The rapid advancement of aerospace, transportation, and electronic technologies has rendered efficient thermal management performance a critical determinant for the operational stability and reliability of polymer-based thermal interface materials (TIMs). Herein, inspired by the thermoregulatory mechanism in mice, which involves calcium ion uptake through the skin, we hypothesize that a bio-inspired and sustainable strategy to enhance the thermal transport capability of natural rubber (NR)-based TIMs through Zeta potential regulation of graphene oxide (GO) using a bio-derived zwitterionic molecule, arginine (Arg), which effectively mitigated electrostatic repulsion, resulting in superior dispersion and suppressed filler agglomeration within the polymer matrix. Consequently, the carbon black/arginine-graphene oxide/natural rubber (CB/Arg-GO/NR) composites exhibited remarkable thermal dissipation enhancements. The through-plane thermal conductivity was boosted by 10.8 times, reaching 2.36 W m-1 K-1, while the compression-induced temperature rise decreased by 1.98% (to 9.9 degrees C) at a GO loading of 0.5 wt%. Moreover, CB/Arg-GO/NR TIMs demonstrated superior heat dissipation in practical evaluations, effectively reducing LED surface temperature and maintaining stable CPU performance. This work introduces a green, molecular-level interfacial engineering approach that leverages bio-derived zwitterionic modifiers to regulate surface potential and enhance phonon transport pathways, offering a promising and eco-friendly solution for next-generation thermal management in high-power electronic systems.

With advancements in aerospace, transportation, and electronics, thermal management in polymer-based composites is critical for high-load applications. Inspired by nature, this study proposes a dual biomimetic strategy which combines a bio-potential regulation by mimicking mouse self-adaptive thermal management and a nacre-inspired brick-and-mortar architecture. Specifically, graphene oxide (GO) is synergistically modified with bio-derived arginine (Arg) and amino-modified silica (SiO2-NH2) via covalent grafting, which precisely tunes the Zeta potential of GO to −28.8 mV. Meanwhile, the covalent linkage between GO as bricks and SiO2-NH2 as mortar constructs a robust brick-and-mortar structure, ensuring efficient phonon transport pathways. The resulting carbon black/amino-silica-arginine-graphene oxide/natural rubber composites (CB/SiO2-NH2-Arg-GO/NR) exhibit excellent mechanical and thermal properties, achieving a tensile strength of 30.8 MPa, tear strength of 77.0 N/mm, and through-plane thermal conductivity of 5.24 W m−1 K−1. Moreover, the composites show superior heat dissipation in high-power LEDs and CPUs, effectively lowering LED surface temperatures by 29.8 °C and ensuring CPU stability. This work demonstrates that the synergistic combination of bio-inspired Zeta potential regulation and brick-and-mortar structural design effectively optimizes filler-matrix interactions and boosts the thermal management capabilities of polymer-based composites, providing a viable solution to thermal issues in high-power electronics.

Driven by the increasing integration and higher power requirements of electronics, polymer-based composites with high-performance in terms of thermal conductivity (TC) and electromagnetic (EM) wave absorption have become an important issue. Herein, multi-layer boron nitride-carbon nanotube/carboxymethyl cellulose/polydimethylsiloxane (BN-CNT/CMC/PDMS) composites with enhanced interface interactions and continuous thermal pathways with gradient impedance were manufactured through a strategy involving chemical surface modification, directional freeze casting, freeze drying and matrix infiltration. Benefiting from the covalent bonding effect between fillers as well as the consecutive thermal conductive pathways, the obtained composites achieved a maximum through-plane TC of 3.56 W m K-1 at a filler content of only 8 wt%. Meanwhile, the composites also achieved an ultra-wide effective electromagnetic wave absorption bandwidth (EMB) of 13.45 GHz, which was attributed to the precisely controllable electromagnetic parameters and the gradient impedance structures. Therefore, these results fully indicate that the composites have great application potential as packaging materials for advanced electronics.

For the preparation of high-performance natural rubber (NR)/graphene oxide (GO) composites, in this study, the effect of modifier charge on the interfacial interaction between GO and NR was investigated. Surfactants with different charges were used to modify GO, and the composites were prepared by latex co-precipitation, and the rubber structures were characterized at the latex, mixing, and vulcanizing rubber stages, respectively. The results showed that the positively charged surface modifier cetyltrimethylammonium bromide (CTAB) acted as bridge between GO and NR chains through electrostatic interaction, significantly enhanced interfacial interaction, and improved the stress transfer efficiency, thus enhancing the material properties. When the filler content was 0.5 phr, the tensile and tear strengths of NR composites (V-NR/GC) prepared with positively charged modified GO were significantly increased to 28.5 MPa and 108.8 N/mm, which were 13.1 % and 35.0 % higher than unmodified V-NR/GO. Entanglement Bound Tube (EBT) mode and Molecular Dynamics (MD) simulations showed that, at the molecular level, NR/GC had the highest binding energy (Ebinding) and the smallest free volume fraction (FFV), which significantly enhanced the chemical cross-linking. This study provides theoretical guidance to enhance the interfacial properties of rubber composites through microstructure modulation, which promotes the application of GO in rubber.

The integrated design and mechanical enhancement of multifunctional electromagnetic interference shielding and infrared stealth aerogels are challenging for the development and application of novel aerogels. Here, inspired by the biological exoskeleton to enhance the body, we develop the exoskeleton-like aramid nanofiber/ polyimide/MXene (APM) aerogel through a secondary impregnation strategy. For APM aerogel, the polyimide reinforcement layer makes the aerogel more elastic and tough; the Ti3C2Tx-MXene exoskeleton enhances the strength and stiffness of the aerogel. Importantly, Ti3C2Tx-MXene forms a continuous conductive network on the surface of the airgel backbone, resulting in high-performance electromagnetic interference (EMI) shielding (EMI shielding efficiency reached 55.315 dB at an ultra-low Ti3C2Tx content of 0.58 vol%), high-efficiency infrared radiation (IR) stealth (ultra-low thermal conductivity of 0.0666 W & sdot;m � 1 & sdot;K- 1 and IR emissivity of 0.566 at 3-5 mu m and 0.55 at 8-14 mu m). This study provides a way to design robust aerogel materials with infrared stealth and electromagnetic shielding compatibility.

Polymer-based thermal interface materials (TIMs) with excellent thermal conductivity and heat dissipation capabilities play a crucial role in addressing the issue of heat accumulation in advanced integrated electronics. However, establishing improved surface interactions and complete networks to enhance efficient phonon transfer remains a significant challenge. To tackle this problem, surface modification and ice-templating techniques are commonly employed to create the robust interface crosslinks and continuously thermal conductive pathways. Herein, 2-mercaptobenzimidazole (MB) was used as a reducing and modifying agent to functionalize graphene oxide (rGO-MB) within the three-dimensional networks, which was prepared using a combination of hydrothermal and ice-templating methods. As a result, the reduced graphene oxide/natural rubber (rGO-MB/NR) TIMs exhibited a remarkable through-plane thermal conductivity of 0.93 W m-1 K-1 with a filler loading of 3 wt%. The enhanced interface interactions between rGO-MB and NR, combined with the establishment of a three-dimensional network, significantly contributed to the improved thermal conductivity and heat dissipation capabilities. Moreover, the obtained TIMs demonstrated favorable mechanical properties (5.06 MPa, 502%) and excellent insulation performance (3 x 1013 omega cm). These findings provide the valuable insights into potential solutions for mitigating heat accumulation issues in next-generation electronics.HighlightsrGO-MB with thiol groups was obtained by the hydrothermal method.Interactions between rGO-MB and NR mainly depended on the chemical bonds.rGO-MB/NR TIMs owned the improved thermal management performance. The preparation process of surface modified GO and the rGO-MB/NR TIMs.image

Numerous researches have drawn on the polymer-based thermal conductive composites to cope with heat dissipation issue both in the integrated electronics and human body. However, the limited thermal conductivity and mono-cooling mode even in the high filler content are always restricted its further application. Currently, the use of latent heat from phase transition has aroused researchers' appetite for the thermal management. Herein, inspired by the sweat modulating the body temperature, a passive dual thermal management strategy was proposed by taking advantage of high latent heat and the improved thermal conductivity, where the liquid-vapor phase transition of water inside the MOF coated on the polymer-based composites to form the heterogeneous composites. In the proof-of-concept test, the obtained MIL-101 (Cr) MOF as the sorbent owned the high specific surface area of 1850 cm(3)/g, cyclic water uptake of 1.18 g and phase change enthalpy of 1780 J/g, which promoted the well spontaneous adsorption and desorption ability of water. While sulfur surface modified boron nitride/natural rubber composites (BN-S/NR) exhibited the excellent anisotropic thermal conductivity (11.48 W m(-1) K-1) in the through-plane direction at the filler loading of 70 wt%. After the MIL-101 (Cr) MOF coated composites (MOF-BN-S/NR) with heterogeneous structure, the composites with 0.07 g MOF possessed the pretty cooling performance and thermal stability to adjust temperature at a proper range both in electronics and human body because of the dual passive heat dissipation approach. Therefore, these findings provide the meaningful insight into research to fabricate composites with heterogeneous-assisted heat dissipation in thermal management.

With the rapid development of modern transportation systems, optimizing the relationship between structure and performance to obtain natural rubber-based nanocomposites with excellent comprehensive performance is still worth to investigation. Herein, the regulation of flocculation potential through different flocculants selection on the thermomechanical properties for carbon black/graphene oxide reinforced natural rubber (CB/GO/NR) nanocomposites were investigated based on the compression electric double layer theory. The results showed that formic acid owned the highest zeta potential with comparison of sodium chloride (NaCl), calcium chloride (CaCl2), and aluminum chloride (AlCl3). Meanwhile, as the content was 8 wt%, tensile strength, tearing strength and thermal conductivity could achieve to 27.64 MPa, 56.89 N/mm, and 1.05 W m-1 K-1, respectively. While the heat generation after compression fatigue dropped to 10.1 degrees C. These findings reveal that the highest zeta potential of formic acid could promote the improvement of flocculation degree between GO and NR latex and significantly enhanced the thermomechanical properties of CB/GO/NR nanocomposites due to the larger flocculation potential difference. Therefore, this study not only provides important theoretical insights for preparing high-performance NR-based nanocomposites, but also highlights the crucial role of high zeta potential flocculants in optimizing the composite performance. More importantly, the findings offer the creative insights for preparation of the excellent comprehensive NR nanocomposites for the practical industry application.Highlights The effect of flocculation degree on the properties of CB/GO/NR composites was studied. Formic acid was benefit to the flocculation and could promote the surface interaction. CB/GO/NR composites possessed the improved thermal and mechanical properties.

Herein, the carbon black/graphene oxide/natural rubber composites (CB/GO/NR) with different crosslink networks were prepared through the latex co-precipitation approach. Meanwhile, the type of crosslinks on the crack propagation resistance and fatigue life in different vulcanized systems was investigated. As a result, CB/GO/NR composites dominated by polysulfide in the conventional vulcanization (CV) system exhibited the highest tear strength (71.6 kN/m) and lowest crack growth rate (64.1 nm/cycle), the crosslink network and polysulfide-based crosslink structure in the CV system were the key factors to improve the crack propagation resistance. In addition, the relationship between viscoelasticity and dynamic crack propagation behavior of CB/GO/NR is studied, and the CV system had the lowest loss compliance modulus (J″ = 0.0014 Mpa−1), thus more energy dissipation occurred in the crack propagation region and the crack propagation resistance of CV system was improved. Importantly, this work can provide the guideline for designing the rubber-based composites in the practical engineering applications.

Polymer-based thermal interface materials (TIMs) have been widely used in electronics to enhance heat transfer through the chip to heat sink. However, it remains a severe challenge to build the efficient phonon transfer pathways for improving the thermal conductivity and heat dissipation ability to cope with the increasing power density. Nowadays, TIMs with introduced template have attracted a great deal of attention because of the continuously three-dimensional (3D) structures. Herein, the reduced graphene oxide (rGO) with 3D networks was fabricated through the self-sacrificing template of melamine foam. Meanwhile, the reduced graphene oxide/natural rubber (rGO/NR) TIMs were prepared by the vacuum-assisted infiltration approach. As a result, the obtained TIMs exhibited the improved thermal conductivity (1.53 W m−1 K−1) and the good electromagnetic interference (EMI) shielding performance (26 dB) in X band at the filler content of 1.15 vol

With the rapid development of transportation system, the safety, reliability, and durability of green tires play an important role in modern transportation. While for the material preparation, the poor dispersion ability of reinforced filler and the weak interfacial interactions with polymer matrix seriously restricted the further application in the green tire field. Meanwhile, avoiding the use of organic solvents is also an environmental issue that needs to be considered in the preparation process. Herein, water-soluble 2-mercapto-1-methylimidazole (MMI) functionalized graphene oxide (GO-MMI) was obtained through a simple, green and one-step hydrothermal method. Additionally, the modified graphene oxide/natural rubber composites (GO-MMI/NR) with different GO-MMI content were prepared by the latex coprecipitation approach. As a result, the modified GO-MMI could be evenly dispersed in the NR matrix through the mechanical blending and the obtained GO-MMI/NR composites possessed the good comprehensive properties after vulcanization. Specifically, the tensile strength (26.8 MPa), elongation at break (801%), low heat build-up (6.2 degrees C), Deutsches Institute for Normung (DIN) abrasion loss volume (71.31 mm(3)) and heat resistance index (162.1 degrees C) were synchronic-lifting when compared with the GO/NR composites. The results demonstrated that obtained GO-MMI/NR composites owned the promising application for the industrial-scale green tires.

Polymer-based thermal interface materials (TIMs) with good comprehensive properties remains a severe challenge for the advanced electronics. Herein, the vertically aligned boron nitride-Mxene (BN-Mxene) hybrids with improved surface interaction were introduced to enhance the thermal conductivity of the polydimethylsiloxanebased (PDMS) TIMs. Specifically, the BN-Mxene hybrids with improved surface interactions were mainly relay on the hydrogen and 7C-7C bonds from the hydroxylated boron nitride (BN-OH) and etched Ti3AlC2 (MAX). Meanwhile, the vertically aligned structures of the obtained TIMs were formed through the modified bidirectional freeze-drying approaches. As a result, the boron nitride-Mxene /polydimethylsiloxane (BN-Mxene/PDMS) TIMs exhibited the elevated through-plane thermal conductivity (2.03 W m-1 K-1), good electromagnetic wave absorption (-49.37 dB, 5.8 GHz) and the compression elasticity properties at a filler loading of 15 wt%. Importantly, the findings provided a bright prospect in the application of next-generation electronics.

Over the past half-century, the increase of on-chip power and on-chip integration density has created new thermal management challenges for 2.5D/3D semiconductor packaging. High-performance thermal management materials in electronic encapsulation are very important to ensure the performance and reliability of the electronic devices. Graphene-based polymer composites have attracted much attention due to the ultrahigh thermal conductivity and large surface area of graphene. However, graphene nanosheets easily aggregate and lack functional groups on their surfaces, leading to phonon scattering within the interfaces. In this work, silver nanoparticles are in-situ formed on the graphene surface by a facile method, then the graphene-silver nanofillers are modified by (3-Mercaptopropyl)trimethoxysilane (MPTS). MPTS reacts with silver nanoparticles to connect them with epoxy. Also, silver nanoparticles on the surface of graphene can fuse together to form metallurgical joints that connect graphene nanosheets. With the fundamental understanding of sintering mechanisms and reducing two types of thermal interfacial resistances (filler-filler and filler-epoxy interface resistances) simultaneously, the resultant epoxy nanocomposites achieve a high through-plane thermal conductivity of 0.99 W/mK at 8 wt% loading. This corresponds to a 465.7% increase in thermal conductivity as compared to that of neat epoxy. Also, the nanocomposites present a low CTE and high thermal stability. They show strong cooling capability and heat dissipation as thermal interface materials (TIMs) through both experimentation and simulation, providing a promising new insight into thermal management materials to meet the demands of next generation high-power and high-density semiconductor packaging.

Composites with high thermal conductivity are urgently needed for thermal management devices. Although natural rubber (NR) with excellent elasticity are promising as flexible polymer for thermal management, their poor thermal conductivity limits their applications. In this work, a general water treatment route and an ice template process are used to prepare a 3D graphene aerogel. And environmentally friendly L-cysteine (Cys) are used to adjust the carbon-to-oxygen ratio of GO and thiol-functionalized GO. Benefiting from the 3D graphene network and strong interfacial interaction, the NR composites with graphene loading of 25 wt% showed thermal conductivity of 0.891 W/(m center dot K). At the same time, it also has good mechanical properties and antistatic prop-erties. All the results indicate that Cys-GO@GNP/NR is expected to be a promising thermal management material.

It has become the mainstream way to take advantage of the new carbon materials to modify polymer matrix to prepare thermal interface materials (TIMs) with excellent comprehensive properties for the modern electronic packaging materials. Yet, how to make full use of the properties of new carbon materials is still facing the severe challenges. Herein, thiol-functionalized carbon nanotubes/natural rubber (CNTs-SH/NR) TIMs with three-dimensional networks (3D) and covalently bonded filler/matrix interactions were fabricated through the sur-face chemical treatment as well as ice-templated approach. The results proved that CNTs-SH/NR TIMs could achieve a high through-plane thermal conductivity of 1.22 W m-1 K-1 with CNTs-SH content was 25 wt%. Simultaneously, it showed sensitive heat response capacity. The improvement of filler/matrix interface and 3D networks were of great importance in abating the total thermal resistance. Moreover, the method provide a novel route to design high-performance thermal conductive TIMs and apply for the thermal management of electronics.

Thermal interface materials (TIMs) with excellent comprehensive performance which own high thermal conductivity, good electrical insulation and mechanical properties have triggered considerable interests in addressing the interfacial transfer issue for the state-of-the-art electronic devices. Herein, a new method was developed to covalently bonded crosslink boron nitride (BN) and reduced graphene oxide (rGO) by the chemical surface modification technology and chemical reaction between the erent functional groups. Meanwhile, the integrated three-dimensional (3D) networks of BN-rGO filler and natural rubber (NR) matrix were fabricated by the ice-templated method. After vulcanization, the boron nitride-reduced graphene oxide/ natural rubber (BN-rGO/NR) TIMs owned good comprehensive performance. As a result, the highest through-plane thermal conductivity could reach 1.04 W m(-1) K-1 and also possessed sensitive response ability of heat flux. Importantly, the approach provided a valuable guidance to design TIMs with excellent comprehensive properties and owned promising applications in the thermal management of electronics.

Owing to the rapid development towards high power density of the modern electronics, heat accumulation and low dissipation efficiency seriously affect its service lifetime. To settle this problem, polymer-based thermal interface materials (TIMs) with high thermal conductivity have become the mainstream strategy to eliminate influence of air factor between chip and heat sink. Herein, the covalently bonded CNTs-rGO hybrids assisted NR hydrogel was proposed by one-step method and then treated by hot-pressing approach to obtain TIMs. As a result, such TIMs exhibited a superior through-plane thermal conductivity of 1.82 W m -1 K -1 , the good tensile strength of 14.5 MPa and the excellent stress sensing capability. The results demonstrated that the strongly interactions and well-ordered structures played the important role in ameliorating thermal conductivity. Simultaneously, the excellent stress sensing capability is benefit to detect its operation stability. Importantly, this work provides the meaningful guidance to design highly comprehensive performance TIMs.

Deposited 3D Ag@T-ZnO and intertwined 1D MWCNTs carbon/metal hybrid conductive network structure in the self-assembly enhanced epoxy curing network.

The vertically arranged structure and strong interface interaction promote a great improvement in the thermal conductivity of the composites.