g. US 7,078,359 B2 discloses synthesis of composite (B) and incorporated herein as reference. Composite B is commercially available, e.g., Slentex® is available from BASF Corporation and can be used as such in place of composite (B)according to presently claimed invention.

Spray transfer molding technique is known a person skilled in art and such method is discloses in WO 2020/021066 A1 and incorporated herein as reference.

Cover sheet: Glass fiber mat having an area weight of 300 to 600 g/m² used as coversheet.

The inventive composite article (P) was obtained using the two-component binder system comprising the isocyanate component and the polyol component, as above.

The composite (B) herein Slentex® was sandwiched between 2 cover sheets made of glass fiber mat. The robotic end of arm tooling held the sandwiched composite article (P) in place and placed it below the polyurethane spray head. The polyurethane resin composition was sprayed on both sides of the cover sheet and subsequently positioned under a heated mold to form and cure the composite article (P). The temperature of the mold was kept at 120°C and pressure of the mold was kept in the range of 100 to 200 tons/m². The product obtained was rigid and structurally stable compared to composite (B) which is flexible. The product could be molded into any shape depends on the mold while curing the article (P).

Paper honeycomb was sandwiched between two glass fibre mat was used for comparison experiments. Paper honeycomb sandwiched between two glass fibre mat and the polyurethane resin composition was sprayed on both sides of the glass fibre mat to obtain the comparative composite article.

Method for Bonfire test:

A 10 mm thick having 12cm X12 cm composite article (P) was prepared. A Bunsen burner was positioned 15 mm below the composite article (P). Two thermocouples were installed in order to measure the temperature change. The first thermocouple was installed in the middle of the cross section ( 5 mm from the bottom), and 60 mm deep in the part and the second thermocouple was install on the top surface in the middle of the cross sections, 60 mm from each side. The Bunsen burner was lightened with flame of 15mm height to touch the lower surface of the composite article (P). The temperature was recorded on every one second for a period of 20 minutes of both the thermocouples 1 and thermocouple 2.

Table 1 : Heat conduction data: This was conducted in accordance with ASTM C 177

It is evident that the composite (P) obtained according to presently claimed invention displays structural rigidity compared to composite (B). Further, the composite (P) displays excellent resistance to heat conduction. The composite article (P) also displayed excellent NVH data.

Claims

1 . A composite article (P) comprising: i. at least one coversheet (A);

II. at least one composite (B) comprising at least one reinforcing structure (B1 ) and at least one aerogel(B2); and ill. at least one binder composition (C); wherein the reinforcing structure (B1) comprises lofty fibrous batting and/or organic sheet and/or inorganic sheet and a continuous aerogel (B2) through said batting/sheet.

2. The composite article according to claim 1 , wherein the composite article (P) comprises at least two coversheets (A).

3. The composite article according to any one of the claims 1 to 2, wherein the composite (B) is sandwiched between the two coversheets (A).

4. The composite article according to any one of the claims 1 to 3, wherein the coversheet is having a thickness in the range of 0.1 mm to 10 mm.

5. The composite article according to any one of the claims 1 to 4, wherein the coversheet is selected from fiber mat, thermosetting sheet, or thermoplastic sheet.

6. The composite article according to any one of the claims 1 to 5, wherein the fiber mat comprises fiberglass, carbon fiber, natural fiber, mineral wool, basalt, ceramic materials or any combination of one or more of the aforementioned.

7. The composite article according to claim 5, wherein the thermosetting coversheet is a polyurethane sheet.

8. The composite article according to claim 1 , wherein the lofty fibrous batting consists essentially of fibers having a thermal conductivity < 50 mW/m.K ASTM C177.

9. The composite article according to claim 8, wherein the lofty fibrous batting is made from fibers having a diameter in the range of 0.1 to 100 pm.

10. The composite article according to any one of the preceding claims wherein the composite (B) further comprises microfibers.

11. The composite article according to claim 1 , wherein the aerogel (B2) is selected from inorganic or organic gel materials or any combinations thereof.

34

12. The composite article according to claim 11 , wherein the inorganic gel material is selected from oxides of zirconia, yttria, hafnia, alumina, titania, ceria, silica, or any combination thereof.

13. The composite article according to claim 12, wherein the organic gel forming material is selected from polyacrylates, polystyrenes, polyacrylonitriles, polyurethanes, polyimides, polyfurfural alcohol, phenol furfuryl alcohol, melamine formaldehydes, resorcinol formaldehydes, cresol formaldehyde, phenol formaldehyde, polyvinyl alcohol dialdehyde, polycyanurates, polyacrylamides, various epoxies, agar, agarose, or any combination thereof.

14. The composite article according to any one of the preceding claims, wherein the composite (B) comprises at least one dopant (B3).

15. The composite article according to claim 14, wherein the dopant (B3) is selected from carbon black, titania, iron oxides, silicon carbide, molybdenum silicide, manganese oxides, polydialkylsiloxanes wherein the alkyl groups contain 1 to 4 carbon atoms, or any combination thereof.

16. The composite article according to any of the claims 14 to 15, wherein the dopant is present in an amount of about 1 to 20% by weight based on the total weight of the composite (B).

17. The composite article according to any one of the preceding claims, wherein the composite (B) has a density at 20 °C in the range of 0.15 and 0.40 g/cm³.

18. The composite article according to any one of the preceding claims, wherein the binder (C) is selected from an organic binder, inorganic binder or any combination thereof.

19. The composite article according to claim 18, wherein the organic binder is a polyurethane resin composition.

20. The composite article according to claim 19, wherein the polyurethane resin composition comprises:

(a) an isocyanate, and

(b) an isocyanate reactive component, wherein (a) and (b) are present at an isocyanate index in the range of 100 to 180.

21. The composite article according to claim 20, wherein the isocyanate index is in the range of 120 to 160.

22. The composite article according to any of the claims 20 to 21 , wherein the isocyanate is an aromatic isocyanate or an aliphatic isocyanate.

35

The composite article according to claims 22, wherein the aromatic isocyanate is selected from toluene diisocyanate; polymeric toluene diisocyanate, polymeric toluene diisocyanate, polymeric methylene diphenyl diisocyanate; 1 ,5-naphthalene diisocyanate; methylene diphenyl diisocyanate; polymeric methylene diphenyl diisocyanate; m-phenylene diisocyanate; 1 ,5-naph- thalene diisocyanate; 4-chloro-1 ; 3-phenylene diisocyanate; 2,4,6-toluylene triisocyanate, 1 ,3- diisopropylphenylene-2,4-diisocyanate; 1-methyl-3,5-diethylphenylene-2,4-diisocyanate; 1 ,3,5- triethylphenylene-2,4-diisocyanate; 1 ,3,5-triisoproply-phenylene-2,4-diisocyanate; 3,3'-diethyl- bisphenyl-4,4'-diisocyanate; 3,5,3',5'-tetraethyl-diphenylmethane-4,4'-diisocyanate; 3, 5,3', 5'- tetraisopropyldiphenylmethane-4,4'-diisocyanate; 1-ethyl-4-ethoxy-phenyl-2,5-diisocyanate;

1 .3.5-triethyl benzene-2,4,6-triisocyanate; 1-ethyl-3,5-diisopropyl benzene-2,4,6-triisocyanate, tolidine diisocyanate, 1 ,3,5-triisopropyl benzene-2,4,6-triisocyanate or mixtures thereof The composite article according to claim 23, wherein the aromatic isocyanate is selected from methylene diphenyl diisocyanate, polymeric methylene diphenyl diisocyanate or combination thereof. The composite article according to claim 22, wherein the aliphatic isocyanate is selected from isophorone diisocyanate, propylene-1 ,2-diisocyanate, propylene-1 ,3-diisocyanate, butylene- 1 ,2-diisocyanate, butylene-1 ,3-diisocyanate, hexamethylene-1 ,6-diisocyanate, 2-methylpen- tamethylene-1 ,5-diisocyanate, 2-ethylbutylene-1 ,4-diisocyanate, 1 ,5-pentamethylene diisocyanate, ethyl ester l-lysine triisocyanate, 1 ,6,11-triisocyanatoundecane, (2,4,6-trioxotriazine- 1 ,3,5(2h,4h,6h)-triyl)tris(hexamethylene) isocyanate, methyl-2,6-diisocyanate caproate, octam- ethlyene-1 ,8-diisocyanate, 2,4,4-trimethylhexamethylene-1 ,6-diisocyanate, nonamethylene diisocyanate, 2,2,4-trimethylhexamethylene-1 ,6-diisocyanate, decamethylene-1 , 10-diisocya- nate, 2,11-diisocyanato-dodecane, triphenylmethane-4,4’,4”-triisocyanate, toluene-2,4,6-triyl tri isocyanate, tris(isocyanatohexyl)biuret, trimethylcyclohexyl] triisocyanate, 2,4,4'-triisocya- nato-dicyclohexylmethane, 2,2,-methylene-bis(cyclohexyl isocyanate), 3,3'-methylene-bis(cy- clohexyl isocyanate), 4,4'-methylene-bis(cyclohexyl isocyanate), 4,4'-ethylene-bis(cyclohexyl isocyanate), 4,4'-propylene-bis-(cyclohexyl isocyanate), bis(paraisocyano-cyclohexyl)sulfide, bis(para-isocyanato-cyclohexyl)sulfone, bis(para-isocyano-cyclohexyl)ether, bis(para-isocya- nato-cyclohexyl)diethyl silane, bis(para-isocyanato-cyclohexyl)diphenyl silane, bis(para-isocya- nato-cyclohexyl)ethyl phosphine oxide, bis(para-isocyanato-cyclohexyl)phenyl phosphine oxide, bis(para-isocyanato-cyclohexyl)N-phenyl amine, bis(para-isocyanato-cyclohexyl)N-methyl amine,3,3-diisocyanato adamantane, 3,3-diisocyano biadamantane, 3,3-diiso-cyanatoethyl-1'- biadamantane, 1 ,2-bis (3-isocyanato-propoxy)ethane, 2,2-dimethyl propylene diisocyanate, 3- methoxy hexamethylene-1 ,6-diisocyanate, 2,5-dimethyl heptamethylene diisocyanate, 5-methyl nonamethylene-1 ,9-diisocyanate, 1 ,4-diisocyanato cyclohexane, 1 ,2-diisocyanato octadecane,

2.5-diisocyanato-1 ,3,4-oxadiazole, OCN(CH2)3O(CH2)2O(CH2)3NCO,

OCN(CH2)3N(CH3)(CH2)3NCO, polymeric forms of diisocyanates or mixtures thereof.

26. The composite article according to claim 20, wherein the isocyanate reactive component is a polyol having an average functionality in the range of 2.0 to 8.0.

27. The composite article according to claim 26, wherein the polyol has a hydroxyl number in the range of 15 mg KOH/g to 1800 mg KOH/g as determined according to the standard acetic anhydride method.

28. The composite article according to any one of the claims 26 to 27, wherein the polyol is a polyether polyol.

29. The composite article according to any one of the claims 19 to 28, wherein the polyurethane resin composition comprises a chain extender and/or cross linker having a molecular weight in the range of 49 g/mol to 399 g/mol.

30. The composite article according to any one of the claims 19 to 29, wherein the polyurethane resin composition further comprises catalysts, additives and fillers.

31 . The composite article according to claim 30, wherein the additives are selected from pigments, dyes, surfactants, graphite, graphene, flame retardants, hindered amine light stabilizers, ultraviolet light absorbers, stabilizers, defoamers, internal release agents, desiccants, blowing agents, curing agents, fire class additive and anti-static agents or a combination thereof.

32. The composite article according to claim 31 , wherein the fire class additive is selected from the group consisting of clay materials, magnesium hydroxide, alumina trihydrate (“ATH”), metal carbonates and mixtures of two or more of the aforementioned.

33. The composite article according to any one of the claims 1 to 32, wherein the composite (B) has a thermal conductivity of < 30 mW/m.K according to ASTM C 177 standard at a temperature of 37.5° C., in an ambient environment, at atmospheric pressure, and at a compression load of about 2 psi.

34. The composite article according to any one of the claims 1 to 33, wherein the composite article (P) has a thickness in the range of 1 mm to 50 mm.

35. The composite article according to any one of the claims 1 to 34, wherein the coversheet has an area weight in the range of 100 g/m² to 1500 g/m².

36. The composite article according to any one of the claims 1 to 35 wherein the composite article comprises: i. at least two coversheets(A); and

38. The process according to claim 37, wherein the binder composition is a polyurethane resin composition.

39. The method according to any one of the claims 37 to 38, wherein the binder composition forms a film on the coversheet(A); and resulting in a pre-impregnated blank

40. The process according to any one of the claims 38 to 39, wherein the polyurethane resin composition is high pressure atomized.

41 . The process according to any one of the claims 37 to 40, wherein the process is a spray transfer moulding process.

42. Use of the composite article (P) according to any one of the claims 1 to 36 as thermal insulator.

43. Use of the composite article (P) according to any one of the claims 1 to 36 as non-combustible or combustible product.

44. Use of the composite article (P) according to any one of the claims 1 to 36 as an automotive part.

45. Use of the composite article (P) according to any one of the claims 1 to 36 as part of a 3- dimensional semi structural or a 3-dimesional structural framework.

46. An article comprising the composite article (P) according to any one of the claims 1 to 36.

47. An automotive part comprising the composite article (P) according to any one of the claims 1 to 36.

38