Liquid metal composition and method

Abstract

This disclosure generally relates to compositions having components that can become liquid or exhibit a phase change during use, and methods associated with said compositions. These can, for example, be used as thermal interface materials for a variety of applications. Some thermal interface materials (such as those discussed herein) can represent novel structures in which the material is solid but becomes liquid during use, which can improve heat transfer, for example, because the liquid improves the contact or bonding of surfaces, thereby allowing improved heat transfer across the interface between surfaces. For example, in some cases, the composition can be a composite of a solid-phase material and a phase change material. In some aspects, said phase change material exhibits a melting temperature, for example, at which the phase change material can change from liquid to solid. The phase change material can include, for example, metals, metal oxides, metal alloys, etc. Other aspects generally relate to methods for preparing or using such compositions, kits including such compositions, etc.

Description

Technical Field

[0001] This disclosure generally relates to liquid metal compositions and methods associated with them. Background Technology

[0002] Liquid metals are metals or metal alloys that can exist as liquids at room temperature. Depending on various factors, including the atomic composition, purity, and / or processing conditions, liquid metals exhibit interesting properties such as high or low viscosity, corrosion resistance, and high or low wettability. Due to their unique properties, liquid metals are used in thermostats, barometers, heat transfer systems, thermal cooling systems, and other applications. Integrating them into composites is challenging; therefore, improvements are needed. Summary of the Invention

[0003] This disclosure generally relates to liquid metal compositions and methods associated with them. In some cases, the subject matter of this disclosure relates to related products, alternative solutions to specific problems, and / or a variety of different uses of one or more systems and / or articles.

[0004] In one aspect, this disclosure relates to a self-supporting composite. In one set of embodiments, the self-supporting composite has a thickness between 10 micrometers and 1 mm. In another set of embodiments, the composite comprises a solid phase material and a phase change material. In some embodiments, the solid phase material comprises an open-pore volume of less than 90 vol%. In another set of embodiments, the phase change material comprises a metal, a metal oxide, a metal alloy, or a combination thereof. In some embodiments, the phase change material exhibits a melting temperature between 10°C and 65°C. In some embodiments, the composite has a thickness of less than 10 mm at a temperature 10°C above the melting temperature. 2 Thermal resistance in k / W. In some embodiments, when tested using a fixture capable of performing ASTM D5470 tests, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

[0005] In one set of embodiments, the self-supporting composite has a thickness between 200 micrometers and 1 mm. In another set of embodiments, the composite comprises a solid-phase material and a phase change material. In yet another set of embodiments, the solid-phase material comprises an open-pore volume of less than 90 vol%. In some embodiments, the phase change material comprises a metal, a metal oxide, a metal alloy, or a combination thereof. In some embodiments, the phase change material exhibits a melting temperature between 10°C and 65°C. In some embodiments, the composite has a thickness of less than 10 mm at a temperature 10°C above the melting temperature. 2Thermal resistance in k / W. In some embodiments, when tested using a fixture capable of performing ASTM D5470 testing, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

[0006] In one set of embodiments, the self-supporting composite has a thickness between 10 micrometers and 1 mm. In another set of embodiments, the composite comprises a solid-phase material and a phase change material that do not chemically react with each other. In yet another set of embodiments, the composite is flux-free. According to some embodiments, the solid-phase material comprises an open-pore volume of less than 90 vol%. In some embodiments, the phase change material comprises a metal, a metal oxide, a metal alloy, or a combination thereof.

[0007] According to some embodiments, the phase change material exhibits a melting temperature between 10°C and 65°C. In some embodiments, the composite has a thickness of less than 10 mm at a temperature 10°C above the melting temperature. 2 Thermal resistance in k / W. In some embodiments, after 1000 hours at a temperature 5°C above the melting temperature, the composite contains 2 mm of the thermal resistance. 2 Thermal resistance within K / W. According to some embodiments, when tested using a fixture capable of performing ASTM D5470 tests, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

[0008] In one set of embodiments, the self-supporting composite has a thickness between 200 micrometers and 1 mm. In some embodiments, the composite comprises a solid-phase material and a phase change material that do not chemically react with each other. In some embodiments, the composite is flux-free. According to some embodiments, the solid-phase material comprises an open-pore volume of less than 90 vol%. In some embodiments, the phase change material comprises a metal, a metal oxide, a metal alloy, or a combination thereof. According to some embodiments, the phase change material exhibits a melting temperature between 10°C and 65°C. In some embodiments, the composite has a thickness of less than 10 mm at a temperature 10°C above the melting temperature. 2 The original thermal resistance in K / W. In some embodiments, after 1000 hours at a temperature 5°C above the melting temperature, the composite contains 2 mm of the thermal resistance. 2 Thermal resistance within k / W. In some embodiments, when tested using a fixture capable of performing ASTM D5470 testing, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

[0009] In another aspect, this disclosure relates to methods for preparing one or more of the embodiments described herein, such as self-supporting composites. In yet another aspect, this disclosure relates to using one or more of the embodiments described herein, such as composites comprising phase change materials and solid-phase materials.

[0010] Other advantages and novel features of this disclosure will become apparent from the following detailed description of various non-limiting embodiments of this disclosure when considered in conjunction with the accompanying drawings. Attached Figure Description

[0011] Non-limiting embodiments of this disclosure will be described by way of example with reference to the accompanying drawings, which are schematic and not intended to be drawn to scale. In the drawings, each identical or substantially identical component shown is typically represented by a single number. For clarity, not every component is labeled in each drawing, nor is every component of each embodiment of this disclosure shown, unless illustrated to the effect of this disclosure on those skilled in the art. In the drawings:

[0012] Figure 1 A composite material formed from a solid-phase material and a phase change material according to a set of embodiments is shown.

[0013] Figure 2 A composite having a first continuous outer surface formed of a phase change material is shown according to another set of embodiments.

[0014] Figure 3 A composite having a first continuous outer surface and a second continuous outer surface formed of a phase change material is shown according to certain embodiments.

[0015] Figure 4 A composite having a first continuous outer surface and a second continuous outer surface connected by a solid phase material is shown according to certain embodiments.

[0016] Figure 5 Optical images of the composite according to some embodiments are shown.

[0017] Figure 6A and Figure 6B A fixture capable of performing ASTM D5470 testing is shown according to certain embodiments. Detailed Implementation

[0018] This disclosure generally relates to compositions having components that can become liquid or exhibit a phase change during use, and methods associated with said compositions. These can, for example, be used as thermal interface materials for a variety of applications. Some thermal interface materials (such as those discussed herein) can represent novel structures in which the material is solid but becomes liquid during use, which can improve heat transfer, for example, because the liquid improves the contact or bonding of surfaces, thereby allowing improved heat transfer across the interface between surfaces. For example, in some cases, the composition can be a composite of a solid-phase material and a phase change material. In some aspects, said phase change material exhibits a melting temperature, for example, at which the phase change material can change from liquid to solid. The phase change material can include, for example, metals, metal oxides, metal alloys, etc. Other aspects generally relate to methods for preparing or using such compositions, kits including such compositions, etc.

[0019] In some embodiments, the composite is a self-supporting composite. The self-supporting composite can be processed without a support (e.g., without a carrier membrane, support material, substrate, etc.). The self-supporting composite can have any suitable structure and any suitable size. For example, the self-supporting composite can be a self-supporting (e.g., self-standing) membrane (e.g., a micrometer-sized membrane). In some embodiments, the composite can be fabricated on a support material, and then the support material can be removed (e.g., peeled off), leaving the composite, for example, as a self-supporting structure. In other embodiments, the self-supporting composition structure can be thicker or have other dimensions. The self-supporting composite can be fabricated by any of the methods disclosed herein. Furthermore, it should be understood that the composite (as described herein) does not need to be self-supporting in all embodiments; for example, in some embodiments, the composite can exist as a membrane on a support, for example, where the composite is not self-supporting.

[0020] In some embodiments, the determination of the self-supporting composite can be performed at different temperatures; for example, the temperature at which the composite exhibits self-supporting behavior can be at least -30°C, at least -20°C, at least -10°C, at least 0°C, at least 5°C, at least 10°C, at least 15°C, or at least 20°C. According to some embodiments, the temperature at which the composite exhibits self-supporting behavior can not exceed 40°C, not exceed 30°C, not exceed 25°C, not exceed 20°C, or not exceed 15°C. Any combination of these temperatures is also possible, for example, at least 10°C but not exceeding 25°C.

[0021] Additionally, in some embodiments, the temperature of the self-supporting composite can be determined by the melting temperature of the phase change material within the self-supporting composite and / or a temperature relatively close to said melting temperature. For example, the temperature of the self-supporting composite can be determined at least 5°C, at least 10°C, at least 15°C, at least 20°C, or at least 25°C higher than said melting temperature. In some cases, the temperature can be no more than 25°C, no more than 20°C, no more than 15°C, no more than 10°C, or no more than 5°C higher than the melting temperature. In some cases, the determination can be performed within any combination of these ranges; for example, the composite can exhibit self-supporting behavior at temperatures between 5°C and 25°C, between 10°C and 15°C, between 5°C and 10°C, between 20°C and 30°C, etc., above the melting temperature of the phase change material.

[0022] In some embodiments, the self-supporting behavior of the composite can be determined by providing a piece of the composite with a width of at least 6 cm and a length of at least 6 cm, and supporting it on a support frame such that the unsupported length of the composite extends 3 cm from the support frame without any support below it. The self-supporting material is one that does not exhibit any significant permanent changes, such as cracking, leakage (e.g., leakage of a phase change material), or permanent deformation (although some sagging may occur due to gravity, e.g., at the unsupported end of the composite). According to some embodiments, the self-supporting material can retain its properties (e.g., mechanical properties) when at least a portion of the self-supporting material is on the support frame (e.g., a clamp).

[0023] In some embodiments, the self-supporting composite may have one or more components that alter the physical state while maintaining its self-supporting behavior. In some cases, one or more components within the self-supporting composite (e.g., a phase change material) may be liquid, which may be advantageous in some embodiments, for example, for improving thermal conductivity at the composite interface. In some cases, one or more liquid components within the self-supporting composition may provide enhanced adhesion to other components within the composite (e.g., particles). In some cases, the self-supporting composite may be solid (e.g., a solid sheet). Self-supporting composites comprising solid sheets do not deform, stretch, break, etc., during their manufacture. In some cases, the self-supporting composite may exhibit mechanical properties similar to or superior to other composites known in the art, such as composites with a metal matrix.

[0024] In some embodiments, for example, the composite may have an average thickness of less than 1 cm, less than 5 mm, less than 3 mm, less than 1 mm, less than 500 micrometers, less than or equal to 250 micrometers, less than or equal to 200 micrometers, less than or equal to 150 micrometers, or less than or equal to 100 micrometers. In some embodiments, the composite may have an average thickness of greater than or equal to 50 micrometers, greater than or equal to 100 micrometers, greater than or equal to 150 micrometers, greater than or equal to 200 micrometers, greater than or equal to 500 micrometers, greater than or equal to 1 mm, greater than or equal to 3 mm, greater than or equal to 5 mm, greater than or equal to 1 cm, etc. Combinations of the ranges listed above are possible (e.g., the composite may have an average thickness of less than or equal to 250 micrometers and greater than or equal to 50 micrometers, or the composite may have an average thickness of less than or equal to 150 micrometers and greater than or equal to 100 micrometers). Other ranges are also possible, as this disclosure is not limiting in this respect.

[0025] In some embodiments, the composite comprises a solid-phase material. In various embodiments, the solid-phase material may be advantageous for the composite (e.g., providing structural support, enhancing composite properties, etc.). In some embodiments, the solid-phase material is solid at room temperature. In some cases, the solid-phase material may include foamed metals (e.g., active or inactive foamed metals), porous metal solids, passivated metal particles, fibers (such as carbon fibers), foamed carbon, carbon paper, carbon nanoparticles, carbon nanotubes, graphene nanosheets, polymer foams, polymer paper, organic foams, organic paper, foam ceramics, carbon-based particles, ceramic particles, ceramic nanosheets, etc. These will be discussed in more detail below.

[0026] In some cases, solid materials can provide structural integrity to the composite during use, for example, when the phase change material can transform into a liquid. For instance, solid materials can prevent the composite from cracking or permanently deforming during use, such as when exposed to temperatures above the melting temperature of the phase change material (as described herein). In some cases, such as when the composite is exposed to temperatures above the melting temperature of the phase change material, solid materials can prevent the composite from leaking the phase change material.

[0027] In some embodiments, the solid material may form the majority of the composite. According to some embodiments, the solid material may be present in the composite at a weight percentage of at least 3 wt%, at least 5 wt%, at least 10 wt%, at least 15 wt%, at least 20 wt%, at least 25 wt%, at least 30 wt%, at least 35 wt%, at least 40 wt%, at least 45 wt%, at least 50 wt%, at least 55 wt%, at least 60 wt%, at least 65 wt%, at least 70 wt%, at least 75 wt%, at least 80 wt%, at least 85 wt%, at least 90 wt%, or at least 95 wt%. In some cases, the solid material may be present in the composite at a weight percentage not exceeding 95 wt%, not exceeding 90 wt%, not exceeding 85 wt%, not exceeding 80 wt%, not exceeding 75 wt%, not exceeding 70 wt%, not exceeding 65 wt%, not exceeding 60 wt%, not exceeding 55 wt%, not exceeding 50 wt%, not exceeding 45 wt%, not exceeding 40 wt%, not exceeding 35 wt%, not exceeding 30 wt%, not exceeding 25 wt%, not exceeding 20 wt%, not exceeding 15 wt%, not exceeding 10 wt%, not exceeding 5 wt%, or not exceeding 3 wt%. In some embodiments, any combination of these is also possible. For example, the solid material may be present in the composite at a weight percentage between 50 wt% and 60 wt%, between 75 wt% and 80 wt%, between 30 wt% and 50 wt%, between 3 wt% and 50 wt%, etc.

[0028] In addition to solid materials, the composite can also contain phase change materials. A non-limiting example is illustrated in... Figure 1 In this embodiment, composite 100 comprises a phase change material 101 and a solid material 102. According to some embodiments, the phase change material may comprise a metal, a metal oxide, a metal alloy, or a combination thereof. For example, in some cases, the phase change material may comprise a metal that is liquid at or near room temperature (approximately 25°C) below or near room temperature (e.g., within + / - 10°C). In some cases, metal oxides or metal alloys may be advantageous when used as phase change materials. For example, depending on the chemical composition of the selected metal oxide / alloy, the metal oxide / alloy may provide a wide range of properties. In some cases, it may be desirable to use any combination of metals, metal oxides, and metal alloys. Non-limiting examples of phase change materials include, but are not limited to, gallium, tin, indium, bismuth, cadmium, lead, antimony, aluminum, zinc, tellurium, alloys thereof, or oxides thereof.

[0029] In some embodiments, the phase change material may exhibit a melting temperature. The melting temperature of a phase change material is the phase transition (e.g., solid to liquid) temperature of the phase change material. When the material is cooled, the melting temperature may also correspond to the phase transition (e.g., liquid to solid) temperature. In some cases, the phase change material may exhibit a supercooling effect.

[0030] In some embodiments, the melting temperature exhibited by the phase change material can be a specific temperature or temperature range. The melting temperature can be at least -30°C, at least -20°C, at least -10°C, at least 0°C, at least 10°C, at least 20°C, at least 30°C, at least 40°C, at least 50°C, or at least 60°C. The melting temperature can not exceed 100°C, 90°C, 80°C, 70°C, 60°C, or 50°C. In some embodiments, the melting temperature of the phase change material can be between these values, for example, between 10°C and 70°C, between 20°C and 60°C, between 30°C and 40°C, between 20°C and 70°C, between 20°C and 60°C, between 20°C and 50°C, between 20°C and 40°C, etc. In some embodiments, for example, the phase change material exhibits a melting temperature between 10°C and 65°C. In another example, the phase change material exhibits a melting temperature between 0°C and 80°C.

[0031] In some cases, the phase change material can be selected to have a melting temperature above room temperature (25°C). For example, the phase change material can exhibit a melting temperature of at least about 30°C, at least about 35°C, at least about 40°C, at least about 45°C, or at least about 50°C. In some cases, the melting temperature can be less than 50°C, less than 45°C, less than 40°C, less than 35°C, less than 30°C, etc. Combinations of these are also possible; for example, the melting temperature can be selected between 25°C and 30°C, between 25°C and 35°C, between 30°C and 40°C, etc. For example, the phase change material can be an alloy or eutectic mixture of gallium, tin, indium, bismuth, or other materials (any of those described herein).

[0032] In some embodiments, the phase change material may form the majority of the composite. According to some embodiments, the phase change material may be present in the composite at a weight percentage of at least 30 wt%, at least 35 wt%, at least 40 wt%, at least 45 wt%, at least 50 wt%, at least 55 wt%, at least 60 wt%, at least 65 wt%, at least 70 wt%, at least 75 wt%, at least 80 wt%, at least 85 wt%, at least 90 wt%, or at least 95 wt%. In some cases, the phase change material may be present in the composite at a weight percentage not exceeding 95 wt%, not exceeding 90 wt%, not exceeding 85 wt%, not exceeding 80 wt%, not exceeding 75 wt%, not exceeding 70 wt%, not exceeding 65 wt%, not exceeding 60 wt%, not exceeding 55 wt%, not exceeding 50 wt%, not exceeding 45 wt%, not exceeding 40 wt%, not exceeding 35 wt%, or not exceeding 30 wt%. In some embodiments, any combination of these is also possible. For example, phase change materials can exist in the composite in amounts between 50 wt% and 60 wt%, between 75 wt% and 80 wt%, between 30 wt% and 50 wt%, etc.

[0033] In some aspects, the phase change material can exist within an open-pore volume defined by the solid phase material within the composite. The open-pore volume can be defined by the solid phase material, for example, in the form of voids, pores, holes, channels, surface textures, surface roughness, etc. According to some embodiments, the open-pore volume of the solid phase material can be the volume of the composite not occupied by the solid phase material. Some or all of the open-pore volume can be filled with the phase change material, although in some cases, other materials (or air) may also be present in at least some of the open-pore volumes defined by the solid phase material. According to some embodiments, for example, the composite has an open-pore volume defined by the solid phase material of at least 1 vol%, at least 5 vol%, at least 10 vol%, at least 15 vol%, at least 20 vol%, at least 25 vol%, at least 30 vol%, at least 35 vol%, at least 40 vol%, at least 45 vol%, at least 50 vol%, at least 55 vol%, at least 60 vol%, at least 65 vol%, at least 70 vol%, at least 75 vol%, at least 80 vol%, etc. In some cases, the complex has an open-cell volume of less than 80 vol%, less than 75 vol%, less than 70 vol%, less than 65 vol%, less than 60 vol%, less than 55 vol%, less than 50 vol%, less than 45 vol%, less than 40 vol%, less than 35 vol%, less than 30 vol%, less than 25 vol%, less than 20 vol%, less than 15 vol%, less than 10 vol%, less than 5 vol%, or less than 1 vol%. Any combination of these is also possible; for example, the complex may have an open-cell volume between 30 vol% and 40 vol%, between 65 vol% and 90 vol%, between 20 vol% and 25 vol%, etc.

[0034] In some cases, for example as described herein, the open-pore volume of solid materials of at least 1 vol%, at least 5 vol%, at least 10 vol%, at least 15 vol%, at least 20 vol%, at least 25 vol%, at least 30 vol%, at least 35 vol%, at least 40 vol%, at least 45 vol%, at least 50 vol%, at least 55 vol%, at least 60 vol%, at least 65 vol%, at least 70 vol%, at least 75 vol%, at least 80 vol%, at least 85 vol%, at least 90 vol%, at least 95 vol%, at least 99 vol%, etc., can be filled with phase change materials. In some cases, the open-pore volume of solid materials less than 99 vol%, less than 95 vol%, less than 90 vol%, less than 85 vol%, less than 80 vol%, less than 75 vol%, less than 70 vol%, less than 65 vol%, less than 60 vol%, less than 55 vol%, less than 50 vol%, less than 45 vol%, less than 40 vol%, less than 35 vol%, less than 30 vol%, less than 25 vol%, less than 20 vol%, less than 15 vol%, less than 10 vol%, less than 5 vol%, or less than 1 vol% can be filled with phase change materials. In some cases, any combination of these is also possible.

[0035] According to some embodiments, the pore volume of the solid material can be continuous and / or discontinuous. A continuous pore volume can have portions of pore volumes (e.g., holes) that are interconnected. A discontinuous pore volume can have portions of pore volumes that are not interconnected. In some embodiments, the composite / solid material can also have a combination of continuous and discontinuous pore volume portions.

[0036] Phase change materials (PCMs) can be distributed within the composite in any suitable arrangement. For example, PCMs can be present in one or more layers within the composite, or uniformly mixed within the composite. In some cases, PCMs can be present in one or more isolated portions or locations within the composite. As a non-limiting example, according to some embodiments, a solid-phase material can form a continuous outer surface of the composite, which, during use of the composite, for example, if the composite is heated to a temperature above the melting temperature of the PCMs, can, for example, prevent or inhibit leakage of the PCMs from the composite. The continuous outer surface can be an exposed (e.g., exposed to the environment) surface of the composite. The continuous outer surface can have other structural features (e.g., gaps, pores, etc.) but can still be considered a continuous outer surface. For example, as... Figure 2 As illustrated schematically, composite 100 may have an outer surface 101 based on a phase change material.

[0037] In some embodiments, one or more continuous outer surfaces (e.g., a first outer surface, a second outer surface, etc.) are possible. According to some embodiments, the first and second outer surfaces can be connected to each other, for example, such that the two outer surfaces form a continuous material through a composite. In some embodiments, for example, the first and second outer surfaces are connected to each other through a solid-phase material. As a non-limiting example, such as Figure 3 The diagram schematically illustrates that in composite 100, the first outer surface 301 and the second outer surface 302 can form a continuous material through a spacer. As another non-limiting example, such as... Figure 4 The diagram schematically illustrates that in composite 100, the first outer surface 401 and the second outer surface 402 are connected to each other by a solid material 102.

[0038] In some embodiments, the solid-phase material and the phase change material do not chemically react with each other. According to some embodiments, the absence of chemical bonds, such as metallic or covalent bonds, between the solid-phase material and the phase change material can indicate chemical inertness between them. The solid-phase material can be chemically inert in the presence of the phase change material. In some embodiments, the chemical inertness of the solid-phase material and the phase change material depends on temperature and / or the properties of both materials. The chemical inertness between the solid-phase material and the phase change material can be tested, for example, by differential scanning calorimetry (DSC) or other techniques. In some embodiments, by DSC, the solid-phase material and the phase change material do not exhibit a phase change at or near (e.g., within + / - 10 °C) the melting temperature of the phase change material. In some cases, by DSC, the phase change material and the solid-phase material exhibit no more than two phase changes. In some other cases, by DSC, the phase change material and the solid-phase material exhibit three phase changes, where at least one phase change is substantially less abundant than the others (e.g., less than 1 wt%).

[0039] Composites can exhibit thermal resistance. According to some embodiments, the thermal resistance of a composite may be important for various reasons (e.g., heat dissipation, heat retention, thermal gradient, etc.). Thermal resistance can depend on the resulting structure and / or composition of the composite. Techniques for determining thermal resistance include, for example, those discussed in the standard test method ASTM D5470. In some cases, thermal resistance can be determined using a fixture capable of performing ASTM D5470 testing at a pressure of 206.8 kPa (30 psi). According to some embodiments, the ASTM D5470 test includes techniques for measuring and calculating thermal resistance. The ASTM D5470 test can be the ASTM D5470-17 test.

[0040] In some embodiments, the thermal resistance of the composite is less than 1 mm. 2 K / W, less than 3mm 2K / W, less than 5mm 2 K / W, less than 7mm 2 K / W, less than 10mm 2 K / W, less than 15mm 2 K / W, less than 20mm 2 K / W, less than 30mm 2 K / W, less than 40mm 2 K / W, or less than 50mm 2 K / W. According to some embodiments, when the composite is above the melting temperature, the thermal resistance can have a certain value (e.g., less than 7 mm). 2 K / W or less than 5mm 2 (e.g., K / W). In some cases, thermal impedance includes the original thermal impedance. In other cases, thermal impedance includes thermal resistance.

[0041] In some respects, the composite can also exhibit effective thermal conductivity, which combines bulk thermal conductivity and surface contact thermal resistance. According to some embodiments, the effective thermal conductivity of the composite may be important for various reasons (e.g., heat dissipation, heat retention, thermal gradient, etc.). Effective thermal conductivity can depend on the resulting structure and / or composition of the composite. Techniques for determining effective thermal conductivity include, for example, those discussed in the standard test method ASTM D5470, or those using a fixture capable of performing ASTM D5470 tests at a pressure of 206.8 kPa (30 psi).

[0042] In some embodiments, the effective thermal conductivity of the composite is determined above the melting temperature. For example, the temperature at which the effective thermal conductivity is determined may be at least 5°C, at least 10°C, at least 15°C, at least 20°C, or at least 25°C above the melting temperature. In some cases, the temperature may be no more than 25°C, no more than 20°C, no more than 15°C, no more than 10°C, or no more than 5°C above the melting temperature. In some cases, the determination may be performed within any combination of these ranges.

[0043] In some embodiments, the composite may also have any of a variety of suitable effective thermal conductivities. In some aspects, the effective thermal conductivity of the composite may be advantageously high. In some embodiments, for example, the composite has an average effective thermal conductivity greater than or equal to 3 W / mK, greater than or equal to 5 W / mK, greater than or equal to 10 W / mK, greater than or equal to 50 W / mK, greater than or equal to 100 W / mK, greater than or equal to 300 W / mK, greater than or equal to 500 W / mK, greater than or equal to 700 W / mK, or greater than or equal to 900 W / mK. In some embodiments, the composite has an average effective thermal conductivity less than or equal to 1000 W / mK, less than or equal to 900 W / mK, less than or equal to 700 W / mK, less than or equal to 500 W / mK, less than or equal to 300 W / mK, less than or equal to 100 W / mK, less than or equal to 50 W / mK, less than or equal to 10 W / mK, or less than or equal to 5 W / mK. Combinations of the ranges listed above are also possible (e.g., a composite having an average effective thermal conductivity greater than or equal to 3 W / mK and less than or equal to 1000 W / mK, or a composite having an average thermal conductivity greater than or equal to 100 W / mK and less than or equal to 300 W / mK). Other ranges are also possible, as this disclosure is not limiting in this respect.

[0044] In some cases, the composite can retain its structure after heating at a temperature higher than the melting temperature of the phase change material. According to some embodiments, the composite can retain its structure after heating, for example, at the temperatures described herein, for at least 1,000 hours, at least 700 hours, at least 500 hours, at least 250 hours, at least 100 hours, at least 10 hours, at least 1 hour, or less than one hour. For example, the temperature may be at least 5°C, at least 10°C, at least 15°C, at least 20°C, at least 25°C, at least 30°C, at least 40°C, at least 50°C, at least 60°C, at least 70°C, at least 80°C, at least 90°C, at least 100°C, or at least 150°C above the melting temperature. In some cases, the temperature may be no more than 150°C, 100°C, 90°C, 80°C, 70°C, 60°C, 50°C, 40°C, 30°C, 25°C, 20°C, 15°C, 10°C, or 5°C higher than the melting temperature. In some cases, combinations of these ranges are also possible. Under such temperatures or other conditions and / or for such durations, the composite may not exhibit any significant permanent changes, such as cracking, leakage (e.g., leakage of a phase change material), permanent deformation, etc.

[0045] Solid-phase materials can include a variety of materials, such as foamed metals (e.g., active or inactive foamed metals), porous metal solids, passivated metal particles, fibers, foamed carbon, carbon paper, carbon nanoparticles, carbon nanotubes, graphene nanosheets, polymer foams, polymer paper, organic foams, organic paper, foam ceramics, carbon-based particles, ceramic particles, ceramic nanosheets, and so on. In various embodiments, one or more of these materials and / or other materials may be present in the composite. The following are non-limiting examples of such solid-phase materials.

[0046] For example, in some embodiments, the solid material may include multiple fibers (e.g., carbon fibers). In some embodiments, the multiple fibers are multiple discontinuous fibers (e.g., discontinuous carbon fibers). In some aspects, the multiple fibers may be substantially orthogonally aligned with the substrate. Further details regarding the substrate and the multiple fibers are explained in more detail herein, including, for example, suitable types of fibers, suitable fiber lengths, suitable fiber diameters, suitable methods for producing the substrate, etc. In some embodiments, the solid material includes multiple fibers, wherein the fibers define the substrate. The multiple fibers defining the substrate may be substantially aligned. According to some embodiments, the substantially aligned fibers are at least 10 vol%, at least 20 vol%, at least 30 vol%, at least 50 vol%, at least 60 vol%, or at least 70 vol% of the fibers defining the substrate. According to a non-limiting embodiment, at least 30 vol% of the fibers defining the substrate are substantially aligned.

[0047] In some embodiments, the solid-phase material includes a foamed metal. The foamed metal may comprise a material having porosity. For example, the foamed metal may be a porous copper alloy foamed metal that can exhibit the properties of a non-foamed copper alloy. According to some embodiments, the foamed metal is a solid-phase material that can form a composite with a phase change material. For example, the porosity of the foamed metal may be at least 50 vol%, at least 60 vol%, at least 70 vol%, at least 80 vol%, or at least 90 vol%.

[0048] According to one set of embodiments, the foam metal may include an active metal. The active metal may include metals such as copper, silver, gold, nickel, zinc, platinum, iron, etc. Additionally, according to some embodiments, the foam metal may include an inactive metal. Non-limiting examples include titanium, tungsten, vanadium, chromium, hafnium, molybdenum, neodymium, zirconium, etc. The foam metal may also be an alloy of active foam metal components and / or inactive foam metal components.

[0049] In some embodiments, the foam metal may have a protective layer, for example, to prevent or inhibit chemical reactions between the foam metal and the phase change material. In some embodiments, having a protective layer may be advantageous, for example, to prevent chemical reactions (e.g., oxidation reactions) and / or to maintain the chemical composition of the foam metal's surface. For example, according to one set of embodiments, a portion of the surface of aluminum or another foam metal material may be covered with an anodized surface. According to another set of embodiments, the foam metal (such as foam copper metal) may have a protective layer, for example, which covers and / or protects at least a portion of its surface.

[0050] According to some embodiments, the solid-phase material may include a porous metallic solid. The porous metallic solid can be any suitable metallic solid known in the art (e.g., a honeycomb metal). The solid may include different topologies, structures, degrees of order, etc. For example, a porous metallic solid may include a honeycomb structure of pores in which a phase change material may be present. For example, a porous metallic solid may contain nickel or other materials, any of those described herein. In some embodiments, the porous metallic solid is formed by powder metallurgy, particle sintering, or other techniques.

[0051] In some embodiments, the solid-phase material may include a passivation layer. For example, the solid-phase material may include metal particles, such as metal particles with a passivation layer that protects the metal from reacting with other substances (e.g., preventing alloying of the metal). The metal in the metal particles may be any suitable metal known in the art, such as copper, silver, nickel, zinc, platinum, iron, etc. In some embodiments, the metal particles may have a passivation layer (e.g., copper oxide) that can prevent alloying and / or undesirable chemical reactions. In some cases, the passivation layer can protect the metal surface from chemical reactions with phase change materials, other solid-phase material components, and / or chemicals in the environment. In some embodiments, the passivation layer may include an active passivation layer and / or an inactive passivation layer.

[0052] In some embodiments, the solid-phase material comprises carbon foam. The carbon foam may have a porous, permeable structure that allows for the introduction of phase change materials. The carbon foam may possess a degree of rigidity, porosity, thermal resistance, etc., which can provide various advantages to the system (e.g., cost-effective manufacturing). For example, the porosity of the carbon foam may be at least 50 vol%, at least 60 vol%, at least 70 vol%, at least 80 vol%, or at least 90 vol%.

[0053] According to some embodiments, the solid material may include carbon paper. In some cases, the carbon paper may be porous, allowing the introduction of solid materials. For example, the porosity of foamed carbon may be at least 50 vol%, at least 60 vol%, at least 70 vol%, at least 80 vol%, or at least 90 vol%.

[0054] In some embodiments, the solid-phase material includes a non-foamed metal. Non-limiting foams include polyethylene foam (e.g., low-density polyethylene foam), polystyrene foam, rubber-based foam, etc. As another non-limiting example, polystyrene foam can be chemically inert to the phase change material.

[0055] In some embodiments, the solid-phase material comprises a non-foamed metal with a metallization surface treatment. Some foams may include polyethylene foam (e.g., low-density polyethylene foam), polystyrene foam, rubber-based foam, etc. As another non-limiting example, polystyrene foam may be chemically inert to the phase change material. Non-limiting metallization surface treatments may include nickel, silver, gold, and / or alloys thereof, etc.

[0056] In some embodiments, the solid-phase material includes non-metallic paper. The non-metallic paper may include, for example, polymeric paper. The paper may comprise, for example, a single sheet or multiple sheets having a porous structure. In some cases, the paper (e.g., cellulose filter paper) may have small pores (e.g., less than 30 micrometers) and may contain a phase change material, such as those discussed herein.

[0057] In some embodiments, the solid-phase material comprises a non-metallic paper having a metallized surface. The non-metallic paper may include, for example, polymeric paper. The paper may comprise, for example, a single sheet or multiple sheets having a porous structure. In some cases, the paper (e.g., cellulose filter paper) may have small pores (e.g., less than 30 micrometers) and may contain a phase change material. Non-limiting examples of metal / metal alloys present in the metallized surface include nickel, silver, gold, and alloys thereof.

[0058] In some embodiments, the solid-phase material includes foamed ceramics. Foamed ceramics are foams containing ceramics. Non-limiting examples include silicon carbide, alumina, silicon dioxide, etc.

[0059] In some embodiments, the solid-phase material may include carbon-based particles. Carbon-based particles may include graphite, graphene, carbon fibers, carbon nanotubes, etc. Carbon-based particles may have different structures and / or geometries. For example, carbon-based particles may be spherical, plate-like, cylindrical, etc.

[0060] In some embodiments, particles such as carbon-based particles, ceramic particles, etc., may have an average size of at least 0.1 micrometers, at least 0.5 micrometers, at least 1 micrometer, at least 2 micrometers, at least 5 micrometers, at least 10 micrometers, at least 20 micrometers, at least 30 micrometers, at least 40 micrometers, at least 50 micrometers, at least 75 micrometers, at least 100 micrometers, at least 200 micrometers, at least 300 micrometers, at least 400 micrometers, or at least 500 micrometers. According to some embodiments, the average size of the particles may be no more than 500 micrometers, no more than 400 micrometers, no more than 300 micrometers, no more than 200 micrometers, no more than 100 micrometers, no more than 75 micrometers, no more than 50 micrometers, no more than 40 micrometers, no more than 30 micrometers, no more than 20 micrometers, no more than 10 micrometers, no more than 5 micrometers, no more than 2 micrometers, no more than 1 micrometer, no more than 0.5 micrometers, or no more than 0.1 micrometers. The particles may have substantially similar sizes, or the particles may exhibit a range of sizes or dimensions, etc.

[0061] In some embodiments, the solid-phase material is ceramic particles. Some non-limiting examples of ceramic particles are silicon carbide, silicon nitride, boron nitride, alumina, zinc oxide, titanium dioxide, silicon dioxide, zirconium dioxide, iron oxide, calcium oxide, magnesium oxide, and barium oxide. Ceramic particles can be shaped into different structures and / or geometries. For example, ceramic particles can be spherical, plate-like, and / or cylindrical.

[0062] In some embodiments, the ceramic particles may have a range of average sizes. According to some embodiments, the ceramic particles may have an average size of at least 0.1 micrometers, at least 0.5 micrometers, at least 1 micrometer, at least 2 micrometers, at least 5 micrometers, at least 10 micrometers, at least 20 micrometers, at least 30 micrometers, at least 40 micrometers, at least 50 micrometers, at least 75 micrometers, at least 100 micrometers, at least 200 micrometers, at least 300 micrometers, at least 400 micrometers, or at least 500 micrometers. According to some embodiments, the ceramic particles may have an average size of no more than 500 micrometers, no more than 400 micrometers, no more than 300 micrometers, no more than 200 micrometers, no more than 100 micrometers, no more than 75 micrometers, no more than 50 micrometers, no more than 40 micrometers, no more than 30 micrometers, no more than 20 micrometers, no more than 10 micrometers, no more than 5 micrometers, no more than 2 micrometers, no more than 1 micrometer, no more than 0.5 micrometers, or no more than 0.1 micrometers. The particles may have substantially similar sizes, or the particles may exhibit a range of sizes or dimensions, etc.

[0063] In some embodiments, the compound does not contain flux. Flux is typically a material that can have different uses, including but not limited to soft soldering, melting, and / or hard soldering. Some benefits of flux are the removal of chemicals (e.g., oxides) and potential contaminants. Flux can be made from a single component (e.g., zinc chloride) or multiple components (e.g., silica and borax).

[0064] In some embodiments, the solid-phase material comprises a metal, alloy, carbon-based material, conductive polymer, and / or a combination thereof. The solid-phase material may comprise any of a variety of suitable metals and / or alloys. In some embodiments, for example, the metal and / or alloy includes aluminum (Al), titanium (Ti), nickel (Ni), zirconium (Zr), niobium (Nb), tantalum (Ta), hafnium (Hf), stainless steel (SS), and / or a combination thereof. In some embodiments, the metal and / or alloy comprises metal and / or alloy foil. In some embodiments, the metal and / or alloy comprises metal and / or alloy particles. Other metals and / or alloys are also possible, as this disclosure is not intended to be limiting in this respect.

[0065] In some embodiments, the solid-phase material may comprise any of a variety of suitable carbon-based materials. In some embodiments, for example, the carbon-based material includes graphite, graphene, carbon nanostructures (e.g., carbon nanotubes, carbon nanowires, etc.), carbon black, and / or combinations thereof. In some aspects, the carbon-based material may comprise powders (e.g., carbon and / or graphite powder) or fibers (e.g., carbon and / or graphite fibers). Other carbon-based materials are also possible, as this disclosure is not limiting in this respect.

[0066] Some embodiments discussed herein generally involve fiber volume fractions of at least 40% fiber volume, at least 45% fiber volume, at least 50% fiber volume, at least 55% fiber volume, at least 60% fiber volume, at least 65% fiber volume, at least 70% fiber volume, etc. (e.g., the fiber volume fraction of substantially aligned fibers, as discussed herein).

[0067] In various embodiments, various techniques can be used to align fibers (e.g., discontinuous fibers), including magnetic fields, shear flow, etc., as discussed in more detail below. As a non-limiting example, magnetic particles (including those discussed herein) can be attached to fibers, and then magnetic fields can be used to manipulate the magnetic particles. For example, magnetic fields can be used to move magnetic particles into a composite and / or to align fibers within the composite. Magnetic fields can be constant or time-varying (e.g., oscillating), for example, as discussed herein. For example, an applied magnetic field can have a frequency from 1 Hz to 500 Hz and an amplitude from 0.01 T to 10 T. Other examples of magnetic fields are described in more detail below.

[0068] In some cases, fibers (e.g., discontinuous fibers) may have any of a variety of suitable lengths. In some embodiments, for example, the fibers have an average length or characteristic dimension of at least 1 nm, at least 3 nm, at least 5 nm, at least 10 nm, at least 30 nm, at least 50 nm, at least 100 nm, at least 300 nm, at least 500 nm, at least 1 micrometer, at least 3 micrometer, at least 5 micrometer, at least 10 micrometer, at least 20 micrometer, at least 30 micrometer, at least 50 micrometer, at least 100 micrometer, at least 200 micrometer, at least 300 micrometer, at least 500 micrometer, at least 1 mm, at least 2 mm, at least 3 mm, at least 5 mm, at least 10 mm, at least 15 mm, etc. In some embodiments, the fibers may have an average length or characteristic dimension not exceeding 5 cm, 3 cm, 2 cm, 1.5 cm, 1 cm, 5 mm, 3 mm, 2 mm, 1 mm, 500 μm, 300 μm, 200 μm, 100 μm, 50 μm, 30 μm, 20 μm, 10 μm, 50 μm, 30 μm, 20 μm, 10 μm, 5 μm, 3 μm, 1 μm, 500 nm, 300 nm, 100 nm, 50 nm, 30 nm, 10 nm, 50 nm, 30 nm, 10 nm, 5 nm, etc. Any combination of these is also possible. For example, multiple fibers may have an average length between 1 mm and 5 mm.

[0069] Additionally, the fibers (e.g., discontinuous fibers) can have any suitable average diameter. For example, fibers can have an average diameter of at least 5 micrometers, at least 10 micrometers, at least 20 micrometers, at least 30 micrometers, at least 50 micrometers, at least 100 micrometers, at least 200 micrometers, at least 300 micrometers, at least 500 micrometers, at least 1 mm, at least 2 mm, at least 3 mm, at least 5 mm, at least 1 cm, at least 2 cm, at least 3 cm, at least 5 cm, at least 10 cm, etc. In some embodiments, the fibers can have an average diameter not exceeding 10 cm, not exceeding 5 cm, not exceeding 3 cm, not exceeding 2 cm, not exceeding 1 cm, not exceeding 5 mm, not exceeding 3 mm, not exceeding 2 mm, not exceeding 1 mm, not exceeding 500 micrometers, not exceeding 300 micrometers, not exceeding 200 micrometers, not exceeding 100 micrometers, not exceeding 50 micrometers, not exceeding 30 micrometers, not exceeding 20 micrometers, not exceeding 10 micrometers, not exceeding 5 micrometers, etc. Any combination of these is also possible. For example, fibers can have an average diameter between 5 micrometers and 50 micrometers, between 10 micrometers and 100 micrometers, between 50 micrometers and 500 micrometers, between 100 micrometers and 5 mm, etc.

[0070] In some embodiments, the fibers (e.g., discontinuous fibers) may have an average length of at least 10 times or at least 50 times their thickness or diameter. In some cases, the fibers may have an average aspect ratio (the ratio of fiber length to diameter or thickness) of at least 3, at least 5, at least 10, at least 30, at least 50, at least 100, at least 300, at least 500, at least 1,000, at least 3,000, at least 5,000, at least 10,000, at least 30,000, at least 50,000, or at least 100,000. In some cases, the average aspect ratio of the fibers may be less than 100,000, less than 50,000, less than 30,000, less than 10,000, less than 5,000, less than 3,000, less than 1,000, less than 500, less than 300, less than 100, less than 50, less than 30, less than 10, less than 5, etc. In some cases, any combination of these is also possible; for example, the aspect ratio can be between 5 and 100,000.

[0071] In some cases, fibers (e.g., discontinuous fibers) may constitute a relatively large portion of the composite. For example, in some embodiments, fibers may constitute at least 1%, at least 2%, at least 3%, at least 4%, at least 5%, at least 7%, at least 10%, at least 15%, at least 20%, at least 25%, at least 30%, at least 35%, at least 40%, at least 45%, at least 50%, at least 55%, at least 60%, at least 65%, at least 70%, at least 75%, at least 80%, at least 85%, at least 90%, at least 95%, or at least 97% of the mass or volume of the composite. In some cases, fibers may constitute no more than 97%, no more than 95%, no more than 90%, no more than 85%, no more than 80%, no more than 70%, no more than 60%, no more than 50%, no more than 40%, no more than 30%, no more than 20%, or no more than 10% of the mass or volume of the composite. Any combination of these is also possible.

[0072] At least some of the fibers (e.g., discontinuous fibers) may be uncoated. However, in some cases, some or all of the fibers (e.g., discontinuous fibers) may be coated. The coating may be used, for example, to promote the adsorption or binding of particles (such as magnetic particles) to the fiber, or for other reasons.

[0073] As a non-limiting example, at least some of the fibers are coated with an adhesive. Examples of coatings or adhesives include, but are not limited to, polypropylene, polyurethane, polyamide, oxyresin, polyimide, epoxy resin, etc. These can be introduced, for example, as solutions, dispersions, emulsions, etc. As other examples, the fibers can be coated with surfactants, silane coupling agents, epoxy resins, glycerol, polyurethane, organometallic coupling agents, etc. Non-limiting examples of surfactants include oleic acid, sodium dodecyl sulfate, sodium lauryl sulfate, etc. Non-limiting examples of silane coupling agents include silane coupling agents based on amino-, benzylamino-, chloropropyl-, disulfide-, epoxy resin-, epoxy resin / melamine-, mercapto-, methacrylate-, tertiary thio-, ureo-, vinyl-, isocyanate-, and vinyl-benzyl-amino. Non-limiting examples of organometallic coupling agents include organometallic coupling agents based on aryl- and vinyl-.

[0074] It should be understood that not all particles (if present) must be magnetic. In some cases, non-magnetic particles may be used, for example, in addition to and / or instead of magnetic particles. Non-limiting examples of non-magnetic particles include glass, polymers, metals, etc. Furthermore, in some embodiments, no particles are present.

[0075] The particles (if present) may be spherical or non-spherical and may have any suitable shape or size. The particles may be relatively monodisperse or within a certain size range. In some cases, the particles may have an average characteristic size of at least 10 micrometers, at least 20 micrometers, at least 30 micrometers, at least 50 micrometers, at least 100 micrometers, at least 200 micrometers, at least 300 micrometers, at least 500 micrometers, at least 1 mm, at least 2 mm, at least 3 mm, at least 5 mm, at least 1 cm, at least 1.5 cm, at least 2 cm, at least 3 cm, at least 5 cm, at least 10 cm, etc. The particles may also have an average characteristic size not exceeding 10 cm, not exceeding 5 cm, not exceeding 3 cm, not exceeding 2 cm, not exceeding 1.5 cm, not exceeding 1 cm, not exceeding 5 mm, not exceeding 3 mm, not exceeding 2 mm, not exceeding 1 mm, not exceeding 500 micrometers, not exceeding 300 micrometers, not exceeding 200 micrometers, not exceeding 100 micrometers, not exceeding 50 micrometers, not exceeding 30 micrometers, not exceeding 20 micrometers, not exceeding 10 micrometers, etc. Any combination of these is also possible. For example, particles can exhibit characteristic sizes between 100 micrometers and 1 mm, or between 10 micrometers and 10 micrometers. The characteristic size of a non-spherical particle can be considered as the diameter of a perfect sphere with the same volume as the non-spherical particle.

[0076] Additionally, in some aspects, the composite may further comprise fillers or other materials, for example, in addition to fibers (e.g., discontinuous fibers). For example, in some embodiments, the composite may further comprise one or more ceramics, such as boron nitride, alumina, titanium dioxide, etc. Additionally, in some embodiments, the composite may further comprise one or more metals, such as aluminum, copper, silver, tin, gold, etc. Furthermore, in one embodiment, such materials present within the composite can be formed, for example, by fusing particles together during the formation of the composite. Similarly, in some cases, other materials may also be present in the substrate.

[0077] In one set of embodiments, an adhesive is also present within the composite, for example, it can be used to bond fibers (e.g., discontinuous fibers) within the composite. For example, the adhesive can facilitate holding the fibers in place within the composite. However, it should be understood that the adhesive is optional and not necessary in all cases. In some cases, the adhesive may include a resin. The adhesive may include, for example, thermosetting materials, thermoplastic materials, and / or vitrifiers. In some embodiments, the adhesive may include thermoplastic solutions, thermoplastic melts, thermoplastic granules, thermosetting resins, volatile compounds (such as volatile organic compounds), water, or oil. Other non-limiting examples of adhesives include epoxy resins, polyesters, vinyl esters, polyethyleneimine, polyetherketone ketones, polyaryl etherketones, polyetheretherketones, polyphenylene sulfide, polyethylene terephthalate, polycarbonate, poly(methyl methacrylate), acrylonitrile-butadiene-styrene, polyacrylonitrile, polypropylene, polyethylene, nylon, silicone rubber, polyvinylidene fluoride, styrene-butadiene rubber, or pre-ceramic monomers, siloxanes, silazanes, or carbosilanes. In some cases, the adhesive may comprise a covalent network polymer prepared by an imine-linked oligomer and an independent crosslinking agent containing an active moiety. Non-limiting examples of the active moiety include epoxy resins, isocyanates, bismaleimides, sulfides, polyurethanes, acid anhydrides, and / or polyesters. Examples of glass-like polymers include, but are not limited to, epoxy resins based on bisphenol A diglycidyl ether, aromatic polyesters, polylactic acid (polylactide), polyhydroxycarbamates, epoxidized soybean oil with citric acid, polybutadiene, etc. In some embodiments, the adhesive may also include a mixture comprising any one or more of these materials and / or other materials.

[0078] In some embodiments, the adhesive may constitute at least 1%, at least 2%, at least 3%, at least 4%, at least 5%, at least 7%, at least 10%, at least 15%, at least 20%, or at least 25% of the composite mass, and / or no more than 25%, no more than 20%, no more than 15%, no more than 10%, no more than 7%, no more than 5%, no more than 4%, no more than 3%, no more than 2%, or no more than 1% of the composite mass.

[0079] According to certain embodiments, the composite as described herein may comprise one or more additives and / or fillers. In some embodiments, for example, the additives and / or fillers may comprise one or more second conductive materials dispersed in one or more components of the composite. In some embodiments, at least a portion of the additives and / or fillers is in electrical contact with at least a portion of the composite.

[0080] Any of a variety of suitable additives and / or fillers can be used. In some embodiments, for example, the additives and / or fillers comprise carbon-based materials. Suitable carbon-based materials include, but are not limited to, graphite, graphene, carbon nanostructures (e.g., carbon nanotubes, carbon nanowires, etc.), carbon black, and / or combinations thereof. In some aspects, the carbon-based material can be a powder (e.g., carbon and / or graphite powder) or a fiber (e.g., carbon and / or graphite fiber). Other carbon-based materials are also possible.

[0081] In some embodiments, the additives and / or fillers comprise metals and / or alloys. Suitable metals and / or alloys include aluminum (Al), titanium (Ti), nickel (Ni), stainless steel (SS), and / or combinations thereof. In some embodiments, the additives and / or fillers comprise polymers (e.g., conductive polymers, non-conductive polymers). In some embodiments, the additives and / or fillers comprise colorants and / or dyes. Other additives and / or fillers are also possible.

[0082] Certain aspects generally relate to methods for preparing any of the composites described herein. Non-limiting examples include, but are not limited to, mechanical mixing; ultrasonic mixing; casting; spraying; cold spraying; liquefaction and curing; casting and curing; electrowetting; electromagnetic mixing; pressing / rolling cryogenically ground particles; immersion; pressing; and so on.

[0083] For example, in some embodiments, the composite is formed by, for example, mechanically mixing a phase change material and a solid material. Mechanical mixing can be performed, for example, by a mixer or agitator, which allows the solid material and the phase change material to be mixed together.

[0084] In some embodiments, the composite is formed by ultrasonic mixing of a solid material and a phase change material. Ultrasonic mixing can be achieved, for example, by ultrasonically treating the solid material and the phase change material at an ultrasonic frequency (i.e., greater than 20 kHz).

[0085] In some embodiments, the composite is formed by casting a phase change material onto a solid material. The phase change material can be cast onto the solid material to form the composite, wherein, according to some embodiments, the phase change material can be a liquid that becomes solid (i.e., solidifies) after casting. In some embodiments, the casting of the phase change material can be carried out in a pressure chamber capable of applying a positive pressure (i.e., greater than 1 atm) or a negative pressure (i.e., less than 1 atm) during casting.

[0086] In some embodiments, a phase change material is sprayed onto a solid material to form a composite. According to some embodiments, spraying the phase change material may be advantageous for various reasons (e.g., uniform dispersion of the phase change material). Spraying the phase change material onto a solid material can be employed in various situations (e.g., roll-to-roll manufacturing), etc.

[0087] In some embodiments, spraying phase change materials may include cold spraying. During cold spraying, the phase change material (e.g., metal particles) is accelerated in a gaseous medium and then deposited onto a solid material, thereby facilitating the formation of the composite. Cold spraying can be performed using various techniques, such as a robotic arm equipped with a cold spray nozzle.

[0088] In some embodiments, the composite is formed by melting a phase change material onto a solid material. In some cases, the phase change material can be a solid that is deposited on a solid material, subsequently heated and liquefied, and then cooled and solidified on the solid material. In some embodiments, the liquefaction and solidification of the phase change material occur under applied pressure (e.g., in a pressure chamber with applied positive or negative pressure).

[0089] In some embodiments, the composite is formed by casting a phase change material (e.g., a liquid phase change material) onto a solid material. In some embodiments, the phase change material is cured (e.g., cooled) after casting the liquid phase material. According to some embodiments, the composite (e.g., a self-supporting composite) is formed after the phase change material has been cured.

[0090] In some embodiments, the composite is formed by electrowetting a solid-phase material. Electrowetting can occur by applying a voltage (e.g., a DC voltage) to the solid-phase material. Electrowetting on a solid-phase material may be advantageous for various reasons (e.g., to alter the wetting properties of the material). In some cases, it may be preferable to form the composite by introducing a phase change material while electrowetting the solid-phase material.

[0091] In some embodiments, electromagnetic mixing (i.e., electromagnetic stirring) can form a composite. It should be understood that electromagnetic mixing involves phase change materials capable of interacting with a magnetic field (e.g., a magnetic field from a static induction coil). In some cases, such a magnetic field can facilitate the mixing of phase change materials and solid-phase materials to form a composite.

[0092] In some embodiments, the phase change material is a cryo-milled phase change material. It may be desirable to use a cryo-milled phase change material to form a composite when the phase change material is difficult to process at room temperature (e.g., forming clumps / clusters). The cryo-milled phase change material can be cryo-milled particles, which can be milled under cryo-milling conditions (e.g., below -50°C). In some embodiments, the cryo-milled particles are mixed with a solid phase material (e.g., polymer particles). In such embodiments, the cryo-milled particles and solid phase material can be pressed and / or rolled together to form a composite.

[0093] In some embodiments, the phase change material is a liquid phase change material, wherein the solid phase material is immersed in the liquid phase change material. In some cases, immersing the solid phase material in the liquid phase change material may be advantageous (e.g., if processability is challenging). When the phase change material is liquid, immersion of the solid phase material in the liquid phase change material can occur at temperatures above room temperature (e.g., above 35°C), and, according to some embodiments, the phase change material and the solid phase material can subsequently be cooled to form a composite.

[0094] In some embodiments, where the phase change material is solid, a composite is formed by pressing the solid phase change material and the solid phase material together. Pressing the solid phase change material and the solid phase material can be performed by any of a variety of methods known in the art (e.g., rolling mill). In some cases, pressing the solid phase change material and the solid phase material can form a composite having components that are substantially adhered to each other.

[0095] The following documents are incorporated herein by reference in their entirety: International Patent Application Publication Nos. WO 2018 / 175134, WO2020 / 123334, WO 2021 / 007381, WO 2021 / 007389, WO 2023 / 163848, and WO 2024 / 039598. Additionally, International Patent Application Serial No. PCT / US24 / 35747 is also incorporated herein by reference in its entirety.

[0096] The following examples are intended to illustrate certain embodiments of this disclosure, but do not represent the full scope of this disclosure.

[0097] Example 1

[0098] This example relates to mechanically stirred carbon fibers and liquid metal. Pitch-derived carbon fibers are mechanically stirred in a mixture of gallium and gallium oxide to produce a slurry with a fiber composition greater than 10% by volume. The slurry is then heated to above 30°C and cast onto a surface under a magnetic field of less than 5T to orient the fibers in a direction perpendicular to the casting surface. The resulting cast film is cooled to room temperature to produce a self-supporting composite film.

[0099] A cross-sectional optical micrograph of the self-supporting composite membrane is shown below. Figure 5 middle.

[0100] Example 2

[0101] This example describes a fixture capable of performing ASTM D5470 tests, and the techniques for using it. See also ASTM D5470-17, which is incorporated herein by reference in its entirety.

[0102] The general features of an apparatus that satisfies the requirements of this method are shown in Figure 6A and Figure 6B This device applies the required test conditions and performs the necessary measurements. It is a possible engineering solution, not the only exclusive implementation.

[0103] The test surface is smooth within 0.4 micrometers and parallel within 5 micrometers.

[0104] The heat source is either an electric heater or a temperature-controlled fluid circulator. A typical electric heater is made by embedding a wire-wound cylinder heater within a block of highly conductive metal. A circulating fluid heater consists of a metal block heat exchanger through which a temperature-controlled fluid circulates to provide the required heat flow and temperature control.

[0105] Regardless of the type of heater used, the heat flow through the sample can be measured with a measuring rod.

[0106] Electric heaters offer convenient measurement of the heating power generated, but must be combined with protective heaters and high-quality insulation to limit heat leakage from the main flow through the sample.

[0107] The heat flow metering rod can be constructed from a highly conductive material with documented thermal conductivity over the temperature range of interest. For accurate heat flow measurement, the temperature sensitivity of thermal conductivity must be considered. A thermal conductivity greater than 50 W / m·K is recommended for the rod material.

[0108] The protective heater consists of a thermal shield surrounding the main heat source to eliminate heat leakage to the environment. The protective heater is insulated from the heat source and maintained at a temperature within + / - 0.2 K of the heater. This effectively reduces heat leakage from the main heater by eliminating the temperature difference across the insulation layer. The insulation layer between the protective heater and the heat source will be at least equivalent to a 5 mm thick layer of FR-4 epoxy material.

[0109] If the heat flow metering rod is used on both the hot and cold surfaces, then a protective heater and thermal insulation layer are not required, and the heat flow through the test sample is calculated as the average heat flow through the two metering rods.

[0110] By extrapolating a linear array of metering bar temperatures to the test surface, the metering bar can also be used to determine the temperature of the test surface. This can be done for both hot-side and cold-side metering bars. Surface temperature can be measured using thermocouples positioned very close to the surface, although this may be mechanically difficult to achieve. The metering bar can be used for both heat flow measurement and surface temperature measurement, or specifically for one of these functions.

[0111] The cooling unit is typically implemented using a metal block cooled by a temperature-controlled circulating fluid with a temperature stability of + / -0.2K.

[0112] The contact pressure on the specimen can be controlled and maintained in various ways, including linear actuators, lead screws, pneumatic devices, and hydraulic devices. The desired range of force must be applied to the test fixture in a direction perpendicular to the test surface, while maintaining the parallelism and alignment of the surfaces.

[0113] The material type will determine the method used to control the specimen thickness. In all cases, a specimen with the same area as the contact test surface is prepared. If the test surface sizes are unequal, a specimen with dimensions equal to the smaller test surface is prepared.

[0114] Type I – Uses shims or mechanical stops to control the thickness of the specimen between test surfaces. Spacer beads with the desired diameter can also be used at a volume ratio of approximately 2%, and should be thoroughly mixed into the sample before being applied to the test surface.

[0115] Type II - Uses adjustable clamping pressure to deflect the test specimen by 5% of its uncompressed thickness. This represents a trade-off between lower surface contact resistance and excessive sample deflection.

[0116] Type III - The sample thickness is measured according to Test Method C of Test Method D374.

[0117] Prepare specimens from materials in their original, as-is manufacturing condition or as otherwise indicated. Remove any contaminants and dirt particles. Do not use solvents that will react with or contaminate the specimen.

[0118] Close the test stack and apply the required clamping pressure to the specimen to be tested.

[0119] Unless otherwise specified, turn on the heating and cooling units and stabilize them at the specified set points to obtain an average sample temperature of 50°C (the average of T2 and T3).

[0120] Zero the thickness measuring device (micrometer, LVDT, laser detector, encoder, etc.).

[0121] The machine does not have an in-situ thickness measurement device.

[0122] The sample thickness was measured at room temperature according to test method C of test method D374.

[0123] The sample is loaded onto the lower test stack.

[0124] Type I grease and paste materials are dispensed onto the surface of the lower test stack. The phase change compound is then melted to dispense it onto the stack.

[0125] Type II and Type III specimens were placed on the lower test stack.

[0126] Close the test stack and apply clamping pressure.

[0127] Type I materials tested with shims to control the test thickness only require sufficient pressure to extrude excess material and bring it into contact with the shims, without requiring too much pressure that would damage the surface of the test stack.

[0128] For machines with screw stops, electromechanical or hydraulic actuators that control the position of test stacks, the magnitude of the clamping pressure is not critical.

[0129] The temperature of the test stack is raised above the sample melting point to allow the phase change material to flow and permit the closure of the test stack. After the material has flowed, unless otherwise specified, the heating and cooling units are returned to the desired setpoints to maintain an average sample temperature of 50°C before the start of the test.

[0130] Type II materials require sufficient pressure to hold stacked specimens together and minimize interfacial thermal resistance. Excessive pressure can damage the specimens. For softer specimens, the pressure may be as low as 0.069 MPa (10 psi), or for harder specimens, it may be as high as 3.4 MPa (500 psi). Alternatively, for easily deformable Type II materials, a screw or linear actuator can be used to control the specimen thickness during testing.

[0131] Type III materials require sufficient pressure to expel excess thermal paste from the interface and flatten uneven samples. For flat samples with low-viscosity thermal paste, the pressure may be as low as 0.69 MPa (100 psi), or for uneven samples or when using high-viscosity thermal paste, the pressure may be as high as 3.4 MPa (500 psi).

[0132] Record the temperature of the measuring rod and the voltage and current applied to the electric heater at equilibrium. Equilibrium is reached when two sets of temperature readings obtained at 5-minute intervals under constant power differ by less than + / - 0.1°C, or if the change in thermal resistance within the 5-minute time span is less than 1% of the current thermal resistance.

[0133] Calculate the average sample temperature and thermal resistance. Label the calculated thermal resistance of the monolayer sample as the sample's "thermal resistance".

[0134] Measure the thermal resistance at least three different specimen thicknesses. Maintain the average temperature of the specimen at 50°C ± 2°C (unless otherwise specified) by reducing the heat flux as the specimen thickness increases.

[0135] For samples that need to be stacked to obtain different thicknesses, the thermal resistance of a single layer is measured first, then the thermal resistance of two layers stacked together is measured, and then the thermal resistance of three layers stacked together is measured.

[0136] For three samples A, B and C with different thicknesses, the thermal resistance of sample A was measured separately first, then the thermal resistance of sample B was measured separately, and then the thermal resistance of sample C was measured separately.

[0137] Although several embodiments of this disclosure have been described and illustrated herein, those skilled in the art will readily conceive of a variety of other means and / or structures for performing the functions described herein and / or obtaining the results and / or one or more advantages described herein, and such variations and / or modifications are each considered to be within the scope of this disclosure. More generally, those skilled in the art will readily understand that all parameters, dimensions, materials, and constructions described herein are intended to be exemplary, and actual parameters, dimensions, materials, and / or constructions will depend on one or more specific applications for which the teachings of this disclosure are intended. Those skilled in the art will recognize, or be able to determine, many equivalents of the specific embodiments of this disclosure described herein without the use of excessive conventional experimentation. Therefore, it should be understood that the foregoing embodiments are presented as examples only, and that this disclosure may be practiced in ways other than those specifically described and claimed within the scope of the appended claims and their equivalents. This disclosure relates to each individual feature, system, article of manufacture, material, kit, and / or method described herein. Furthermore, any combination of two or more such features, systems, articles of manufacture, materials, kits, and / or methods is included within the scope of this disclosure if such features, systems, articles of manufacture, materials, kits, and / or methods are not contradictory.

[0138] In the event of conflicting and / or inconsistent disclosures in this specification and other documents incorporated by reference, this specification shall prevail. If two or more documents incorporated by reference contain conflicting and / or inconsistent disclosures, the document with the later effective date shall prevail.

[0139] All definitions defined and used herein should be understood to take precedence over dictionary definitions, definitions incorporated by reference in other documents, and / or the general meaning of the defined terms.

[0140] As used herein in the specification and claims, the indefinite article “a / an” should be understood to mean “at least one / an” unless otherwise expressly stated.

[0141] As used herein in the specification and claims, the phrase “and / or” should be understood to mean “any one or two” of the elements so combined, that is, elements that exist together in some cases and separately in others. Multiple elements listed with “and / or” should be interpreted in the same way, that is, “one or more” of the elements so combined. In addition to the elements specifically indicated by the “and / or” clause, other elements may optionally be present, whether related to or unrelated to those specifically indicated elements. Thus, as a non-limiting example, when used in conjunction with open-ended language such as “comprising,” a reference to “A and / or B” may in one embodiment refer only to A (optionally including elements other than B); in another embodiment only to B (optionally including elements other than A); in yet another embodiment both A and B (optionally including other elements); and so on.

[0142] As used herein in the specification and claims, “or” should be understood to have the same meaning as “and / or” as defined above. For example, when separating items in a list, “or” or “and / or” should be interpreted as inclusive, meaning it includes at least one, but also includes multiple elements or more than one in the list of elements, as well as optional additional unlisted items. Only explicitly contrasting terms such as “only one” or “exact one” or, when used in the claims, “consisting of” will refer to multiple elements or exactly one element in the list of elements. In general, the term “or” as used herein should only be interpreted to indicate an exclusive alternative (e.g., “the other of one or two”) preceding an exclusive term such as “any one,” “one,” “only one,” or “exact one.”

[0143] As used herein in the specification and claims, the phrase “at least one” in relation to a list of one or more elements should be understood to mean any one or more elements selected from the list of elements, but not necessarily including at least one of each element specifically listed in the list of elements, and does not exclude any combination of elements in the list of elements. This definition also allows for the optional presence of elements other than those specifically indicated in the list of elements referred to by the phrase “at least one,” whether related to or unrelated to those specifically indicated elements. Thus, as a non-limiting example, “at least one of A and B” (or equivalently, “at least one of A or B,” or equivalently, “at least one of A and / or B”) may, in one embodiment, mean at least one A, optionally including more than one A, without B (and optionally including elements other than B); in another embodiment, mean at least one B, optionally including more than one B, without A (and optionally including elements other than A); in yet another embodiment, mean at least one A, optionally including more than one A, and at least one B, optionally including more than one B (and optionally including other elements); and so on.

[0144] When the word “about” is used in relation to numbers in this document, it should be understood that another embodiment of this disclosure includes numbers that are not modified by the presence of the word “about”.

[0145] It should also be understood that, unless expressly stated to the contrary, in any method claimed herein that includes more than one step or action, the order of the steps or actions of the method is not necessarily limited to the order in which the steps or actions of the method are listed.

[0146] In the claims and in the foregoing description, all conjunctions such as “comprising,” “including,” “carrying,” “having,” “containing,” “involving,” “holding,” “constituting,” etc., shall be understood as open-ended, that is, meaning including but not limited to. As described in Section 2111.03 of the United States Patent Office Manual of Patent Examining Procedures, only the conjunctions “constituting of” and “substantially consisting of” shall be closed or semi-closed conjunctions, respectively.

Claims

1. An article comprising: A self-supporting composite having a thickness between 10 micrometers and 1 mm, the composite comprising a solid phase material and a phase change material, the solid phase material comprising less than 90 vol% of open-pore volume, and the phase change material comprising a metal, a metal oxide, a metal alloy, or a combination thereof. The phase change material exhibits a melting temperature between 10°C and 65°C, and the composite has a thickness of less than 10 mm at temperatures 10°C above the melting temperature. 2 The thermal resistance in k / W, wherein when tested using a fixture capable of performing ASTM D5470 tests, is measured at a pressure of 206.8 kPa (30 psi).

2. An article comprising: A self-supporting composite having a thickness between 200 micrometers and 1 mm, the composite comprising a solid phase material and a phase change material, the solid phase material comprising less than 90 vol% of open-pore volume, and the phase change material comprising a metal, a metal oxide, a metal alloy, or a combination thereof. The phase change material exhibits a melting temperature between 10°C and 65°C, and the composite has a thickness of less than 10 mm at temperatures 10°C above the melting temperature. 2 The thermal resistance in k / W, wherein when tested using a fixture capable of performing ASTM D5470 tests, is measured at a pressure of 206.8 kPa (30 psi).

3. An article comprising: A self-supporting composite having a thickness between 10 micrometers and 1 mm, the composite comprising a solid-phase material and a phase change material that do not chemically react with each other, the composite being flux-free, the solid-phase material comprising less than 90 vol% of open-pore volume, and the phase change material comprising a metal, a metal oxide, a metal alloy, or a combination thereof. The phase change material exhibits a melting temperature between 10°C and 65°C, and the composite has a thickness of less than 10 mm at temperatures 10°C above the melting temperature. 2 The thermal resistance is K / W, and the composite contains 2 mm of the thermal resistance after 1000 hours at a temperature 5°C above the melting temperature. 2 The thermal resistance within K / W, wherein when tested using a fixture capable of performing ASTM D5470 testing, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

4. An article comprising: A self-supporting composite having a thickness between 200 micrometers and 1 mm, the composite comprising a solid-phase material and a phase change material that do not chemically react with each other, the composite being flux-free, the solid-phase material comprising less than 90 vol% of open-pore volume, and the phase change material comprising a metal, a metal oxide, a metal alloy, or a combination thereof. The phase change material exhibits a melting temperature between 10°C and 65°C, and the composite has a thickness of less than 10 mm at temperatures 10°C above the melting temperature. 2 The original thermal resistance in K / W, and wherein after 1000 hours at a temperature 5°C above the melting temperature, the composite contains 2 mm of the thermal resistance. 2 The thermal resistance within K / W, wherein when tested using a fixture capable of performing ASTM D5470 testing, the thermal resistance is measured at a pressure of 206.8 kPa (30 psi).

5. The article of any one of claims 1-4, wherein, The phase change material contains gallium.

6. The article of manufacture according to any one of claims 1-5, wherein, The phase change material contains indium.

7. The article of manufacture according to any one of claims 1-6, wherein, The phase change material contains tin.

8. The article of manufacture according to any one of claims 1-7, wherein, The phase change material contains bismuth.

9. The article of manufacture according to any one of claims 1-8, wherein, The solid material comprises foamed metal.

10. The article of manufacture according to any one of claims 1-9, wherein, The foamed metal contains inactive metals.

11. The article of manufacture as claimed in claim 10, wherein, The inactive metal includes titanium.

12. The article of manufacture according to any one of claims 10-11, wherein, The inactive metal includes tungsten.

13. The article of manufacture according to any one of claims 10-12, wherein, The inactive metal includes vanadium.

14. The article of manufacture according to any one of claims 10-13, wherein, The inactive metal includes chromium.

15. The article of manufacture according to any one of claims 10-14, wherein, The inactive metal includes hafnium.

16. The article of manufacture according to any one of claims 10-15, wherein, The inactive metal includes molybdenum.

17. The article of manufacture according to any one of claims 10-16, wherein, The inactive metal includes neodymium.

18. The article of manufacture according to any one of claims 10-17, wherein, The inactive metal includes zirconium.

19. The article of manufacture according to any one of claims 1-18, wherein, The foam metal contains active metals.

20. The article of manufacture as claimed in claim 11, wherein, The active metal includes copper.

21. The article of manufacture as claimed in claim 20, wherein, The active metal includes silver.

22. The article of manufacture according to any one of claims 20-21, wherein, The active metal includes gold.

23. The article of manufacture according to any one of claims 20-22, wherein, The active metal includes nickel.

24. The article of manufacture according to any one of claims 20-23, wherein, The active metal includes zinc.

25. The article of manufacture according to any one of claims 20-24, wherein, The active metal includes platinum.

26. The article of manufacture according to any one of claims 20-25, wherein, The active metal contains iron.

27. The article of manufacture according to any one of claims 1-26, wherein, The solid material is adjacent to a layer that prevents chemical reactions with the solid material.

28. The article of manufacture as claimed in claim 27, wherein, The chemical reaction is a redox reaction.

29. The article of manufacture as claimed in any one of claims 27 or 28, wherein, The chemical reaction is an acid-base chemical reaction.

30. The article of manufacture according to any one of claims 27-29, wherein, The chemical reaction is a hydrolysis chemical reaction.

31. The article of manufacture according to any one of claims 27-30, wherein, The layer that prevents the chemical reaction is an anodized layer.

32. The article of manufacture according to any one of claims 27-31, wherein, The layer that prevents the chemical reaction is a coating.

33. The article of manufacture according to any one of claims 1-32, wherein, The solid material comprises fibers.

34. The article of manufacture according to any one of claims 1-33, wherein, The solid material comprises a porous metallic solid.

35. The article of manufacture as claimed in claim 34, wherein, The porous metal solid is formed by powder metallurgy.

36. The article of manufacture as claimed in any one of claims 34 or 35, wherein, The porous metal solid is formed by particle sintering.

37. The article of manufacture according to any one of claims 1-36, wherein, The solid material contains passivated metal particles.

38. The article of manufacture as claimed in claim 37, wherein, The passivated metal particles include an inactive passivation layer.

39. The article of manufacture according to any one of claims 1-38, wherein, The solid material comprises carbon foam.

40. The article of manufacture according to any one of claims 1-39, wherein, The solid material includes carbon paper.

41. The article of manufacture according to any one of claims 1-40, wherein, The solid material comprises organic foam.

42. The article of manufacture according to any one of claims 1-41, wherein, The solid material comprises polymer foam.

43. The article of manufacture according to any one of claims 1-42, wherein, The solid material includes organic paper.

44. The article of manufacture according to any one of claims 1-43, wherein, The solid material comprises polymer paper.

45. The article of manufacture according to any one of claims 1-44, wherein, The solid material comprises carbon-based particles.

46. ​​The article of manufacture as claimed in claim 45, wherein, The carbon-based particles contain graphite.

47. The article of manufacture as claimed in any one of claims 45 or 46, wherein, The carbon-based particles contain graphene.

48. The article of manufacture according to any one of claims 45-47, wherein, The carbon-based particles contain carbon fibers.

49. The article of manufacture according to any one of claims 45-48, wherein, The carbon-based particles contain carbon nanotubes.

50. The article of manufacture according to any one of claims 45-49, wherein, The carbon-based particles are spherical.

51. The article of manufacture according to any one of claims 45-50, wherein, The carbon-based particles are plate-shaped.

52. The article of manufacture according to any one of claims 45-51, wherein, The carbon-based particles are cylindrical.

53. The article of manufacture according to any one of claims 45-52, wherein, The carbon-based particles have a diameter of at least 0.1 micrometers.

54. The article of manufacture according to any one of claims 45-53, wherein, The carbon-based particles have a diameter of no more than 500 micrometers.

55. The article of manufacture according to any one of claims 1-54, wherein, The solid material comprises ceramic particles.

56. The article of manufacture as claimed in claim 55, wherein, The ceramic particles contain silicon carbide.

57. The article of manufacture as claimed in any one of claims 55 or 56, wherein, The ceramic particles contain silicon nitride.

58. The article of manufacture as claimed in any one of claims 55-57, wherein, The ceramic particles contain boron nitride.

59. The article of manufacture according to any one of claims 55-58, wherein, The ceramic particles contain alumina.

60. The article of manufacture as claimed in any one of claims 55-59, wherein, The ceramic particles contain zinc oxide.

61. The article of manufacture according to any one of claims 55-60, wherein, The ceramic particles contain titanium dioxide.

62. The article of manufacture according to any one of claims 55-61, wherein, The ceramic particles contain silicon dioxide.

63. The article of manufacture as claimed in any one of claims 55-62, wherein, The ceramic particles contain zirconium dioxide.

64. The article of manufacture according to any one of claims 55-63, wherein, The ceramic particles contain iron oxide.

65. The article of manufacture according to any one of claims 55-64, wherein, The ceramic particles contain calcium oxide.

66. The article of manufacture as claimed in any one of claims 55-65, wherein, The ceramic particles contain magnesium oxide.

67. The article of manufacture as claimed in any one of claims 55-66, wherein, The ceramic particles contain barium oxide.

68. The article of manufacture as claimed in any one of claims 55-67, wherein, The ceramic particles are spherical.

69. The article of manufacture as claimed in any one of claims 55-68, wherein, The ceramic particles are plate-shaped.

70. The article of manufacture as claimed in any one of claims 55-69, wherein, The ceramic particles are cylindrical.

71. The article of manufacture according to any one of claims 55-70, wherein, The ceramic-based ceramic particles have a diameter of at least 0.1 micrometers.

72. The article of manufacture according to any one of claims 55-71, wherein, The ceramic particles have a diameter of no more than 500 micrometers.

73. The article of manufacture according to any one of claims 1-72, wherein, The solid structure comprises foam ceramic.

74. The article of manufacture according to any one of claims 1-73, wherein, The self-supporting composite can be processed without a support at a temperature not exceeding 40°C.

75. The article of manufacture according to any one of claims 1-74, wherein, The thickness was measured at a pressure not exceeding 400 psi.

76. The article of manufacture as claimed in claim 75, wherein, The pressure mentioned is the clamping pressure.

77. The article of manufacture according to any one of claims 1-76, wherein, The opening volume is continuous.

78. The article of manufacture according to any one of claims 1-77, wherein, The opening volume is discontinuous.

79. The article of manufacture according to any one of claims 1-78, wherein, The solid material constitutes the composite in a weight ratio between 3% and 90%.

80. The article of manufacture according to any one of claims 1-79, wherein, The phase change material forms the continuous outer surface of the composite.

81. A method for manufacturing an article as claimed in any one of claims 1-80.

82. The method of claim 81, wherein the method comprises forming a composite by mechanically mixing the phase change material and the solid material.

83. The method of any one of claims 81 or 82, wherein the method comprises forming a composite by ultrasonically mixing the solid material and the phase change material.

84. The method of any one of claims 81-83, the method comprising forming a composite by casting the phase change material onto the solid material.

85. The method of claim 84, wherein, The phase change material is cast onto the solid material under pressure during casting.

86. The method of any one of claims 81-85, the method comprising forming a composite by spraying the phase change material onto the solid material.

87. The method of claim 86, wherein, The phase change material is sprayed using cold spraying.

88. The method of any one of claims 81-87, the method comprising forming a composite by casting the phase change material onto the solid material.

89. The method of any one of claims 81-88, the method comprising forming a composite by electrowetting the phase change material onto the solid material.

90. The method of any one of claims 81-89, wherein the method comprises forming a composite by electromagnetically mixing the phase change material and the solid material.

91. The method of any one of claims 81-90, the method comprising cryogenically grinding the phase change material and the solid material, wherein the solid material comprises support particles.

92. The method of any one of claims 81-91, the method further comprising forming a composite by pressing the cryo-milled phase change material and support particles together.

93. The method of any one of claims 81-92, the method comprising forming a composite by immersing the solid material in the phase change material, wherein the phase change material is a liquid phase change material.

94. The method of any one of claims 81-93, the method comprising forming a composite by pressing the phase change material and the solid material together, wherein the phase change material is a solid phase change material.

95. The method according to any one of claims 81-94, wherein, When tested using a fixture capable of performing ASTM D5470 tests, the thermal resistance was measured at a pressure of 206.8 kPa (30 psi).

96. The method according to any one of claims 81-95, wherein, The composition has a particle size of less than 10 mm. 2 Thermal resistance in K / W.

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