Along with the technology evolution for dense integration of high-power, high-frequency devices in electronics, the accompanying interfacial heat transfer problem leads to urgent demands for advanced ...thermal interface materials (TIMs) with both high through-plane thermal conductivity and good compressibility. Most metals have satisfactory thermal conductivity but relatively high compressive modulus, and soft silicones are typically thermal insulators (0.3 W m–1 K–1). Currently, it is a great challenge to develop a soft material with the thermal conductivity up to metal level for TIM application. This study solves this problem by constructing a graphene-based microstructure composed of mainly vertical graphene and a thin cap of horizontal graphene layers on both the top and bottom sides through a mechanical machining process to manipulate the stacked architecture of conventional graphene paper. The resultant graphene monolith has an ultrahigh through-plane thermal conductivity of 143 W m–1 K–1, exceeding that of many metals, and a low compressive modulus of 0.87 MPa, comparable to that of silicones. In the actual TIM performance measurement, the system cooling efficiency with our graphene monolith as TIM is 3 times as high as that of the state-of-the-art commercial TIM, demonstrating the superior ability to solve the interfacial heat transfer issues in electronic systems.
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With the increasing integration of devices in electronics fabrication, there are growing demands for thermal interface materials (TIMs) with high through-plane thermal conductivity for efficiently ...solving thermal management issues. Graphene-based papers consisting of a layer-by-layer stacked architecture have been commercially used as lateral heat spreaders; however, they lack in-depth studies on their TIM applications due to the low through-plane thermal conductivity (<6 W m–1 K–1). In this study, a graphene hybrid paper (GHP) was fabricated by the intercalation of silicon source and the in situ growth of SiC nanorods between graphene sheets based on the carbothermal reduction reaction. Due to the formation of covalent C–Si bonding at the graphene–SiC interface, the GHP possesses a superior through-plane thermal conductivity of 10.9 W m–1 K–1 and can be up to 17.6 W m–1 K–1 under packaging conditions at 75 psi. Compared with the current graphene-based papers, our GHP has the highest through-plane thermal conductivity value. In the TIM performance test, the cooling efficiency of the GHP achieves significant improvement compared to that of state-of-the-art thermal pads. Our GHP with characteristic structure is of great promise as an inorganic TIM for the highly efficient removal of heat from electronic devices.
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Urged by the increasing power and packing densities of integrated circuits and electronic devices, efficient dissipation of excess heat from hot spot to heat sink through thermal interface materials ...(TIMs) is a growing demand to maintain system reliability and performance. In recent years, graphene‐based TIMs received considerable interest due to the ultrahigh intrinsic thermal conductivity of graphene. However, the cooling efficiency of such TIMs is still limited by some technical difficulties, such as production‐induced defects of graphene, poor alignment of graphene in the matrix, and strong phonon scattering at graphene/graphene or graphene/matrix interfaces. In this study, a 120 µm‐thick freestanding film composed of vertically aligned, covalently bonded graphene nanowalls (GNWs) is grown by mesoplasma chemical vapor deposition. After filling GNWs with silicone, the fabricated adhesive TIMs exhibit a high through‐plane thermal conductivity of 20.4 W m−1 K−1 at a low graphene loading of 5.6 wt%. In the TIM performance test, the cooling efficiency of GNW‐based TIMs is ≈1.5 times higher than that of state‐of‐the‐art commercial TIMs. The TIMs achieve the desired balance between high through‐plane thermal conductivity and small bond line thickness, providing superior cooling performance for suppressing the degradation of luminous properties of high‐power light‐emitting diode chips.
Graphene nanowalls, composed of high‐quality, vertically aligned, and covalently bonded graphene frameworks, exhibit excellent ability to improve the thermal conductivity of polymer‐based thermal interface materials. The resulting composites show a through‐plane thermal conductivity of 20.4 W m−1 K−1 at a filler content of 5.6 wt%, resulting in ≈1.5 times higher cooling efficiency compared to that of a commercial thermal pad.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
As the power density and integration level of electronic devices increase, there are growing demands to improve the thermal conductivity of polymers for addressing the thermal management issues. On ...the basis of the ultrahigh intrinsic thermal conductivity, graphene has exhibited great potential as reinforcing fillers to develop polymer composites, but the resultant thermal conductivity of reported graphene-based composites is still limited. Here, an interconnected and highly ordered graphene framework (HOGF) composed of high-quality and horizontally aligned graphene sheets was developed by a porous film-templated assembly strategy, followed by a stress-induced orientation process and graphitization post-treatment. After embedding into the epoxy (EP), the HOGF/EP composite (24.7 vol %) exhibits a record-high in-plane thermal conductivity of 117 W m–1 K–1, equivalent to ≈616 times higher than that of neat epoxy. This thermal conductivity enhancement is mainly because the HOGF as a filler concurrently has high intrinsic thermal conductivity, relatively high density, and a highly ordered structure, constructing superefficient phonon transport paths in the epoxy matrix. Additionally, the use of our HOGF/EP as a heat dissipation plate was demonstrated, and it achieved 75% enhancement in practical thermal management performance compared to that of conventional alumina for cooling the high-power LED.
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Vacuum filtration is a highly effective and easy scale-up approach and has been widely used to fabricate graphene monoliths, such as graphene paper and graphene frameworks for various applications. ...In general, the microstructure of filtrated monoliths exhibits layer-by-layer stacking of graphene sheets due to the directional flow-induced assembly process. In this work, we found that the horizontally oriented structure of filtrated graphene frameworks can be modulated to an approximately isotropic arrangement by lowering the lateral size of graphene sheets. This size-dependent microstructure transition from anisotropic to isotropic was further confirmed by measuring the in- and through-plane thermal conductivity of the graphene/epoxy composites with different arrangements of graphene frameworks as a filler. Optimally, we obtained an epoxy composite embedded with a quasi-isotropic graphene framework (QIGF) by a simple two-step process: vacuum filtration of small graphene sheets to obtain the framework followed by the infiltration of epoxy resin. Based on the interconnected graphene sheets with an approximately isotropic arrangement, QIGF provides heat channels of graphene–graphene along both the in- and through-plane directions within epoxy. With a low graphene loading of 5.5 wt%, QIGF/epoxy (QIGF/EP) presents in- and through-plane thermal conductivities of 10.0 and 5.4 W mK −1 , respectively, which are equivalent to ∼55 and 29 times higher than those of neat epoxy. As compared to the current graphene/epoxy composites prepared by various methods, our QIGF/EP has the highest thermal conductivity value with this level of filler loading. Our findings provide an insight for the development of polymer composites for thermal management applications in industry.
Graphene is usually embedded into polymer matrices for the development of thermally conductive composites, preferably forming an interconnected and anisotropic framework. Currently, the directional ...self‐assembly of exfoliated graphene sheets is demonstrated to be the most effective way to synthesize anisotropic graphene frameworks. However, achieving a thermal conductivity enhancement (TCE) over 1500% with per 1 vol% graphene content in polymer matrices remains challenging, due to the high junction thermal resistance between the adjacent graphene sheets within the self‐assembled graphene framework. Here, a multiscale structural modulation strategy for obtaining highly ordered structure of graphene framework and simultaneously reducing the junction thermal resistance is demonstrated. The resultant anisotropic framework contributes to the polymer composites with a record‐high thermal conductivity of 56.8–62.4 W m−1 K−1 at the graphene loading of ≈13.3 vol%, giving an ultrahigh TCE per 1 vol% graphene over 2400%. Furthermore, thermal energy management applications of the composites as phase change materials for solar‐thermal energy conversion and as thermal interface materials for electronic device cooling are demonstrated. The finding provides valuable guidance for designing high‐performance thermally conductive composites and raises their possibility for practical use in thermal energy storage and thermal management of electronics.
The dual‐assembled graphene framework (DAGF), which combines a highly oriented graphene structure along the vertical direction and a low junction thermal resistance between the graphene building blocks, exhibits excellent performance in improving the thermal conductivity of polymers. The resultant composites have a record‐high thermal conductivity of 56.8–62.4 W m−1 K−1(≈13.3 vol%), significantly outperforming previously reported results.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The vertical spacing among reinforcements in geosynthetic-reinforced earth embankment is crucial to its overall stability. Based on the upper bound theorem of plastic limit analysis and pseudo-static ...approach, an overall stability analysis method for bilaterally wrapped reinforced embankments under strip surcharge and seismic action is put forward in view of the planar and log-spiral failure mechanism of the reinforced embankments, which quantitatively expresses the relationship between the reinforcement spacing and the factor of safety of the embankments. Some examples show that the maximum relative error of the factor of safety between the proposed method and some existing methods is around 10% under a specified reinforcement spacing. The factor of safety is nonlinearly decreasing as the reinforcement spacing increases, and the results by the log-spiral mode are slightly more conservative than those by the planar mode. The proposed method can quantitatively reflect the influence of the filling properties, reinforcement strength, seismic forces, strip surcharge, and embankment geometry on the reinforcement spacing. The nonlinear negative relationship between the factor of safety and the reinforcement spacing is noticeable under different reinforcement strengths. The reinforcement spacing is almost linearly reducing with the increase of the vertical seismic coefficient increases, while it decreases clearly nonlinearly as the horizontal seismic coefficient increases.
With the continuous progress in electronic devices, thermal interface materials (TIMs) are urgently needed for the fabrication of integrated circuits with high reliability and performance. Graphene ...as a wonderful additive is often added into polymer to build composite TIMs. However, owing to the lack of a specific design of the graphene skeleton, thermal conductivity of graphene‐based composite TIMs is not significantly improved. Here a chloroform‐assisted method for rapid growth of vertical graphene (VG) arrays in electric field‐assisted plasma enhanced chemical vapor deposition (PECVD) system is reported. Under the optimum intensity and direction of electric field and by introducing the highly electronegative chlorine into the reactor, the record growth rate of 11.5 µm h−1 is achieved and VG with a height of 100 µm is successfully synthesized. The theoretical study for the first time reveals that the introduction of chlorine accelerates the decomposition of methanol and thus promotes the VG growth in PECVD. Finally, as an excellent filler framework in polymer matrix, VG arrays are used to construct a free‐standing composite TIM, which yields a high vertical thermal conductivity of 34.2 W m−1 K−1 at the graphene loading of 8.6 wt% and shows excellent cooling effect in interfacial thermal dissipation of light emitting diode.
With a chloroform‐assisted method, a record growth rate of 11.5 µm h−1 was achieved and vertical graphene arrays with a height of 100 µm was successfully synthesized. Vertical graphene together with polydimethylsiloxane were used to construct a free‐standing thermal interface material, which yielded a high vertical thermal conductivity of 34.2 W m−1 K−1 and excellent cooling effect in light emitting diode.
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Highlights
A three-tiered thermal interface materials was proposed with the through-plane thermal conductivity up to176 W m
−1
K
−1
and contact thermal resistance as low as 4–6 K mm
2
W
−1
(double ...sides).
The liquid metal acts as a buffer layer to connect vertically aligned graphene with the rough heater/heat sink, improving effective contact thermal conductance by more than an order of magnitude.
Developing advanced thermal interface materials (TIMs) to bridge heat-generating chip and heat sink for constructing an efficient heat transfer interface is the key technology to solve the thermal management issue of high-power semiconductor devices. Based on the ultra-high basal-plane thermal conductivity, graphene is an ideal candidate for preparing high-performance TIMs, preferably to form a vertically aligned structure so that the basal-plane of graphene is consistent with the heat transfer direction of TIM. However, the actual interfacial heat transfer efficiency of currently reported vertically aligned graphene TIMs is far from satisfactory. In addition to the fact that the thermal conductivity of the vertically aligned TIMs can be further improved, another critical factor is the limited actual contact area leading to relatively high contact thermal resistance (20–30 K mm
2
W
−1
) of the “solid–solid” mating interface formed by the vertical graphene and the rough chip/heat sink. To solve this common problem faced by vertically aligned graphene, in this work, we combined mechanical orientation and surface modification strategy to construct a three-tiered TIM composed of mainly vertically aligned graphene in the middle and micrometer-thick liquid metal as a cap layer on upper and lower surfaces. Based on rational graphene orientation regulation in the middle tier, the resultant graphene-based TIM exhibited an ultra-high thermal conductivity of 176 W m
−1
K
−1
. Additionally, we demonstrated that the liquid metal cap layer in contact with the chip/heat sink forms a “liquid–solid” mating interface, significantly increasing the effective heat transfer area and giving a low contact thermal conductivity of 4–6 K mm
2
W
−1
under packaging conditions. This finding provides valuable guidance for the design of high-performance TIMs based on two-dimensional materials and improves the possibility of their practical application in electronic thermal management.
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