Interfacial Thermal Resistance Research Articles

Interweaved filler network in epoxy resin with reduced interface thermal resistance via in-situ high-temperature “welding” for significantly improved thermal conductivity

For heterogeneous integration in harsh environments, polymeric materials are required to integrate excellent insulating property with significant thermal conductivity. Traditional discrete fillers used in polymeric matrix to create thermal pathways introduce numerous contact interfaces, leading to limited thermal conductivity enhancement efficiency (TCE) and unstable dielectric properties. Here, a distinctive strategy, involving the preparation of an interweaved thermally conductive filler with inherent heat channels through self-templated electrospinning and in-situ high-temperature “interface welding”, is proposed to reduce the interface thermal resistance (ITR). The growth of grains at high temperature facilitates the process of “interface welding”, while self-templated electrospinning establishes intrinsic thermal conduction pathways. Consequently, the epoxy resin fortified with this interweaved filler exhibits an exceptionally TCE of 162.15 % and enhanced in-plane thermal conductivity of 3.75 W m−1 K−1 at ultra-low filler ratio of 7.10 vol%. The combination of high electrical insulation of filler and low filler content results in excellent electrical insulating property (>1017 Ω cm) and stable dielectric properties over a frequency range of 103-106 Hz, enabling the successful implementation of heterogeneous integration in challenging environments. This work has the potential to offer a groundbreaking approach for achieving interconnected functional networks within polymer-based composites.

Thermal conductivity of composites with heterogeneous fillers under effects of interface thermal resistance

There has been significant interest in enhancing the effective thermal conductivity (ETC) of polymer by incorporating spherical hybrid fillers. However, the effect of interface thermal resistance (Rc) on the ETC of composites has not been investigated. In this paper, this effect is investigated. Meanwhile, the combined effects of filler thermal conductivities (K1, K2), filler sizes (V1, V2), the Rc sum (R*c1 + R*c2) and the Rc ratio (R*c1/R*c2) are also considered. The results show that for a given K1, K2 and R*c1 + R*c2, the ETC is largely independent of R*c1/R*c2 when the R*c1 + R*c2 is less than 10−4. However, when the R*c1/R*c2 ranges from 10−2 to 10, the competing effects of hybrid fillers Rc have a significant effect on the ETC. The ETC is not affected by the TC of filler-1 when K1 exceeds a critical value of 103, instead becoming dependent on K2. For each sum of Rc, there exists a critical value of R*c1/R*c2 where the ETC reaches its nadir, this critical value is influenced by the R*c1 + R*c2, V and K of two fillers. The Rc of fillers with high K is <10−2, it is not feasible to improve the ETC by continuing to reduce its Rc, this value is 10−4 for fillers with low K.

Nitrogen-doped bean-like SiC-based nanofibers for thermal insulation and electromagnetic wave absorption

SiC nanofibers that can be used to absorb electromagnetic wave (EMW) radiation and as thermal insulators simultaneously are highly desirable. In this work, nitrogen-doped bean-like SiC-based nanofibers were prepared by a simple electrospinning and high-temperature pyrolysis in a nitrogen atmosphere, focusing on studying the effects of nitrogen atom doping on the microstructure, EMW absorption, and thermal insulation properties of the fibers. The results showed that nitrogen doping promoted the formation of the SiOxCyNz phase in the fibers, which improved their interfacial thermal resistance and endowed the fibers with extremely low thermal conductivities (∼0.024 W·m−1·K−1 at 25 ℃, 0.092 W·m−1·K−1 at 1000 ℃). Furthermore, the density of carbon defects in the fibers was improved by nitrogen doping, which created numerous new polarization centers and effectively improved the dielectric loss. With a 4 mm thickness, a minimum reflection loss of −51.8 dB was exhibited at 6.3 GHz, indicating that these fibers are highly promising as an absorption material in harsh environments.

Multiphase Symbiotic Engineered Elastic Ceramic-Carbon Aerogels with Advanced Thermal Protection in Extreme Oxidative Environments.

Elastic aerogels can dissipate aerodynamic forces and thermal stresses by reversible slipping or deforming to avoid sudden failure caused by stress concentration, making them the most promising candidates for thermal protection in aerospace applications. However, existing elastic aerogels face difficulties achieving reliable protection above 1500°C in aerobic environments due to their poor thermomechanical stability and significantly increased thermal conductivity at elevated temperatures. Here, a multiphase sequence and multiscale structural engineering strategy is proposed to synthesize mullite-carbon hybrid nanofibrous aerogels. The heterogeneous symbiotic effect between components simultaneously inhibits ceramic crystalline coarsening and carbon thermal etching, thus ensuring the thermal stability of the nanofiber building blocks. Efficient load transfer and high interfacial thermal resistance at crystalline-amorphous phase boundaries on the microscopic scale, coupled with mesoscale lamellar cellular and locally closed-pore structures, achieve rapid stress dissipation and thermal energy attenuation in aerogels. This robust thermal protection material system is compatible with ultralight density (30mg cm-3), reversible compression strain of 60%, extraordinary thermomechanical stability (up to 1600°C in oxidative environments), and ultralow thermal conductivity (50.58mW m-1 K-1 at 300 °C), offering new options and possibilities to cope with the harsh operating environments faced by space exploration.

Reduced interfacial thermal resistance in acidic alumina-filled adhesives for heat dissipative applications

Reduced interfacial thermal resistance in acidic alumina-filled adhesives for heat dissipative applications

Unveiling the magic of twist angle: Thermal transport in Two-dimensional Graphene/MoS2/Graphene Heterostructures

Thermal transport properties of two-dimensional vdW heterostructures have attracted considerable research interests in electron-related devices due to their powerful capability of multi-functional integration. Herein, we investigated the in-plane and out-of-plane thermal conductivity of graphene/MoS2 heterostructures under various twist angles utilizing molecular dynamics simulations. It was found that the in-plane thermal conductivity of MoS2 layer in heterostructures decreases with twist angle. Notably, the lowest thermal conductivity occurs at a twist angle of 10.893°, just 47.3 % of that in untwisted MoS2 layers in heterostructure. In addition, the interlayer interfacial thermal resistance between graphene and MoS2 layer increases with the twist angle but decreases with the layer numbers of graphene. The atomic position deviation, potential energy surface, phonon state of density are calculated to reveal the regulation mechanism of thermal conductivity by twist angle. Interestingly, it is found that the twist angles and the layer numbers of graphene can control the atomic vibration arising from potential energy surfaces and phonon transport through the overlap of phonon density of states between graphene and MoS2 layers. This study can provide valuable insights into the thermal conductivity modulation and phonon transport mechanism of heterostructures.

Comparison of SiNx Dielectric Layer Grown by Plasma‐Enhanced Chemical Vapor Deposition, Low‐Pressure Chemical Vapor Deposition, and Metal‐Organic Chemical Vapor Deposition in Diamond‐ and GaN‐Based Integrated Devices

To address the issue of heat dissipation caused by the high output power density of gallium nitride (GaN) devices, using diamond‐integrated devices is an effective solution. Recent studies have suggested that incorporating a dielectric layer, such as silicon nitride (SiNx), between diamond and GaN can improve adhesion while also reducing thermal boundary resistance (TBR). In this study, plasma‐enhanced chemical vapor deposition (CVD), low‐pressure CVD, and metal‐organic CVD (MOCVD) techniques are utilized to grow the SiNx layer. The interface behavior of diamond/SiNx/GaN is analyzed through scanning electron microscopy, transmission electron microscopy (TEM), scanning TEM, and energy‐dispersive X‐ray spectroscopy, while time‐domain thermoreflectance measurement is used to characterize thermal properties. After analyzing the impact of the growth dielectric layer on the interface thermal resistance of the three growth modes, it is concluded that the dielectric layer produced by the MOCVD technique exhibits a smoother surface and lower TBR compared to the other two methods. Therefore, the use of the MOCVD technique is recommended to achieve optimal thermal performance in diamond/SiNx/GaN systems.

Equivalent Thermal Conductivity of Topology-Optimized Composite Structure for Three Typical Conductive Heat Transfer Models

Composite materials and structural optimization are important research topics in heat transfer enhancement. The current evaluation parameter for the conductive heat transfer capability of composites is effective thermal conductivity (ETC); however, this parameter has not been studied or analyzed for its applicability to different heat transfer models and composite structures. In addition, the optimized composite structures of a specific object will vary when different optimization methods and criteria are employed. Therefore, it is necessary to investigate a suitable method and parameter for evaluating the heat transfer capability of optimized composites under different heat transfer models. Therefore, this study analyzes and summarizes three typical conductive heat transfer models: surface-to-surface (S-to-S), volume-to-surface (V-to-S), and volume-to-volume (V-to-V) models. The equivalent thermal conductivity (keq) is proposed to evaluate the conductive heat transfer capability of topology-optimized composite structures under the three models. A validated simulation method is used to obtain the key parameters for calculating keq. The influences of the interfacial thermal resistance and size effect on keq are considered. The results show that the composite structure optimized for the V-to-S and V-to-V models has a keq value of only 79.4 W m−1 K−1 under the S-to-S model. However, the keq values are 233.4 W m−1 K−1 and 240.3 W m−1 K−1 under the V-to-S and V-to-V models, respectively, which are approximately 41% greater than those of the in-parallel structure. It can be demonstrated that keq is more suitable than the ETC for evaluating the V-to-S and V-to-V heat transfer capabilities of composite structures. The proposed keq can serve as a characteristic parameter that is beneficial for heat transfer analysis and composite structural optimization.

Experimental Study on Interface Thermal Resistance of Heat Dissipation Channel in Low-Temperature Detector

Abstract To achieve a good heat dissipation effect in the heat dissipation channel of the low-temperature detector, it is necessary to study the thermal conductivity performance of GD414C and indium foil between detector and thermal conductive aluminum block. Based on the experimental principle and referring to the ASTM D-5470 testing method, a set of interface thermal resistance experimental testing equipment is designed. The experiment comparatively studies the relationship between the temperature difference between detector and thermal conductive aluminum block (TCAB) under different power and thermal conductive fillers. The experimental results show that when GD414C is filled between detector and thermal conductive aluminum block, the total thermal resistance is 0.728 ℃/W. When 0.1-mm-thick indium foil is filled, the total thermal resistance is 0.235 ℃/W. When 0.2-mm-thick indium foil is filled, the total thermal resistance is 0.123 ℃/W. Therefore, 0.2-mm-thick indium foil should be selected as the thermal conductive filler.

Strategies for optimizing interfacial thermal resistance of thermally conductive hexagonal boron nitride/polymer composites: A review

AbstractWith the continuous development of high‐end electronic information technologies such as 5G communications, thermal management is an urgent issue in the electronic and circuit industries due to the miniaturization, functionalization and integration. Recently, polymer‐based composites with the fillers of hexagonal boron nitride (h‐BN) have been regarded as promising candidates resulting from their excellent thermal conductivity (TC), good insulation and remarkable comprehensive properties. However, the high surface inertness of h‐BN itself, incompatibility with matrix and other fillers and mismatch of phonon‐spectrum will bring about the matrix/filler and filler/filler interfacial thermal resistance (ITR), which will greatly decline the TC of the composites, and limit their thermal management ability. Therefore, how to design, regulate and improve the interfacial states in composites and eventually enhance the TC is a current challenge. Researchers have made great effort to reduce the ITR of the composites to improve their TC. However, a comprehensive summary and analysis of researches on the improvement methods of the interface states in composites in the past 3 years is still lacking. In this work, the commonly used mechanism models, and simulation methods for calculating and predicting TC was summarized. From perspectives of Synthesis of h‐BNNs, modification, orientation, bridging and three‐dimensional structures construction, we reviewed strategies for improving the interface states in composites, and focused on the ITR regulation and TC improvement. The improvement effects of various methods on TC were compared. The development trend of high TC composite materials was prospected.Highlights Crystallinity, defect, size, flatness, thickness of hexagonal boron nitride nanosheets (BNNSs) affect interfacial thermal resistance (ITR). Nature of interaction between adjacent layers of BNNS need exploited. Interface and defect are root cause of extra phonon scattering. Shape, density, surface area, distribution and compatibility reduce ITR. Theory, model, simulation methods need developed on different levels.

Boosting thermal energy transport across the interface between phase change materials and metals via self-assembled monolayers

Thermal energy storage using phase change materials (PCMs) has great potential to reduce the weather dependency of sustainable energy sources. However, the low thermal conductivity of most PCMs is a long-standing bottleneck for large-scale practical applications. In modifications to increase the thermal conductivity of PCMs, the interfacial thermal resistance (ITR) between PCMs and discrete additives or porous networks reduces the effective thermal energy transport. In this work, we investigated the ITR between a metal (gold) and a polyol solid–liquid PCM (erythritol) at various temperatures including temperatures below the melting point (300 and 350 K), near the melting point (390, 400, 410 K, etc) and above the melting point (450 and 500 K) adopting non-equilibrium molecular dynamics. Since the gold-erythritol interfacial thermal conductance (ITC) is low regardless of whether erythritol is melted or not (<40 MW m−2 K−1), self-assembled monolayers (SAMs) were used to boost the interfacial thermal energy transport. The SAM with carboxyl groups was found to increase the ITC most (by a factor of 7–9). As the temperature increases, the ITC significantly increases (by ∼50 MW m−2 K−1) below the melting point but decreases little above the melting point. Further analysis revealed that the most obvious influencing factor is the interfacial binding energy. This work could build on existing composite PCM solutions to further improve heat transfer efficiency of energy storage applications in both liquid and solid states.

Interfacial thermal resistance between mechanically exfoliated nm-thick MoS2 and silicon from −60 °C to 50 °C based on ns-ET Raman technique

In the miniaturization and integration development of micro-devices, the large thermal contact resistance significantly affects the overall performance of micro-devices, which is influenced by both interfacial contact condition and material properties. However, the temperature dependence of interfacial thermal resistance of realistic materials remains unclear. In this work, the interfacial thermal resistance between nm-thick MoS2 nanosheets and Si substrate is measured by using the ns energy transport state-resolved Raman (ns ET-Raman) technique. By comparing the experimental data with finite difference numerical simulation, the real value of the interfacial thermal resistance is determined. By changing the ambient temperature from -60 °C to 50 °C, the interfacial thermal resistance against temperature curve is obtained. As the environmental temperature deviates from room temperature, a large increasement of the interfacial thermal resistance can be observed. As temperature goes back to room temperature, the unreversible interfacial thermal resistance indicates that the large thermal expansion mismatch deteriorates the contact situation. In the last, the interfacial thermal resistance evolution under varying environmental temperatures from both experiments and modeling results in literatures are compared and discussed to illustrate the effect of different interface formation methods. For epitaxial and CVD grown materials, the interfacial thermal resistance generally reduces with raising ambient temperature. While for mechanically exfoliated samples, the effect of thermal expansion mismatch and the resulting gaps dominate the interfacial thermal resistance, which leads to non-monotonous temperature dependency with a valley located at room temperature.

Insight into the relationship between interfacial structure and thermal conductivity in epoxy resin/Al2O3 composite

AbstractThe relationship between interfacial structure and thermal conductivity in epoxy resin/Al2O3 composite is important but is still elusive. Here, we illuminate this issue by investigating the role of four silane coupling agents in thermal conductivity for epoxy resin/Al2O3 composites. The results show that 3‐glycidoxypropyltrimethoxysilane (KH560) is the best silane coupling agent to modify Al2O3, resulting in the lowest viscosity and the highest thermal conductivity of the epoxy resin/Al2O3‐KH560 composite compared with alternative systems. This is attributed to the strong interfacial interaction between Al2O3‐KH560 and epoxy resin, as confirmed by the Fowkes model and broadband dielectric spectroscopy. The interfacial thermal resistance between the epoxy resin and Al2O3 is also quantitatively measured via a photothermal radiometry technique. The epoxy resin/Al2O3‐KH560 also has the lowest interfacial thermal resistance (1.50 ± 0.02 × 10−6 m2 K W−1), compared with the other three systems. This study advances the understanding of the relationship between interfacial structure and thermal conductivity in polymer composites.Highlights The relationship between interfacial structure and thermal conductivity in epoxy resin/Al2O3 composite is understood. The interfacial structure is characterized by broadband dielectric spectroscopy. The interfacial thermal resistance is quantitatively measured via a photothermal radiometry technique.

Reducing Kapitza resistance of graphene–paraffin interfaces by alkyl functionalisation

Paraffin waxes are a promising material for heat storage. Improvement of the thermal conductivity can be obtained by adding graphene nanofillers, but interfacial thermal resistance (ITR) forms a problem. Reduction of ITR by functionalisation of the graphene was previously shown possible in the liquid state. For application in heat storage, the thermal properties in solid state are equally important. In the present study, the most optimal reduction of ITR in the solid state was shown for octyl functional groups; in both molten and solid samples, a striking reduction by 95% as compared to pristine graphene was achieved.

Design of Soft/Hard Interface with High Adhesion Energy and Low Interfacial Thermal Resistance via Regulation of Interfacial Hydrogen Bonding Interaction.

Adhesion ability and interfacial thermal transfer capacity at soft/hard interfaces are of critical importance to a wide variety of applications, ranging from electronic packaging and soft electronics to batteries. However, these two properties are difficult to obtain simultaneously due to their conflicting nature at soft/hard interfaces. Herein, we report a polyurethane/silicon interface with both high adhesion energy (13535 J m-2) and low thermal interfacial resistance (0.89 × 10-6 m2 K W-1) by regulating hydrogen interactions at the interface. This is achieved by introducing a soybean-oil-based epoxy cross-linker, which can destroy the hydrogen bonds in polyurethane networks and meanwhile can promote the formation of hydrogen bonds at the polyurethane/silicon interface. This study provides a comprehensive understanding of enhancing adhesion energy and reducing interfacial thermal resistance at soft/hard interfaces, which offers a promising perspective to tailor interfacial properties in various material systems.

Preparations and Thermal Properties of PDMS-AlN-Al2O3 Composites through the Incorporation of Poly(Catechol-Amine)-Modified Boron Nitride Nanotubes

As one of the emerging nanomaterials, boron nitride nanotubes (BNNTs) provide promising opportunities for diverse applications due to their unique properties, such as high thermal conductivity, immense inertness, and high-temperature durability, while the instability of BNNTs due to their high surface induces agglomerates susceptible to the loss of their advantages. Therefore, the proper functionalization of BNNTs is crucial to highlight their fundamental characteristics. Herein, a simplistic low-cost approach of BNNT surface modification through catechol-polyamine (CAPA) interfacial polymerization is postulated to improve its dispersibility on the polymeric matrix. The modified BNNT was assimilated as a filler additive with AlN/Al2O3 filling materials in a PDMS polymeric matrix to prepare a thermal interface material (TIM). The resulting composite exhibits a heightened isotropic thermal conductivity of 8.10 W/mK, which is a ~47.27% increase compared to pristine composite 5.50 W/mK, and this can be ascribed to the improved BNNT dispersion forming interconnected phonon pathways and the thermal interface resistance reduction due to its augmented compatibility with the polymeric matrix. Moreover, the fabricated composite manifests a fire resistance improvement of ~10% in LOI relative to the neat composite sample, which can be correlated to the thermal stability shift in the TGA and DTA data. An enhancement in thermal permanence is stipulated due to a melting point (Tm) shift of ∼38.5 °C upon the integration of BNNT-CAPA. This improvement can be associated with the good distribution and adhesion of BNNT-CAPA in the polymeric matrix, integrated with its inherent thermal stability, good charring capability, and free radical scavenging effect due to the presence of CAPA on its surface. This study offers new insights into BNNT utilization and its corresponding incorporation into the polymeric matrix, which provides a prospective direction in the preparation of multifunctional materials for electric devices.

Enhancing thermal conductance between graphene and epoxy interfaces through non-covalent cation-π interactions

Although graphene has high thermal conductivity, its application in thermal management remains challenging because of the large interfacial thermal resistance between graphene and adjacent materials. This work demonstrates that non-covalent cationic-π interaction can significantly improve the thermal conductance between graphene and substrate interfaces. Cationic polyacrylamide (CPAM) bridges substrate and graphene with hydrogen bonding and cation-π interaction, respectively. The cation-π interaction between graphene and CPAM is confirmed by Raman, UV–Vis and NMR spectroscopy. The results show that CPAM increases the interfacial adhesion of graphene/epoxy from 18.7 ± 2.2 mN to 37.4 ± 7.6 mN (100.0 % improvement) and improves the interfacial thermal conductivity (ITC) from 22 ± 2 MW/m2K to 51 ± 5 MW/m2K (131.8 % improvement). Enhancing the ITC of graphene/epoxy by introducing CPAM assembled layer has advantages over covalent modifications because it provides a similar level of ITC improvement rate, but has little effect on the intrinsic thermal conductivity of graphene. Finally, it is demonstrated that the sample with graphene/cationic polyelectrolyte/substrate structure exhibits great potential for applications in the area of thermal management and printed circuit boards.

High throughput screening of thermal interface materials by machine learning

Till now, it remains a challenge for effective prediction and screening of novel materials with high thermal conductivity, as well as further optimization of the interface thermal resistance. Normally, people have to spend long time on tedious calculations when predicting and screening these materials. In this paper, I combined machine learning with molecular dynamics simulations to investigate the thermal conductive properties of materials with the aim of significantly reducing computational consumption. I first applied molecular dynamics simulations to obtain the relevant properties of materials, then generated models for predicting physical properties by machine learning, and finally made predictions of thermophysical properties of materials. The use of machine learning significantly reduces the prediction time compared to direct molecular dynamics simulations. Especially when the XGBoost and the neural network models are employed, the prediction efficiency is significantly improved. This work guides a new way for the future screening of high-performance thermal interface materials.

Carbon nanotubes grafting aminated epoxy resin with improved elasticity and surface adhesion for enhanced thermal management performance

It is a great challenge to develop thermal interface materials that enable fast heat transfer between the surface of microelectronic materials and heat sinks. In this paper, multi-walled carbon nanotube/epoxy composites (EP-NH2-x) were synthesized by amidation reaction using aminated epoxy resin as matrix and carboxylated multi-walled carbon nanotubes. EP-NH2-x can reduce the interfacial thermal resistance and the promotion of phonon conduction through the chemical bonding connection between the resin and the carbon nanotubes, which will in turn improve the thermal conductivity of the composites. The thermal conductivity of EP-NH2-10 reaches 0.531 W·m−1·K−1 at a and has good variable temperature cycling stability, internal elasticity and surface adhesion. This work highlights the potential application of carbon materials to improve the thermal conductivity of epoxy resins.

A study on novel dual-functional photothermal material for high-efficient solar energy harvesting and storage

The solar-heat storage efficiency of devices based on phase change materials (PCMs) is limited due to the light absorption and internal heat transfer within the PCMs, unclear thermal conductivity-enhancement mechanism within nanocomposite PCMs, and uncontrollable photothermal-interface modulation. Therefore, a novel controllable strategy was proposed in this study to fabricate dual-functional photothermal storage three-dimensional (3D) phase change blocks (PCBs) with higher thermal conductivity (27.98 W/m·K) and spectral absorption (98.03 %) compared to those of most previously reported PCM-based devices. The as-synthesized PCBs contained millimeter-sized graphite plates with horizontal Van der Waals bonds and oriented micro/nanoscale graphite nanosheets. The structural properties of thin PCM layers between the PCB sheets have synergistically reduced the internal interfacial thermal resistance of the PCBs. Laser-controllable induction was used to fabricate integrated biomimetic-forest 3D optical absorbers on the high thermal conductivity interface of the PCBs, which significantly reduced the thermal resistance of the optical-thermal interface. The resulting 3D-PCBs, integrated with thermoelectric generators, powered portable electronic devices, expanding the applications of traditional PCM heat-storage devices. Therefore, this study will guide the future design of high-performance solar-thermal storage PCMs with a wide range of practical applications.