PI Composites Research Articles

Integrated Thermal Conductive and Electromagnetic Interference Shielding Performance in Polyimide Composite: Impact of Carbon Felt-Graphene Van der Waals Heterostructure.

With the widespread application of highly integrated electronic devices, the urgent development of multifunctional polymer-based composite materials with high electromagnetic interference shielding effectiveness (EMI SE) and thermal conductivity capabilities is critically essential. Herein, a graphene/carbon felt/polyimide (GCF/PI) composite is prepared through constructing 3D van der Waals heterostructure by heating carbon felt and graphene at high temperature. The GCF-3/PI composite exhibits the highest through-plane thermal conductivity with 1.31 W·m-1·K-1, when the content of carbon felt and graphene is 14.1 and 1.4 wt.%, respectively. The GCF-3/PI composite material achieves a thermal conductivity that surpasses pure PI by 4.9 times. Additionally, GCF-3/PI composite shows an outstanding EMI SE of 69.4dB compared to 33.1dB for CF/PI at 12GHz. The 3D van der Waals heterostructure constructed by carbon felt and graphene sheets is conducive to the formation of continuous networks, providing fast channels for the transmission of phonons and carriers. This study provides a guidance on the impact of 3D van der Waals heterostructures on the thermal and EMI shielding properties of composites.

5‐aminobenzimidazole@graphene oxide nanosheets doped polyimide nanocomposites: Low‐temperature curing and improved mechanical properties

AbstractThe preparation of polyimide matrix composites with low curing temperature and high mechanical properties is of great importance. In this study, a low‐cost and multi‐functional nanofiller, 5‐aminobenzimidazole grafted graphene oxide (5‐ABZ@GO) has been designed. By nucleophilic attack on 5‐aminobenzimidazole basic groups and doping of GO, the above requirements of polyimide composites were skillfully realized. The results show that when the addition of 5‐ABZ@GO is 1%, the 5‐ABZ@GO/PI nanocomposites can achieve complete imidized at 200°C. Moreover, the nanocomposite prepared by imidization at 200°C has good mechanical and thermal properties (tensile strength is 141.64 MPa, modulus is 6.05 GPa, T5% is as high as 543.5°C), which is better than the PI composites prepared at 320°C. This study provides an innovative approach to preparing polyimide composites that meet mechanical performance requirements while utilizing comparatively lower curing temperatures, low curing temperature polyimide resins provide a new path for integrated composites with structure–function integration.

Fabrication of hybrid polyimide composites containing Ladder-like poly(phenyl-co-glycidoxypropyl)silsesquioxane)

Ladder-like structured poly(phenyl-co-glycidoxypropyl) silsesquioxanes with different ratios of phenyl to glycidyl group (LPS64 and LPS 82) were synthesized using simple hydrolysis reaction followed by condensation polymerization of phenyltrimethoxysilane (PTMS) and (3-glycidyloxypropyl)trimethoxysilane (GPTMS). Two series of hybrid polyimide composites (PI/LPS64 and PI/LPS82) with different contents of LPS (10, 20, and 30 wt%) were prepared by the chemical reaction of epoxy groups in LPS64 or LPS82 and the terminal amine groups in poly(amic acid). The dielectric constant (k) of hybrid PI composites (k = 1.3) was lower than that of pure polyimide (k = 2.9) and the degree of roughness was increased according to the increase of LPS contents. The dispersion of LPS in the PI matrix was improved due to the chemical bonding between LPS and PI. The thermal stability of PI/LPS82 was higher than that of PI/LPS64 due to the enhanced π-π stacking between PI matrix and LPS82 with more phenyl groups as compared to LPS64.

Excellent thermal conductivity and electrical insulation in polyimide/graphene oxide/carbon nanotubes composites

AbstractPolymer composites with heat resistance, good thermal conductivity, and insulation properties can meet the special needs of electronics and electrical appliances. In this work, graphene oxide (GO) and carbon nanotubes (CNTs) are coated by polydopamine (PDA). 4,4′‐diaminodiphenyl ether (ODA), pyromellitic dianhydride (PMDA), and 4,4′‐oxydiphthalic anhydride (ODPA) in‐situ polymerize to prepare poly(amide acid) (PAA) containing thermally conductive yet insulating fillers (PDA@GO, PDA@CNTs). As the concentration of fillers in PI composites increases, the thermal conductivity rises, but the insulation property decreases. Keeping the filler content constant and varying the ratio of PDA@GO and PDA@CNTs, the thermal conductivity increases and then decreases. When PDA@GO and PDA@CNTs have a mass ratio of 10:1, the significant synergistic effect affects the thermal conductivity. The PI/PG10C1–25 sample has a thermal conductivity of 1.46 W/(m·K), which is 6.9 times greater than the pure PI. Additionally, the volume resistivity, dielectric permittivity, and dielectric loss (100 kHz) of PI/PG10C1–25 are 2.8 × 1013 Ω cm, 5.4 and 0.28, respectively. The heat resistance of PI composites is almost the same as that of pure PI. Given these outstanding attributes, the developed PI composites offer vast applications in many fields.Highlights Synergistic PDA@GO and PDA@CNTs (10:1) optimize thermal conductivity. PI/PG10C1–25 achieves 6.9 times higher thermal conductivity than pure PI. Volume resistivity of PI/PG10C1–25 reaches 2.8 × 1013 Ω·cm. Dielectric permittivity of PI/PG10C1–25 reaches 5.4 at 100 kHz. Developed PI composites maintain excellent heat resistance.

Improved Tribological Performance of MOF@MXene/PI under High Temperature.

High-temperature-resistant and self-lubricating polymer composites with long life and high reliability are increasingly indispensable in the aerospace field. Herein, ZIF-67 grown on the MXene lamella was successfully prepared, and ZIF-67@MXene/PI composites with a regular layered structure were obtained by a hot-pressing three-dimensional network aerogel. It was revealed that incorporating ZIF-67@MXene into PI dramatically reduced the friction and abrasion with elevated temperatures. Largely, aerogel walls always paralleled the sliding direction by compressing, providing a significant antifriction effect. More notably, the presence of a vigorous tribofilm composed of a PI matrix and a diamond-type lattice MOF-modified MXene provided rolling and sliding interface friction under high temperatures, simultaneously. In addition, the uniform tribofilm with a thickness of about 200 nm can effectively avoid the direct contact of the friction pair during the sliding process. Hence, the combination of the constructed multiscale nanocomposites and nanostructured tribofilm with outstanding tribological performance endow the material potentially useful in reducing energy consumption, thus addressing the energy wastage problem caused by friction.

Highly lubricating and wear‐resistant Ti3C2Tx@SiO2/PI composites based on the action of transfer film at the friction surface

AbstractPolyimide (PI) is a special engineering plastic, widely involved in mechanical components, instruments, and petrochemicals. However, single PI material is inevitably subject to wear and tear in practice, which leads to weakened material properties. In this work, Ti3C2Tx@SiO2 was prepared to enhance the wear resistance and lubrication properties of PI by intercalating SiO2 into the interlayer of Ti3C2Tx sheets. Ti3C2Tx@SiO2/PI composites were fabricated in two steps to test the tribological performances. SiO2 particles change the form of interfacial friction from sliding to rolling, thus relieving direct friction between material and steel ball. So, the composites have a minimum COF (COF = 0.33) when the content of Ti3C2Tx@SiO2 is 0.80 wt%. Moreover, the average value of wear rate was 0.24 × 10−5 mm3/(N·m) when Ti3C2Tx@SiO2 content was 1.60 wt%, which was 91.0% lower compared to the PI matrix. During the friction process, the abrasive chips of the material migrate to the surface of the steel ball to form a transfer film, which protects the material and thus reduces the wear rate. Therefore, the hybrids Ti3C2Tx@SiO2 are effective and important wear‐resistant agents and solid lubricants to improve the wear resistance and lubricity of PI or other polymer materials.Highlights SiO2 insert Ti3C2Tx is a key factor in changing sliding friction into rolling friction, effectively reducing the COF. The average wear rate was 91.0% lower than that of the polyimide matrix when Ti3C2Tx@SiO2 content was 1.60 wt%. The minimum COF of Ti3C2Tx@SiO2/PI composites reached 0.33 when the content of Ti3C2Tx@SiO2 was 0.80 wt%. The transfer film effectively reduces further wear of the material during friction.

Phase field model for electric-thermal coupled discharge breakdown of polyimide nanocomposites under high frequency electrical stress

In contrast to conventional transformers, power electronic transformers, as an integral component of new energy power system, are often subjected to high-frequency and transient electrical stresses, leading to heightened concerns regarding insulation failures. Meanwhile, the underlying mechanism behind discharge breakdown failure and nanofiller enhancement under high-frequency electrical stress remains unclear. An electric-thermal coupled discharge breakdown phase field model was constructed to study the evolution of the breakdown path in polyimide nanocomposite insulation subjected to high-frequency stress. The investigation focused on analyzing the effect of various factors, including frequency, temperature, and nanofiller shape, on the breakdown path of Polyimide (PI) composites. Additionally, it elucidated the enhancement mechanism of nano-modified composite insulation at the mesoscopic scale. The results indicated that with increasing frequency and temperature, the discharge breakdown path demonstrates accelerated development, accompanied by a gradual dominance of Joule heat energy. This enhancement is attributed to the dispersed electric field distribution and the hindering effect of the nanosheets. The research findings offer a theoretical foundation and methodological framework to inform the optimal design and performance management of new insulating materials utilized in high-frequency power equipment.

Thermo-mechanical properties and internal architecture of PI composites for high-pressure hydrogen applications

The efficient transport of Hydrogen is pivotal to the wide scale adaption of energy produced from renewable sources. Reciprocating piston compressors with high strength non-lubricated sealing solutions for piston and rod packing rings will be a key technology to fulfill gas purity and high-pressure gradients demands set by hydrogen applications. Polyimide polymer matrix composites have seen use in tribological applications and promise high mechanical strength and temperature resistance. The presented work describes carbon fiber reinforced Polyimide blends in comparison, characterized by complementary advanced methods to investigate their properties and potential for reciprocating compressor applications. Thermo-mechanical and tribological testing was supported by microstructure analysis utilizing synchrotron tomography and electron microscopy, pinpointing the necessity of dry lubricating additives such as PTFE. New insights in micromechanical deformation behavior of fiber reinforced polymers are given and promising fiber-reinforced polyimide compositions suitable for high-pressure hydrogen compression applications were identified.

Bioinspired construction of size adjustable hollow polydopamine microspheres for ultra-low dielectric polyimide composites

Polydopamine (PDA) has been extensively investigated due to its excellent adhesion ability and versatile chemical potential for secondary reactions. However, the potential application of hollow polydopamine microspheres (H-PDA) in the field of low-dielectric electronic packaging remains an unexplored area. Here, H-PDA microspheres with adjustable size were synthesized by a template-assisted approach, and the influence of size and content of H-PDA on the comprehensive performance of PI/H-PDA composites was explored in detail. The morphology observation revealed that the presence of H-PDA could be homogeneously dispersed in the PI matrix, and the PI/H-PDA composite containing 2 wt% H-PDA-800 achieved the lowest dielectric constant of 1.96 with a dielectric loss of 0.0123 at 1 MHz. It was attributed to the synergistic effects of nano-sized air bubbles from H-PDA and the dielectric confinement effect. Meanwhile, PI/H-PDA composites maintained high thermal stability (T5> 517 °C). In addition, the incorporation of H-PDA had a strengthening and toughening effect on PI composites, which can be explained by the sliding theory of macromolecular chains. This work offers a feasible strategy to obtain ultra-low dielectric constant of porous PI composites while maintaining good mechanical properties and thermal stability.

Investigate on the dry friction tribological behaviors and mechanism of carbon quantum dot/polyimide composites coating

The comprehensive utilization of biomass resources is to be prepared into functional nanomaterial. This paper prepared carbon quantum dots (CQDs) using citric acid. A new CQDs/polyimide composites (CQDs/PI) coating fabricated on the surface of steel disks, has been widely used in bearing sleeve material or coatings in marine equipment parts and aerospace industries. Tribological properties of coating materials were investigated at different loads and reciprocating speeds of 10 mm/s under dry sliding conditions using a UMT-2 tribometer and compared to those of commercial MoS2 particles in PI composites. Scanning electron microscopy accompanied by energy spectroscopy (SEM/EDS) and 3D laser scanning microscopy were used to characterize the morphologies of the abrasion marks to clarify the tribological mechanisms. Results show that different levels of CQDs can improve composite coatings' anti-wear and friction reduction properties. The tribological mechanisms of CQDs were attributed to the enhancement of the hardness of the polyimide coatings by the CQDs and the formation of a transfer film on the surface of the ceramic balls during the friction process reducing the direct contact at the friction sub-interface.1

Tough polyimide composites synergistically reinforced by carbon nanofiber-grafted carbon fiber and rGO for improved heat dissipation and electromagnetic interference shielding

The rapid miniaturization and a consequent increase in electromagnetic wave (EM) and heat emission in integrated electronic devices are now urgently desiring for multifunctional polymer composites that simultaneously possess high mechanical properties, excellent electromagnetic interference (EMI) shielding ability and heat dissipation capability. Herein, a series of novel polyimide-based composite films were constructed by rationally assembling the carbon nanofiber-grafted carbon fiber (NCF) and reduced graphene oxide (rGO) into a highly electrically and thermally conductive pathway within polyimide matrix via a sequential bidirectional freezing casting and hot-pressing strategy. The combination of high tensile strength and toughness was obtained by incorporating rGO into the NCF-reinforced PI composite, giving rise to a hierarchical reinforcing structure of NCF and crack deflection induced by rGO nanosheets. The high electrical conductivity (7.0 × 103 S m−1) endows the PI/NCF30/rGO3.5 composite film with a good EMI shielding effectiveness of 45 dB. Moreover, the well-aligned thermally conductive NCF and rGO and strong interfacial bonding between the polymer matrix and reinforcing fibers give rise to improved thermal conductivity (λ), particularly along the in-plane direction. Typically, the PI/NCF30/rGO3.5 exhibits an in-plane thermal conductivity of 5.18 W m−1 K−1, ∼4.7 times increment compared to the pure PI (0.91 W m−1 K−1). Besides, the resultant PI/NCF30/rGO3.5 composite film presents a superior Joule heating performance with some features of fast thermal response, ease of regulation and sufficient reliability. Accordingly, the developed multifunctional polyimide-based composite films demonstrate high potential as advanced EMI shielding materials with excellent heat dissipation.

Adaptive strategies of plants to conserve internal phosphorus under P deficient condition to improve P utilization efficiency.

Phosphorus (P) is one of the limiting factors for plant growth and productivity due to its slow diffusion and immobilization in the soil which necessitates application of phosphatic fertilizers to meet the crop demand and obtain maximum yields. However, plants have evolved mechanisms to adapt to low P stress conditions either by increasing acquisition (alteration of belowground processes) or by internal inorganic P (Pi) utilization (cellular Pi homeostasis) or both. In this review, we have discussed the adaptive strategies that conserve the use of P and maintain cellular Pi homeostasis in the cytoplasm. These strategies involve modification in membrane lipid composition, flavanol/anthocyanin level, scavenging and reutilization of Pi adsorbed in cell wall pectin, remobilization of Pi during senescence by enzymes like RNases and purple acid phosphatases, alternative mitochondrial electron transport, and glycolytic pathways. The remobilization of Pi from senescing tissues and its internal redistribution to various cellular organelles is mediated by various Pi transporters. Although much efforts have been made to enhance P acquisition efficiency, an understanding of the physiological mechanisms conserving internal Pi and their manipulation would be useful for plants that can utilize P more efficiently to produce optimum growth per unit P uptake.

Synergistic effects of boron nitride sheets and reduced graphene oxide on reinforcing the thermal conduction, SERS performance and thermal property of polyimide composite films

AbstractPolyimide (PI) composite films with hybrid fillers containing hBN (hexagonal boron nitride) sheets and rGO (reduced graphene oxide) were successfully fabricated by in‐situ polymerization. Herein, hBN sheets and rGO were obtained by ball milling and chemical reduction, respectively. In PI composite films, hBN can be tightly attached onto the surface of rGO via π‐π interaction, which can benefit the construction of heat‐conduction pathways and reduce boundary of heat resistance. The results show that the addition of rGO and hBN could enhance the thermal conductivity by synergistic effects. Specially, hBN and rGO are at the weight ratio of 1:1 and at the total loading of 33 wt%, thermal conductivity of PI composites can reach up to 1.19 Wm−1 K−1, which is 5.61 times higher than that of pure PI. Thermal property and dynamic mechanical property of composite films were also investigated. Besides, compared with pure PI, mixed fillers have obvious surface‐enhanced Raman scattering signals, indicating the synergistic effect of the mixed fillers. Overall, this study gives insights into heat dissipative and high sensitivity analysis components which may be used in the field of high‐temperature micro fabrication.

Dilute Bicelles for Glycosyltransferase Studies, Novel Bicelles with Phosphatidylinositol.

Solution-state NMR can be used to study protein–lipid interactions, in particular, the effect that proteins have on lipids. One drawback is that only small assemblies can be studied, and therefore, fast-tumbling bicelles are commonly used. Bicelles contain a lipid bilayer that is solubilized by detergents. A complication is that they are only stable at high concentrations, exceeding the CMC of the detergent. This issue has previously been addressed by introducing a detergent (Cyclosfos-6) with a substantially lower CMC. Here, we developed a set of bicelles using this detergent for studies of membrane-associated mycobacterial proteins, for example, PimA, a key enzyme for bacterial growth. To mimic the lipid composition of mycobacterial membranes, PI, PG, and PC lipids were used. Diffusion NMR was used to characterize the bicelles, and spin relaxation was used to measure the dynamic properties of the lipids. The results suggest that bicelles are formed, although they are smaller than “conventional” bicelles. Moreover, we studied the effect of MTSL-labeled PimA on bicelles containing PI and PC. The paramagnetic label was shown to have a shallow location in the bicelle, affecting the glycerol backbone of the lipids. We foresee that these bicelles will be useful for detailed studies of protein–lipid interactions.

Fire performance of piperazine phytate modified rigid polyurethane foam composites

Using phytic acid (PA) and piperazine (Pi) as raw materials, piperazine phytate (PA‐Pi) was fabricated by simple ionic reaction. Furthermore, A series of rigid polyurethane foam/piperazine phytate (RPUF/PA‐Pi) composites were prepared by one‐step water‐blown technology. Thermogravimetric (TG) results showed that the addition of PA‐Pi improved the thermal stability of RPUF/PA‐Pi composites at high temperature. At 700°C, RPUF/PA‐Pi20 exhibited the highest carbon residue of 25.8 wt%. Cone calorimetry and smoke density tests suggested that PA‐Pi could reduce the heat and smoke release during combustion process of the composites, thus reducing their fire hazard. Thermogravimetric‐Fourier transform infrared spectroscopy (TG‐FTIR) indicated that PA‐Pi significantly inhibited the release of toxic gases (isocyanate compounds, aromatic compounds, CO and HCN) and flammable gases (hydrocarbons and esters) during the decomposition process of RPUF/PA‐Pi composites, effectively improving fire performance of the composites. Scanning electron microscope (SEM), Raman and Fourier transform infrared spectroscopy (FTIR) were used to characterize the carbon residue of RPUF/PA‐Pi composites. The results showed that PA‐Pi could promote the formation of dense carbon layer of composites and effectively prevented heat and mass transfer in the combustion process.

Enhanced dielectric properties and thermostability in polyimide composites with core-shell structured polyimide@BaTiO3 nanoparticles

Polymer composites with high dielectric constant and thermal stability have shown great potential applications in the fields relating to the energy storage. Herein, core-shell structured polyimide@BaTiO3 (PI@BT) nanoparticles were fabricated via in-situ polymerization of poly(amic acid) (PAA) and the following thermal imidization, then utilized as fillers to prepare PI composites. Increased dielectric constant with suppressed dielectric loss, and enhanced energy density as well as heat resistance were simultaneously realized due to the presence of PI shell between BT nanoparticles and PI matrix. The dielectric constant of PI@BT/PI composites with 55 wt% fillers increased to 15.0 at 100 Hz, while the dielectric loss kept at low value of 0.0034, companied by a high energy density of 1.32 J·cm−3, which was 2.09 times higher than the pristine PI. Moreover, the temperature at 10 wt% weight loss reached 619°C, demonstrating the excellent thermostability of PI@BT/PI composites. In addition, PI@BT/PI composites exhibited improved breakdown strength and toughness as compared with the BT/PI composites due to the well dispersion of PI@BT nanofillers and the improved interfacial interactions between nanofillers and polymer matrix. These results provide useful information for the structural design of high-temperature dielectric materials.

Stable Mixed-Organic-Cation Perovskite MA1–xFAxPbI3 Integrated with MoS2 for Enhanced Visible-Light Photocatalytic H2 Evolution

Unary-organic-cation lead halide perovskites like MAPbI3 have been emerging as tremendous photocatalysts for H2 evolution recently. However, their photocatalytic performances are inferior without modification. Here, a series of mixed-organic -cation perovskites MA1–xFAxPbI3 (M1–xFxPI, x = 0, 0.2, 0.3, 0.4, 0.5) were synthesized by introducing FA+ into MAPbI3 precursor and then composited with MoS2 as photocatalysts for H2 evolution reaction (HER). We demonstrate that the fabricated MoS2/M0.6F0.4PI is highly efficient and ultrastable during the photocatalytic HER process. The optimal MoS2/M0.6F0.4PI composite, i.e., 20 wt % MoS2/M0.6F0.4PI exhibits a visible HER rate of 2131 μmol h–1 g–1, increasing by 88-fold in comparison with pure MAPbI3 (24 μmol h–1 g–1) and better than the optimized Pt/M0.6F0.4PI (1328 μmol h–1 g–1). No activity degradation of 20 wt % MoS2/M0.6F0.4PI occurs in repeated HER experiments. The (photo)electrochemical performances of the composite are studied to reveal the photoinduced charge transfer and consequent HER process.

On the machining behavior of carbon fiber reinforced polyimide and PEEK thermoplastic composites

AbstractPolyimide (PI) and polyetheretherketone (PEEK) are superior high‐performance thermoplastics being extensively used in the fields of fiber‐reinforced polymer composites. However, there is very limited literature addressing the machining behavior of the PI and PEEK composites. The present paper aims to conduct a comparative study into the machining characteristics of these two representative high‐performance thermoplastic matrix composites under varying cutting conditions. Machinability aspects of the carbon/PI and carbon/PEEK thermoplastic composites were evaluated in terms of drilling forces, machining temperatures, delamination damage, surface morphologies, hole dimensional accuracy and tool wear. The results indicate that the carbon/PEEK composites generally show a much poorer machinability than the carbon/PI composites in terms of higher drilling forces, higher cutting temperatures, larger delamination extents and excessive tool wear. Since the carbon/PEEK composites exhibit certain ductility leading to the continuous chip formation, the cut hole surface morphologies and dimensional accuracy are much better than those gained in the carbon/PI composites. Both the cutting speed and the feed rate affect significantly the drilling forces and the resulting delamination damage. The fundamental wear mechanisms of drilling carbon/PI composites are abrasion wear in the form of edge rounding and slight chip adhesion, while for the carbon/PEEK composites, they are abrasion, serious chip adhesion because of the high drilling temperatures promoted at the drill‐work interface and catastrophic failures of coating peeling and edge fracture.

Thermal conductivity and mechanical properties of polyimide composites with mixed fillers of BN flakes and SiC@SiO2 whiskers

AbstractPolyimide (PI) composites with mixed fillers of BN flakes and SiC whiskers exhibit enhanced thermal conductivity and mechanical properties. In order to improve dispersion and interaction of these mixed fillers within the PI matrix, BN flakes were modified by a titanate coupling agent while SiC whiskers were oxidized at 750°C for 60 minutes to produce SiC@SiO2 followed by silane coupling agent modification. PI composites reached a maximum thermal conductivity of 0.95 W/m K at volume fraction of mixed fillers of 27.6 vol% when the weight ratio of BN flakes to SiC@SiO2 whiskers was 1:4. The enhanced thermal conductivity is likely attributed to the formation of heat conductive networks constructed by BN flakes and SiC@SiO2 whiskers and the improved interfacial affinity between fillers and matrix. The optimized Nielsen‐mold confirms the distribution and morphology of fillers affect the thermal conductivity of PI composites. In addition, SiC whiskers enhanced the mechanical property of PI composites and the influence of fillers on the mechanical property was further elaborated.

Stress Controllability in Thermal and Electrical Conductivity of 3D Elastic Graphene‐Crosslinked Carbon Nanotube Sponge/Polyimide Nanocomposite

AbstractStress controllability in thermal and electrical conductivity is important for flexible piezoresistive devices. Due to the strength‐elasticity trade‐off, comprehensive investigation of stress‐controllable conduction in elastic high‐modulus polymers is challenging. Here presented is a 3D elastic graphene‐crosslinked carbon nanotube sponge/polyimide (Gw‐CNT/PI) nanocomposite. Graphene welding at the junction enables both phonon and electron transfer as well as avoids interfacial slippage during cyclic compression. The uniform Gw‐CNT/PI comprising a high‐modulus PI deposited on a porous templated network combines stress‐controllable thermal/electrical conductivity and cyclic elastic deformation. The uniform composites show different variation trends controlled by the porosity due to different phonon and electron conduction mechanisms. A relatively high k (3.24 W m−1 K−1, 1620% higher than PI) and suitable compressibility (16.5% under 1 MPa compression) enables the application of the composite in flexible elastic thermal interface conductors, which is further analyzed by finite element simulations. The interconnected network favors a high stress‐sensitive electrical conductivity (sensitivity, 973% at 9.6% strain). Thus, the Gw‐CNT/PI composite can be an important candidate material for piezoresistive sensors upon porosity optimization based on stress‐controllable thermal or electrical conductivity. The results provide insights toward controlling the stress‐induced thermal/electrical conductivities of 3D interconnected templated composite networks for piezoresistive conductors or sensors.