Linking Interfacial Bonding and Thermal Conductivity in Molecularly-Confined Polymer-Glass Nanocomposites with Ultra-High Interfacial Density

Thermal transport in polymer nanocomposites becomes dependent on the interfacial thermal conductance due to the ultra-high density of the internal interfaces when the polymer and filler domains are intimately mixed at the nanoscale. However, there is a lack of experimental measurements that can link the thermal conductance across the interfaces to the chemistry and bonding between the polymer molecules and the glass surface. Characterizing the thermal properties of amorphous composites are a particular challenge as their low intrinsic thermal conductivity leads to poor measurement sensitivity of the interfacial thermal conductance. To address this issue here, polymers are confined in porous organosilicates with high interfacial densities, stable composite structure, and varying surface chemistries. The thermal conductivities and fracture energies of the composites are measured with frequency dependent time-domain thermoreflectance (TDTR) and thin-film fracture testing, respectively. Effective medium theory (EMT) along with finite element analysis (FEA) is then used to uniquely extract the thermal boundary conductance (TBC) from the measured thermal conductivity of the composites. Changes in TBC are then linked to the hydrogen bonding between the polymer and organosilicate as quantified by Fourier-transform infrared (FTIR) and X-ray photoelectron (XPS) spectroscopy. This platform for analysis is a new paradigm in the experimental investigation of heat flow across constituent domains.     

Manipulating thermal conductance at metal-graphene contacts via chemical functionalization

Graphene-based devices have garnered tremendous attention due to the unique physical properties arising from this purely two-dimensional carbon sheet leading to tremendous efficiency in the transport of thermal carriers (i.e., phonons). However, it is necessary for this two-dimensional material to be able to efficiently transport heat into the surrounding 3D device architecture in order to fully capitalize on its intrinsic transport capabilities. Therefore, the thermal boundary conductance at graphene interfaces is a critical parameter in the realization of graphene electronics and thermal solutions. In this work, we examine the role of chemical functionalization on the thermal boundary conductance across metal/graphene interfaces. Specifically, we metalize graphene that has been plasma functionalized and then measure the thermal boundary conductance at Al/graphene/SiO(2) contacts with time domain thermoreflectance. The addition of adsorbates to the graphene surfaces are shown to influence the cross plane thermal conductance; this behavior is attributed to changes in the bonding between the metal and the graphene, as both the phonon flux and the vibrational mismatch between the materials are each subject to the interfacial bond strength. These results demonstrate plasma-based functionalization of graphene surfaces is a viable approach to manipulate the thermal boundary conductance.     

Ultra-High Interfacial Thermal Conductance via Double hBN Encapsulation for Efficient Thermal Management of 2D Electronics

Heat dissipation is a major limitation of high-performance electronics. This is especially important in emerging nanoelectronic devices consisting of ultra-thin layers, heterostructures, and interfaces, where enhancement in thermal transport is highly desired. Here, ultra-high interfacial thermal conductance in encapsulated van der Waals (vdW) heterostructures with single-layer transition metal dichalcogenides MX₂ (MoS₂, WSe₂, WS₂) sandwiched between two hexagonal boron nitride (hBN) layers is reported. Through Raman spectroscopic measurements of suspended and substrate-supported hBN/MX₂/hBN heterostructures with varying laser power and temperature, the out-of-plane interfacial thermal conductance in the vertical stack is calibrated. The measured interfacial thermal conductance between MX₂ and hBN reaches 74 ± 25 MW m⁻² K⁻¹, which is at least ten times higher than the interfacial thermal conductance of MX₂ in non-encapsulation structures. Molecular dynamics (MD) calculations verify and explain the experimental results, suggesting a full encapsulation by hBN layers is accounting for the high interfacial conductance. This ultra-high interfacial thermal conductance is attributed to the double heat transfer pathways and the clean and tight vdW interface between two crystalline 2D materials. The findings in this study reveal new thermal transport mechanisms in hBN/MX₂/hBN structures and shed light on building novel hBN-encapsulated nanoelectronic devices with enhanced thermal management.     

Photothermal Evidence of Laterally Inhomogeneous Interfacial Thermal Resistance in Copper-Coated Carbon Samples

In this study, the heat transport in copper?Ccarbon flat model systems was studied by frequency-dependent photothermal radiometry (PTR). The samples consist of Cu films of about 1???m thickness deposited by magnetron sputtering on vitreous carbon (Sigradur). Particular interest was devoted to the influence of interface defects on the interfacial thermal conductance (or resistance) of the CuC systems. The PTR data were analyzed in the frame of a heat diffusion equation for one- and three-dimensional heat transport. By comparing PTR signals from as-prepared and from heat-treated samples, the lateral inhomogeneities of the interfacial thermal conductance could be quantified. The measured phase differences were analyzed in the scope of a model where a small part of the surface area has a different interfacial thermal conductance than the major part of the surface.     

Phonon Contribution to Thermal Boundary Conductance at Metal Interfaces Using Embedded Atom Method Simulations

The phonon contribution to the thermal boundary conductance (TBC) at metal–metal interfaces is difficult to study experimentally, and it is typically considered negligible. In this study, molecular dynamics simulations (MDS), employing an embedded atom method (EAM) potential, are performed to study the phonon contribution to thermal transport across an Al–Cu interface. The embedded atom method provides a realistic model of atomic behavior in metals, while suppressing the effect on conduction electrons. In this way, measurements on the phonon system may be observed that would otherwise be dominated by the electron contribution in experimental methods. The relative phonon contribution to the TBC is calculated by comparing EAM results to previous experimental results which include both electron and phonon contributions. It is seen from the data that the relative phonon contribution increases with decreasing temperature, possibly accounting for more than half the overall TBC at temperatures below 100 K. These results suggest that neglect of interfacial phonon transport may not be a valid assumption at low temperatures, and may have implications in the future development of TBC models for metal interfaces.     

Model calculations on heat flow in inhomogeneous thermal systems. 1 — Thermal conductivity and boundary resistance at low temperatures

A network modelling technique is applied to the analysis of inhomogeneous thermal systems at low temperatures. A calculation is presented of the temperature distribution and the heat flow in an experimental cell used for the measurement of thermal conductivity and thermal boundary conductance. In a sequel to this paper (part 2) a random number method will be used to analyse the behaviour of sinters in cryogenic heat exchangers.     

On the thermal conductivity of Cu–Zr/diamond composites

Interfaces and close proximity between the diamond and the metal matrix are very important for their thermal conductance performance. Matrix-alloying is a useful approach to greatly enhance the interfacial bonding and thermal conductivity. In this study, the copper–diamond (Cu/Dia) composites with addition of 0.8, 1.2 and 2.4 wt.% zirconium (Zr) are prepared to investigate the influence of minor addition of Zr on the microstructure and thermal conductivity of the composites. The thermal conductivity of the composites is analyzed both experimentally and theoretically. It is demonstrated that moderate interfacial modification due to the Zr added is beneficial to improve the thermal conductivity of the Cu/Dia composites.     

MoS<Subscript>2</Subscript>-graphene in-plane contact for high interfacial thermal conduction

Recent studies have indicated that two-dimensional (2D) MoS₂ exhibits low in-plane and inter-plane thermal conductivities. This poses a significant challenge to heat management in MoS₂-based electronic devices. To address this challenge, we have designed MoS₂-graphene interfaces that fully utilize graphene, a 2D material that exhibits very high thermal conductivity. First, we performed ab initio atomistic simulations to understand bonding and structural stability at the interfaces. The interfaces that we designed, which were connected via strong covalent bonds between Mo and C atoms, were energetically stable. We then performed molecular dynamics simulations to investigate interfacial thermal conductance in these materials. Surprisingly, the interfacial thermal conductance was high and comparable to those of covalently bonded graphene-metal interfaces. Importantly, each interfacial Mo–C bond served as an independent thermal channel, enabling modulation of the interfacial thermal conductance by controlling the Mo vacancy concentration at the interface. The present work provides a viable heat management strategy for MoS₂-based electronic devices.

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Thermal conduction across the one-dimensional interface between a MoS<Subscript>2</Subscript> monolayer and metal electrode

The thermal conductance across the one-dimensional (1D) interface between a MoS2 monolayer and Au electrode (edge-contact) has been investigated using molecular dynamics simulations.Although the thermal conductivity of monolayer MoS2 is 2-3 orders of magnitude lower than that of graphene,the covalent bonds formed at the interface enable interfacial thermal conductance (ITC) that is comparable to that of a graphene-metal interface.Each covalent bond at the interface serves as an independent channel for thermal conduction,allowing ITC to be tuned linearly by changing the interfacial bond density (controlling S vacandes).In addition,different Au surfaces form different bonding configurations,causing large ITC variations.Interestingly,the S vacancies in the central region of MoS2 only slightly affect the ITC,which can be explained by a mismatch of the phonon vibration spectra.Further,at room temperature,ITC is primarily dominated by phonon transport,and electron-phonon coupling plays a negligible role.These results not only shed light on the phonon transport mechanisms across 1D metal-MoS2 interfaces,but also provide guidelines for the design and optimization of such interfaces for thermal management in MoS2-based electronicdevices.     

Thermal resistance of nanoscopic liquid-liquid interfaces: dependence on chemistry and molecular architecture

Systems with nanoscopic features contain a high density of interfaces. Thermal transport in such systems can be governed by the resistance to heat transfer, the Kapitza resistance (RK), at the interface. Although soft interfaces, such as those between immiscible liquids or between a biomolecule and solvent, are ubiquitous, few studies of thermal transport at such interfaces have been reported. Here we characterize the interfacial conductance, 1/RK, of soft interfaces as a function of molecular architecture, chemistry, and the strength of cross-interfacial intermolecular interactions through detailed molecular dynamics simulations. The conductance of various interfaces studied here, for example, water-organic liquid, water-surfactant, surfactant-organic liquid, is relatively high (in the range of 65-370 MW/m2 K) compared to that for solid-liquid interfaces ( approximately 10 MW/m2 K). Interestingly, the dependence of interfacial conductance on the chemistry and molecular architecture cannot be explained solely in terms of either bulk property mismatch or the strength of intermolecular attraction between the two phases. The observed trends can be attributed to a combination of strong cross-interface intermolecular interactions and good thermal coupling via soft vibration modes present at liquid-liquid interfaces.     

Interfacial heat flow in carbon nanotube suspensions

The enormous amount of basic research into carbon nanotubes has sparked interest in the potential applications of these novel materials. One promising use of carbon nanotubes is as fillers in a composite material to improve mechanical behaviour, electrical transport and thermal transport. For composite materials with high thermal conductivity, the thermal conductance across the nanotube-matrix interface is of particular interest. Here we use picosecond transient absorption to measure the interface thermal conductance (G) of carbon nanotubes suspended in surfactant micelles in water. Classical molecular dynamics simulations of heat transfer from a carbon nanotube to a model hydrocarbon liquid are in agreement with experiment. Our findings indicate that heat transport in a nanotube composite material will be limited by the exceptionally small interface thermal conductance (G approximately 12 MW m(-2) K(-1)) and that the thermal conductivity of the composite will be much lower than the value estimated from the intrinsic thermal conductivity of the nanotubes and their volume fraction.     

An experimental study of heat transfer characteristics of a two-phase nitrogen thermosyphon over a large dynamic range operation

Heat transport characteristics of a cryogenic two-phase nitrogen thermosyphon have been experimentally investigated in this study. The thermal resistance and the maximum heat transfer rate were mainly investigated over a wide dynamic range from near the triple point to the critical point. The experimental data suggests that the nominal thermal resistance does not have pressure dependence in the high pressure and high temperature region. The present experimental result is well explained by the theoretical prediction. From the experimental result of the operating limit of the thermosyphon, it is found that the maximum heat transfer rate is governed by the interaction between the vapor flow and the returning liquid film flow along the wall in the evaporator section, even near the critical point.     

Modeling the thermal conductivity of diamond reinforced aluminium matrix composites with inhomogeneous interfacial conductance

A reasonable model for describing the thermal conductivity of diamond reinforced aluminium matrix composites behaving a distinctive character of inhomogeneous distribution of interfacial thermal conductance on diamond surfaces is proposed in terms of an equivalent diameter approach combined with a double effective-medium approximation scheme. Theoretical analyses for the thermal conductivity of diamond reinforced Al (Si) composites prepared by different infiltration techniques (squeeze casting (SQ), gas pressure infiltration (GPI)) are given for rediscovering the existing experimental results considering inhomogeneous conductance behavior. Numerical results using present model agree reasonably well with the experimental observations and explore new findings, i.e. the diffusion bonding also occurs at Al–diamond {1 1 1} interfaces of GPIed composites; the interconnected particles is possibly existed in GPIed Al/diamond composites.     

Thermal Stress Analysis in Particulate Composite Components

Abstract: Thermal stresses resulting from flow of hot and cold water were obtained in sinks manufactured with acrylic casting dispersions by both experimental and numerical analysis. The experimental work was performed in two poly(methyl methacrylate) (PMMA) -silica based particulate composites, compositions of which are different by the volume fraction of filler and the particle size. The thermal stresses in sinks were obtained using strain gauges. The alternate flow of cold and hot water using a mixed tap, results in the formation of thermal gradients, leading to the occurrence of thermal stresses . The experimental results were compared with the numerical results obtained with a commercial finite element software. For this analysis, some thermal parameters such as the convective heat transfer coefficient, the density, the thermal conductivity and the specific heat were experimentally obtained. In general, a good agreement between experimental and numerical results was observed. The results of this study, together with the results of fatigue and fracture tests, will be used in a tolerance analysis of defects in the products manufactured with these composites.     

电热作用对碳纤维树脂基复合材料力学性能的影响

采用复合材料电热实验平台,测试碳纤维树脂基复合材料（Carbon Fiber Reinforced Polymer,CFRP）电热作用下温度场变化规律,同时从单丝拉伸断裂界面剪切强度、短梁剪切性能变化和剪切断口等多方面揭示电热作用对CFRP力学性能的影响机制。结果表明:电热作用会使CFRP整体温度迅速升高,在约4 min时达到稳态温度,随着电流强度的增大,CFRP层板表面温度越高,当电流强度为8 A（0.44 A/mm2）时,CFRP的表面温度达到151℃;单丝拉伸和短梁剪切界面强度都随着电流强度增加呈现先增加后降低的趋势;小电流时,电热作用产生较少的焦耳热,优化界面性能,提高界面剪切强度,大电流时,电热作用产生的焦耳热过大,对界面产生烧蚀等不可逆损伤,降低了界面结合性能。      

Effect of gravity on pool boiling heat transfer on thermal spray coating

This study deals with heat transfer enhancement surface manufactured by thermal spraying. Two thermal spraying methods using copper as a coating material, wire flame spraying (WFS) and vacuum plasma spraying (VPS), were applied to the outside of copper cylinder with 20 mm OD. The surface structure by WFS was denser than that by VPS. The effect of gravity on boiling heat transfer coeffcient and wall superheat at the onset of boiling were experimentally evaluated under micro- and hyper-gravity condition during a parabolic trajectory flight of an airplane. Pool boiling experiments in saturated liquid of HCFC123 were carried out for heat fluxes between 1.0 and 160 kW/m² and saturated temperature of 30 °C. As a result, the surface by VPS produced higher heat transfer coefficient and lower superheat at the onset of boiling under microgravity. For the smooth surface, the effect of gravity on boiling heat transfer coefficient was a little. For the coating, a large difference in heat transfer coefficient to gravity was observed in the moderate heat flux range. The heat transfer coefficinet decreased as gravity changed from the normal to hypergravity, and was improved as gravity changed from the hyperto microgravity. The difference in heat transfer coefficient between the normal and microgravity was a little. Heat transfer enhancement factor was kept over the experimental range of heat flux. It can be said that boiling behavior on thermal spray coating might be influenced by flow convection velocity.     

The importance of water migration in the measurement of the thermal conductivity of unsaturated frozen soils

The transport of heat in frozen soil may occur by conduction and by the convective transport of sensible and latent heat arising from the flow of water in the vapor, liquid and solid states. Theory describing the coupled flow of heat and of water in the liquid and vapor states is used to derive a definition of apparent thermal conductivity (the convective transport of heat in the movement of ice in unstaturated soils is assumed to be negligible). Calculations suggest that, at temperatures close to 0°C, the transport of latent heat may exceed the contribution of heat flow by conduction. Under these conditions, the apparent thermal conductivity will be much greater than the thermal conductivity calculated from the thermal conductivities and volume fractions of the components.Insufficient published data prevent a rigorous evaluation of the theory. However the functional dependence on temperature of both thermal conductivity and the apparent thermal conductivity are calculated for a Tomakomai soil at different subzero temperatures. These values are compared to the apparent thermal conductivities of this soil which were measured at a water content in the unfrozen state of 0.48 cm³ cm^?3 and at temperatures ranging from ?0.7°C to ?10°C using the line heat source technique. The dependence of apparent thermal conductivity on subzero temperature, as calculated from theory, compares favourably to the dependence which was observed for this soil.     

Fabrication and thermal conductivity of copper matrix composites reinforced with Mo2C or TiC coated graphite fibers

Graphite fiber reinforced Cu-based composites have good thermal conductivity, low coefficient of thermal expansion for heat sink applications. In these composites, the quality of interfacial bonding between the copper matrix and the graphite fibers has significant influence on the thermal properties of composites. In this study, two different carbide coatings (Mo₂C or TiC) were synthesized on graphite fiber to promote the interfacial bonding in composites. Fibers/Cu composites had been produced by spark plasma sintering process. The results showed that the densification, interfacial bonding and thermal conductivity of coated composites were improved distinctly compared to that of uncoated ones. The enhanced composites present 16–44% increase of thermal conductivity in X–Y plane. An original theoretical model was proposed to estimate the interface thermal resistance. The result showed that the interfacial thermal resistance was largely reduced by one order of magnitude with the introduction of carbide interlayer.     

Effect of amphiphilic coupling agent on heat flow and dielectric properties of flax–polypropylene composites

The study on heat transport in composites is of fundamental importance in engineering design and for tailoring thermal and mechanical behaviour of materials. In this study, the thermal conductivity and thermal diffusivity of flax reinforced polypropylene (PP) composites were determined at room temperature. Chemical modification in the form of a biodegradable zein coating was applied to the flax nonwovens. The effect of fibre loading and chemical modification on the thermo-physical properties was investigated. Dielectric permittivity studies were also evaluated and the dielectric constant of fibre reinforced composites was found to be higher than that of PP. The heat flow and crystallinity effects of the composites were also determined by differential scanning calorimetric (DSC) studies. Zein modification of the flax fibres resulted in a decrease of thermal conductivity and diffusivity which was attributed to a decrease in velocity and mean free path of phonons due to increase in interfacial adhesion.     

Strain Modulation of Electronic and Heat Transport Properties of Bilayer Boronitrene

Strain engineering has been proven as an effective approach to modify electronic and thermal properties of materials. Recently, strain effects on two-dimensional materials have become important relevant topics in this field. We performed density functional theory studies on the electronic and heat transport properties of bilayer boronitrene samples under an isotropic strain. We demonstrate that the strain will reduce the band gap width but keep the band gap type robust and direct. The strain will enhance the thermal conductivity of the system because of the increase in specific heat. The thermal conductivity was studied as a function of the phonon mean-free path.