Preparation of polypropylene/ethylene‐propylene‐diene terpolymer/nitrile rubber ternary thermoplastics vulcanizates with good mechanical properties and oil resistance by core‐shell dynamic vulcanization

As the most successful commercialized thermoplastic vulcanizates (TPVs), polypropylene (PP)/ethylene propylene rubber (EPDM) TPVs exhibit poor oil resistance. In this work, we prepared PP/EPDM/butadiene acrylonitrile rubber (NBR) ternary TPVs with good oil resistance using core‐shell dynamic vulcanization. According to the theoretical analysis of the spreading coefficient and the transmission electron microscopy results, the rubber phases exhibited a special core‐shell structure, in which the cross‐linkedNBR‐core was encapsulated by the EPDM‐shell. The core‐shell structure effectively improved the interfacial compatibility between PP and NBR phase as the EPDM‐shell could avoid the direct contact of them, thus improving the mechanical properties of the TPVs. For example, the PP/EPDM/NBR (40/30/30) ternary TPV showed enhanced tensile strength of 12.57 MPa, compared with 10.71 MPa of PP/EPDM (40/60) TPV and 11.11 MPa of PP/NBR (40/60) TPV, respectively. Moreover, the oil resistance of the TPVs was also improved. Compared with PP/EPDM TPV, the change rates in mass, volume, tensile strength and elongation at break of PP/EPDM/NBR TPV after oil immersion decreased by 42.18%, 48.69%, 52.68% and 28.77%, respectively.     

Bio-based ethylene-co-vinyl acetate/poly (lactic acid) thermoplastic vulcanizates with enhanced mechanical strength and shape memory behavior

With the increasing attention to the shortage of petroleum resources and environmental pollution, it is more urgent to develop new type biomass-derived and bio-degradability polymer materials. In this study, a various of bio-based ethylene-co-vinyl acetate (EVA)/poly (lactic acid) (PLA) thermoplastic vulcanizates (TPVs) with enhanced mechanical strength and shape memory behavior were prepared. The Fourier transform infrared spectroscopy (FTIR), torque rheometer, swelling equilibrium experiments, and thermal gravimetric analysis (TGA) indicate that the EVA component is more aggressive to the active radicals than PLA component, and the improvement of gel content for EVA component is more than that of PLA component. The scanning electronic microscope (SEM) and transmission electron microscopy (TEM) show that the co-continuous structure of EVA/PLA/AD TPV could be well maintained when the TMPTA was introduced into the multicomponent system. Obviously, the results also exhibit that the improvement of mechanical strength and shape memory behavior for EVA/PLA/AD TPV could be attributed to the increased gel content, especially the gel content of EVA component, without changing the crystallization behavior of EVA/PLA/AD TPV.     

Raman investigation of thermoplastic vulcanizates based on hydrogenated natural rubber/polypropylene blends

Raman spectroscopy including mapping technique appears as a powerful technique for the characterization of polymer blends like thermoplastic elastomers (TPEs) and thermoplastic vulcanizates (TPVs). The Raman spectra of polymers blends such as natural rubber/polypropylene (NR/PP) and 65% hydrogenated natural rubber/polypropylene (65%HNR/PP) were identified and the phase distribution was determined. The study was driven for the same type of blends in TPEs state and TPVs state obtained after to 2 different processes, either peroxide cure or sulfur cure. The morphology of TPEs and TPVs obtained by Raman spectroscopy were compared and confirmed using scanning electronic microscopy.Raman mapping shows that the phase morphology of NR/PP, 65%HNR/PP, were characterized as continuous rubber phase morphology of the thermoplastic elastomers (TPEs) and a fine dispersion of cross-linked rubber phase in a continuous matrix of the thermoplastic vulcanizates (TPVs). Raman spectroscopy is demonstrated to be a reference to determine the content ratio of each component in the TPVs. Moreover, Raman mapping could be used to calculate the phase size of cross-linked rubber phase dispersed in the thermoplastic vulcanizates (TPVs).     

Preparation and flammability of EPDM/PP/Mg(OH)2 dynamic vulcanizates

Magnesium hydroxide (MH) flame retardant dynamic vulcanized ethylene‐propylene‐diene terpolymer (EPDM)/polypropylene (PP) thermoplastic vulcanizates (TPVs) were prepared by a twin‐screw extruder. Influences of MH on their morphology, mechanical properties, flammability, and crystallization behavior have been investigated. Static tensile measurements exhibited that TPVs have higher mechanical properties than un‐vulcanized EPDM/PP/MH blends (UVBs). Scanning electron microscopy (SEM) studies showed that the formation of the larger‐size “micro‐encapsulated structure” where the MH aggregates were covered with a cross‐linked rubber phase improved the interaction between MH and polymer matrix. Results of limiting oxygen index (LOI) and microscale combustion calorimetry (MCC) confirmed that TPVs had superior fire‐resistant properties to UVBs. SEM images showed that more uniform and compact charred layers were generated in TPVs. The differential scanning calorimetry (DSC) results indicated that the crystallization behavior of the flame retardant TPVs changed marginally with increase in MH content. Copyright © 2009 John Wiley & Sons, Ltd.     

Novel fluorosilicone thermoplastic vulcanizates prepared via core‐shell dynamic vulcanization: Effect of fluororubber/silicone rubber ratio on morphology,crystallization behavior,and mechanical properties

Recently, we have reported a novel core‐shell dynamic vulcanization method to prepare poly(vinylidene fluoride) (PVDF)/fluororubber (FKM)/silicone rubber (SR) thermoplastic vulcanizates (TPVs) with cross‐linked rubber core‐shell particles. However, the shell thickness on the properties has not been studied in detail. Herein, these PVDF‐based TPVs different FKM‐shell thickness were prepared by changing FKM/SR ratios. The effect of FKM‐shell/SR‐core ratio on morphology, crystallization, and mechanical properties of the ternary TPVs was studied. The results showed that the FKM shell had more positive effect on interfacial‐induced crystallization behavior than the SR core due to its better compatibility with PVDF. When the FKM/SR ratio was <1, FKM was not enough to encapsulate SR completely, which resulted in the formation of imperfect core‐shell structure. However, when the FKM/SR ratio was >1, perfect core‐shell structure was formed. Therefore, the mechanical properties improved with increasing FKM content; especially, a remarkable improvement was observed when FKM/SR ratio was >1. This study could provide more information for the design of TPVs with core‐shell structure.     

Biobased PLA/NR-PMMA TPV with balanced stiffness-toughness: In-situ interfacial compatibilization,performance and toughening model

Using rubber to toughen polylactide (PLA) is always accompanied by the sharp reduction in stiffness. Herein, PLA/poly (methyl methacrylate) grafted natural rubber (NR-PMMA) thermoplastic vulcanizates (TPVs) with balanced stiffness-toughness were fabricated. With the addition of 40 wt % NR-PMMA, the impact strength and tensile toughness of PLA/NR-PMMA TPV significantly improved to about 102.7 kJ/m² and 66.1 MJ/m³, respectively, compared with those of 2.7 kJ/m² and 2.4 MJ/m³ for the pure PLA. Meanwhile, the yielding stress was maintained at 34.5 MPa. Fourier transform infrared spectroscopy (FTIR) confirmed the formation of in-situ interfacial compatibilization between PLA and rubber phases. Both tensile and impact toughening mechanism were studied and deduced as considerable energy dissipation provided by the continuous rubber phase. Instrumented notched impact tests demonstrated that the energy dissipating in crack propagation process contributed to the main part of impact toughness. In addition, a novel toughening model based on bicontinuous structure was incorporated, which showed good applicability in predicting the impact strength of PLA/NR-PMMA TPVs.     

Reinforcement of compatibilized NR/NBR blends by fly ash particles and precipitated silica

Effects of precipitated silica (PSi) and silica from fly ash (FA) particles (FASi) on the cure and mechanical properties before and after thermal and oil aging of natural rubber (NR) and acrylonitrile–butadiene rubber (NBR) blends with and without chloroprene rubber (CR) or epoxidized NR (ENR) as a compatibilizer have been reported in this paper. The experimental results suggested that the scorch and cure times decreased with the addition of silica and the compound viscosity increased on increasing the silica content. The mechanical properties for PSi filled NR/NBR vulcanizates were greater than those for FASi filled NR/NBR vulcanizates in all cases. The PSi could be used for reinforcing the NR/NBR vulcanizates while the silica from FA was regarded as a semi‐reinforcing and/or extending filler. The incorporation of CR or ENR enhanced the mechanical properties of the NR/NBR vulcanizates, the ENR being more effective and compatible with the blend. The mechanical properties of the NR/NBR vulcanizates were improved by post‐curing effect from thermal aging but deteriorated by the oil aging. Copyright © 2008 John Wiley & Sons, Ltd.     

Design of PP/EPDM/NBR TPVs with tunable mechanical properties via regulating the core-shell structure

In this work, polypropylene (PP)/ethylene-propylene-diene monomer (EPDM)/butadiene acrylonitrile rubber (NBR) TPVs with different EPDM/NBR ratios were prepared by the core-shell dynamic vulcanization. The relationship between the core-shell structure and mechanical properties of the TPVs were thoroughly investigated. The formation of core-shell structure by adding NBR is conducive to the mechanical properties of the TPVs. The ratio of EPDM to NBR has an important effect on the structure and performances of the final products, and there is a critical ratio for this effect change. Transmission electron microscope (TEM), tensile test, reprocessing test, ageing test, rheological behavior test and stress relaxation were used to characterize the morphology and properties of the TPVs in detail. It was found that when the ratio of EPDM/NBR was 2:4, the tensile strength increased by ~14% compared with PP/EPDM TPV without NBR. Meanwhile, the reprocessing properties, rheological characteristics and instantaneous tensile deformation, etc. all exhibited sudden changes at this critical ratio.     

One-step process to make electrically conductive thermoplastic vulcanizates filled with MWCNTs

Electrically conductive thermoplastic vulcanizates(TPVs) filled by multi-walled carbon nanotubes(MWCNTs) are prepared by a simple one-step melt mixing process,based on linear low density polyethylene(LLDPE) and ultrafme full-vulcanized rubber particles(UFRP).An ideal morphology with controlled localization of MWCNTs in continuous LLDPE matrix and appropriate size of finely-dispersed UFRP can be achieved at the same time.The controlled localization of MWCNTs in the continuous phase facilitates the formation of conductive pathway,and thus the volume resistivity of the as-prepared LLDPE/UFRP/MWCNTs thermoplastic vulcanizates is significantly decreased.The results show that both the blend ratio of LLDPE/UFRP and the loading of MWCNTs have remarkable effect on the volume resistivity.Significantly, the electrically conductive TPVs exhibit good mechanical properties duo to the fine dispersion of UFRP in LLDPE.The added MWCNTs are capable of imparting reinforcement effects to thermoplastic vulcanizates with just a slight loss of stretchability and elasticity.     

Electrospun hyperbranched polylactic acid–modified cellulose nanocrystals/polylactic acid for shape memory membranes with high mechanical properties

The polylactic acid (PLA) nanofiber membranes reinforced with hyperbranched PLA‐modified cellulose nanocrystals (H‐PLA‐CNCs) were prepared by electrospinning. The H‐PLA‐CNCs and the nanofiber membranes were researched by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), thermal gravimetric analysis (TGA), differential scanning calorimetry (DSC), and dynamic mechanical analysis (DMA). The outcomes embodied that the cellulose nanocrystals (CNCs) could be successfully improved by the hyperbranched PLA, which would offer powerful CNCs/matrix interfacial adhesion. Thus, the mechanical and shape memory properties of PLA can be improved by adding the H‐PLA‐CNCs. In particular, when the addition of H‐PLA‐CNCs was 7 wt%, the tensile strength and an ultimate strain of PLA composite nanofiber membranes was 15.56 MPa and 25%, which was 228% and 72.4% higher than that of neat PLA, respectively. In addition, the shape recovery rate of the PLA/5 wt% H‐PLA‐CNCs composite nanofiber membrane was 93%, which was 37% higher than that of neat PLA. We expected that this present study would provide unremitting efforts for the development of more effective approaches to prepare biology basic shape memory membranes with high mechanical properties.     

Synthesis and properties of shape memory polymers of LLA,TMC, and ε‐CL terpolymers

Biodegradable polylactide (PLA) and its copolymers with shape memory properties have attracted great interests because of their important application prospects in biomedical field. In this study, random poly(L‐lactide‐co‐trimethylene carbonate‐co‐ε‐caprolactone) (LTCL) terpolymers with different molar ratio were synthesized and characterized. Monomer ε‐caprolactone (ε‐CL) was used in this study instead of glycolide in preliminary study of LTG terpolymers to investigate the transition temperature and the shape memory performance. Characterization on crystallization, mechanical properties, shape fixing, and recovery ratios of the terpolymers was conducted to investigate the correlation between crystallization and shape memory performance of LTCL terpolymers. The results are consistent with the formation of crystallized LLA segments, which could act as crosslinks, strengthened the stationary phase within the polymer matrix, and significantly improved the shape memory performance of LTCL terpolymers. For example, LTCL801010 is a crystalline polymer with high shape fixity and shape recovery ratio; its shape recovery temperature is 39°C. LTCL terpolymers with high CL content do not show shape memory performance for the rubbery at room temperature. Based on this study, PLA materials with shape memory property can be designed through the selection of monomers or the adjustment of comonomer ratio. These polymers with recovery temperature close to 37°C are expected to be used in human body such as scaffolds in tissue engineering.     

界面粘结对聚氯乙烯/丁腈橡胶共混物脆韧转变的影响

应用丙烯腈（ＡＮ）含量不同的丁腈橡胶（ＮＢＲ）与聚氯乙烯（ＰＶＣ）共混，研究了界面粘结对ＰＶＣ／ＮＢＲ共混物脆韧转变的影响．结果表明：当基体层度Ｔ相等时，过强的界面粘结，使ＰＶＣ／ＮＢＲ共混物的冲击强度降低，并且其产生脆韧转变的临界基体层厚度Ｔｃ减小．界面粘结对于聚合物共混物的增韧行为具有直接的影响．损伤区分析给出：随着界面粘结强度增大，空洞化过程受阻，减弱能量的耗散，并且不利于诱导剪切屈服损伤的产生，因而不利于增韧；但是界面粘强度过小，意味着共混物的相容性太差，致使分散相粒径过大，也不利于增韧．所以对增韧来讲，共混物的界面粘结强度存在一个最佳范围．     

Structure evolution of bio-based PLA/ENR thermoplastic vulcanizates during dynamic vulcanization processing

The thermoplastic vulcanizates (TPVs) of Polylactide (PLA)/Epoxidized natural rubber (ENR) were prepared by dynamic vulcanization technology. The processing torque, crosslink density, morphology of PLA/ENR blends, and PLA's molecular weight during the processing were investigated by HAAKE rheometer, swelling measurement, scanning electron microscopy (SEM), and gel permeation chromatography (GPC). It was found that the vulcanization of ENR completed at the turning point after torque peak. After the turning point, the torque and crosslink density decreased with the processing time increasing. Moreover, the morphology of PLA/ENR blends showed bi-continuous structure during the dynamic vulcanization processing, and the phase size of PLA/ENR was increased with processing time and temperature. GPC results showed PLA degradation mainly happened after torque turning point. Thermal gravimetric analysis (TGA) results indicated that some parts of PLA would graft on ENR during processing, and the higher the processing temperature, the more the PLA was grafted.     

Thermo‐responsive shape memory behavior of poly(styrene‐b‐isoprene‐b‐styrene)/ethylene‐1‐octene copolymer thermoplastic elastomer blends

Thermally‐triggered shape memory polymers (SMPs) are smart materials, which are capable of changing their shapes when they are exposed a heat stimulant. Blending semi‐crystalline and elastomeric polymers is an easy and low‐cost way to obtain thermo‐responsive SMPs. In this work, novel poly(ethylene‐co‐1‐octene) (PEO) and poly(styrene‐b‐isoprene‐b‐styrene) (SIS) thermoplastic elastomer blends were prepared via melt blending method. The morphological, mechanical, rheological properties and shape memory behaviours of the blends were investigated in detail. In morphological analysis, co‐continuous morphology was found for 50 wt% PEO/50 wt% SIS and 60 wt% PEO/40 wt% SIS (60PEO/40SIS) blends. The shape memory analysis performing by dynamic mechanical analyzer showed that the 60PEO/40SIS blend also exhibited the optimum shape memory performance with 95.74% shape fixing and 98.98% shape recovery. Qualitatively shape memory analysis in hot‐water pointed out that the amount of semi‐crystalline PEO promotes shape fixing ability of the blends whereas SIS content enhances shape recovery capability. Although the SIS and PEO are immiscible polymers, the blends of them were exhibited good elastomeric properties with regard to tensile strength, toughness, and elongation at break.     

Direct visualization of the nanoscopic three‐phase structure and stiffness of NBR/PVC blends by AFM nanomechanical mapping

The PeakForce Quantitative Nanomechanical Mapping based on atomic force microscope (AFM) is employed to first visualize and then quantify the elastic properties of a model nitrile rubber/poly(vinyl chloride) (NBR/PVC) blend at the nanoscale. This method allows us to consistently observe the changes in mechanical properties of each phase in polymer blends. Beyond measuring and discriminating elastic modulus and adhesion forces of each phase, we tune the AFM tips and the peak force parameters in order to reliably image samples. In view of viscoelastic difference in each phase, a three‐phase coexistence of an unmixed NBR phase, the mixed phase, and PVC microcrystallites is directly visualized in NBR/PVC blends. The nanomechanical investigation is also capable of recognizing the crosslinked rubber phase in cured rubber. The contribution of the mixed phase was quantified and it was found that the mechanical properties of blends are mainly determined by the homogeneity and stiffness of the mixed phase. This study furthers our understanding the structure–mechanical property relationship of thermoplastic elastomers, which is important for their potential design and applications. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 662–669     

Preparation of Polylactide/Poly(ether)urethane Blends with Excellent Electro-actuated Shape Memory via Incorporating Carbon Black and Carbon Nanotubes Hybrids Fillers

In this work, hybrid conductive fillers of carbon black(CB) and carbon nanotubes(CNTs) were introduced into polylactide(PLA)/thermoplastic poly(ether)urethane(TPU) blend(70/30 by weight) to tune the phase morphology and realize rapid electrically actuated shape memory effect(SME). Particularly, the dispersion of conductive fillers, the phase morphology, the electrical conductivities and the shape memory properties of the composites containing CB or CB/CNTs were comparatively investigated. The results suggested that both CB and CNTs were selectively localized in TPU phase, and induced the morphological change from the sea-island structure to the co-continuous structure. The presence of CNTs resulted in a denser CB/CNTs network, which enhanced the continuity of TPU phase.Because the formed continuous TPU phase provided stronger recovery driving force, the PLA/TPU/CB/CNTs composites showed better shape recovery properties compared with the PLA/TPU/CB composites at the same CB content. Moreover, the CB and CNTs exerted a synergistic effect on enhancing the electrical conductivities of the composites. As a result, the prepared composites exhibited excellent electrically actuated SME and the shape recovery speed was also greatly enhanced. This work demonstrated a promising strategy to achieve rapid electrically actuated SME via the addition of hybrid nanoparticles with self-networking ability in binary PLA/TPU blends over a much larger composition range.     

Biodegradable compositions by reactive processing of aliphatic polyester/polysaccharide blends

Commercially available biodegradable aliphatic polyesters, i.e., high molecular weight poly(ϵ-caprolactone) (PCL) and polylactide (PLA), were melt blended with a well-known natural and biodegradable polysaccharide: starch either as corn starch granules or as thermoplastic corn starch after plasticization with glycerol. Conventional melt blending yielded compositions with poor mechanical performances as a result of lack of interfacial adhesion between the rather hydrophobic polyester matrix and the highly hydrophilic and moisture sensitive starch phase. Interface compatibilization was achieved via two different strategies depending on the nature of the polyester chains. In case of PLA/starch compositions, PLA chains were grafted with maleic anhydride through a free radical reaction conducted by reactive extrusion. The maleic anhydride-grafted PLA chains (MAG-PLA) allowed for reinforcing the interfacial adhesion with granular starch as attested by TEM of cryofracture surface. As far as PCL/starch blends were concerned, the compatibilization was achieved via the interfacial localization of amphiphilic graft copolymers formed by grafting of PCL chains onto a polysaccharide backbone such as dextran. The PCL-grafted polysaccharide copolymers were synthesized by controlled ring-opening polymerization of ϵ-caprolactone proceeding via a coordination-insertion mechanism. These compatibilized PCL/starch compositions displayed much improved mechanical properties as determined by tensile testing as well as a much more rapid biodegradation as measured by composting testing.     

Rheological,mechanical and morphological properties of thermoplastic vulcanizates based on NR‐g‐PMMA/PMMA blends

Graft copolymer of natural rubber and poly(methyl methacrylate) (NR‐g‐PMMA) was prepared using semi‐batch emulsion polymerization technique via bipolar redox initiation system. It was found that the grafted PMMA increased with the increase of methyl methacrylate (MMA) concentration used in the graft copolymerization. The NR‐g‐PMMA was later used to prepare thermoplastic vulcanizates (TPVs) by blending with PMMA through dynamic vulcanization technique. Conventional vulcanization (CV) and efficient sulphur vulcanization (EV) systems were studied. It was found that the CV system provided polymer melt with lower shear stress and viscosity at a given shear rate. This causes ease of processability of the TPVs via extrusion and injection molding processes. Furthermore, the TPVs with the CV system showed higher ultimate tensile strength and elongation. The results correspond to the morphological properties of the TPVs. That is, finer dispersion of the small vulcanized rubber particles were observed in the PMMA matrix. Various blend ratios of the NR‐g‐PMMA/PMMA blends using various types of NR‐g‐PMMA (i.e. prepared using various percentage molar ratios of NR and MMA) were later studied via dynamic vulcanization by a conventional sulphur vulcanization system. It was found that increasing the level of PMMA caused increasing trend of the tensile strength and hardness properties but decreasing level of elongation properties. Increasing level of the grafted PMMA in NR molecules showed the same trend of mechanical properties as in the case of increasing concentration of PMMA used as a blend component. From morphological studies, two phase morphologies were observed with a continuous PMMA phase and dispersed elastomeric phase. It was also found that more finely dispersed elastomeric phase was obtained with increasing the grafted PMMA in the NR molecules. Copyright © 2005 John Wiley & Sons, Ltd.     

Prediction models for the key mechanical properties of EPDM/PP blends as affected by processing parameters and their correlation with stress relaxation and phase morphologies

The optimum condition of processing parameters (mixing temperature, rotor speed, fill factor, and blend ratio) and prediction models for the best key mechanical properties of ethylene propylene diene terpolymer/polypropylene thermoplastic vulcanizates (EPDM/PP TPVs) was investigated by using the Taguchi's optimization technique and data analysis. The results reveal that all of the processing parameters affected significantly the mechanical properties of the EPDM/PP TPVs, but specifically the blend ratio contributed more than 90% in effect size on tensile strength and tension set. There were three main factors, the mixing temperature, the fill factor, and the blend ratio, influencing the elongation at break. Furthermore, the mathematic models were effective and reliable in predicting the properties of TPVs. The correlation of mechanical properties, stress relaxation, and phase morphologies of the TPVs prepared from the predicted models was also investigated. It can be summarized that the morphological structure and stress relaxation of the TPVs were strongly governed by the EPDM content in the blend ratio. That is, the higher the EPDM content, the better phase morphology having smaller size of the vulcanized EPDM particles distributed in the PP matrix and the higher rate of stress relaxation. Moreover, these two properties were then principally pushing the mechanical characteristics of the EPDM/PP TPVs. Copyright © 2015 John Wiley & Sons, Ltd.     

Preparation of Polylactide/Poly(ether)urethane Blends with Excellent Electro-actuated Shape Memory <Emphasis Type="Italic">via</Emphasis> Incorporating Carbon Black and Carbon Nanotubes Hybrids Fillers

In this work, hybrid conductive fillers of carbon black (CB) and carbon nanotubes (CNTs) were introduced into polylactide (PLA)/thermoplastic poly(ether)urethane (TPU) blend (70/30 by weight) to tune the phase morphology and realize rapid electrically actuated shape memory effect (SME). Particularly, the dispersion of conductive fillers, the phase morphology, the electrical conductivities and the shape memory properties of the composites containing CB or CB/CNTs were comparatively investigated. The results suggested that both CB and CNTs were selectively localized in TPU phase, and induced the morphological change from the sea-island structure to the co-continuous structure. The presence of CNTs resulted in a denser CB/CNTs network, which enhanced the continuity of TPU phase. Because the formed continuous TPU phase provided stronger recovery driving force, the PLA/TPU/CB/CNTs composites showed better shape recovery properties compared with the PLA/TPU/CB composites at the same CB content. Moreover, the CB and CNTs exerted a synergistic effect on enhancing the electrical conductivities of the composites. As a result, the prepared composites exhibited excellent electrically actuated SME and the shape recovery speed was also greatly enhanced. This work demonstrated a promising strategy to achieve rapid electrically actuated SME via the addition of hybrid nanoparticles with self-networking ability in binary PLA/TPU blends over a much larger composition range.