- Abstract：Heat-, light-, and humidity-responsive materials were fabricated via chemical design and cold drawing processing. The crystallizable polyether/polyester diols were first reacted with isophorone diisocyanate (IPDI), followed by chain extension with azobenzene units. The synthesized polyurethanes exhibited ductile behavior and drawing-induced orientation when the soft segments possessed high crystallinity. Upon heating or UV irradiation, the oriented polyurethane strips underwent bending, whereas the pristine strips did not. Under humid conditions, both oriented and pristine polyurethane strips containing poly(ethylene oxide) (PEO) soft segments bent, albeit in opposite directions. In contrast, polyurethane strips with polycaprolactone (PCL) and polytetramethylene ether glycol (PTMEG) soft segments showed no response to humidity, regardless of whether they were stretched. Mechanistic investigations revealed that the temperature increase resulting from the photothermal effect of the azobenzene moieties is the main reason for light-induced actuation, which differs from that in many other azobenzene-based materials. The entropic elastic energy stored during stretching is released upon UV irradiation, heating, or humidification to drive the bending deformation. This work presents a strategy for constructing multi-stimuli- responsive materials via molecular design and post-processing, highlighting the synergy between functional moieties and microscopic structures, which holds great significance for the development of advanced intelligent materials.Keywords：Polymer crystallization;Polyurethanes;Humidity sensitivity;Photothermal effect;Stimuli-responsive materials2|0|0
Updated：2026-07-22 - Abstract：Fully π-conjugated polymers are promising for flexible optoelectronics; however, their inherent brittleness poses a challenge for achieving high-performance flexible electronic devices. In this study, we developed a carbazole-based semiconductor fluid plasticizer, TODPFCZ, to simultaneously enhance the stretchability and optoelectronic properties of poly(9,9-di-n-octylfluorene-alt-benzothiadiazole) (F8BT) films using an external plasticizing strategy. The fluid TODPFCZ molecules incorporated into the F8BT matrix disrupted interchain π-π stacking and crystallinity, which significantly enhanced the stretchability, increasing the fracture strain from 18% to 44% and the crack-onset strain from 5% to 35%. Owing to the efficient energy transfer from TODPFCZ to F8BT, polymer light-emitting diodes (PLEDs) based on the optimized blend films showed stable electroluminescence and maintained efficiency even after being pre-strained up to 15%, revealing outstanding stress tolerance. The blended films also exhibited excellent recoverability and thermoplasticity. This study demonstrates that carbazole-based semiconductor fluid plasticizers provide a versatile and effective pathway for designing high-performance, intrinsically stretchable, fully π-conjugated polymers for durable flexible electronics.Keywords：Intrinsically stretchable semiconductors;Conjugated polymer films;Semiconductor fluid plasticizer;Mechanical-optoelectronic synergy;Flexible polymer light-emitting diodes (PLEDs)2|0|0Updated：2026-07-22
- Abstract：Traditional acrylate reactive diluents, which are derived from fossil resources, are known to exhibit significant irritation and allergenic potential, leading to their prohibition in high-end electronics, particularly in wearable devices. To address these limitations, four bio-based acrylate reactive diluents (BRDs) were synthesized via the reaction of alcohols derived from renewable sources, piperitol, vanillin, eugenol, and isosorbide, with methacrylic anhydride. The viscosity of the synthesized BRDs and the Tg of their corresponding polymers were systematically evaluated and compared with those of the petroleum-based diluent isobornyl acrylate (IBOA). The BRDs were then blended with acrylate-terminated polyurethane (APU) to formulate a series of UV-curable polyurethane adhesives (APU-BRDs). The results suggest that BRDs effectively reduce the viscosity of APU. By selecting and combining BRDs, the bonding strength of APU-BRDs to polar substrates such as PC and glass can reach 20 MPa. Even for non-polar substrates like PE, the strength is close to 5 MPa. The values obtained in this study exceed those of adhesives prepared using the conventional petroleum-based diluent IBOA. Furthermore, the study explored the potential application of APU-BRDs in smart wearable devices, confirming their suitability for next-generation wearable technology.Keywords：Bio-based acrylate;Reactive diluents;Polyurethane;UV-curable adhesives;Electronic watch packaging2|0|0Updated：2026-07-22
- Abstract：Acrylonitrile butadiene styrene (ABS) is widely used owing to its excellent mechanical properties, thermal stability, and processability; however, its poor inherent flame retardancy limits its applications, which require higher safety. Conventional flame-retardant ABS systems mainly rely on a bromine-antimony synergistic system, in which antimony trioxide (ATO) is costly and environmentally concerning. In this study, decabromodiphenylethane (DBDPE) and ATO were first selected as the flame-retardant systems and combined at a mass ratio of 3:1. The results showed that the ABS/12DBDPE/4ATO composite achieved a UL-94 V-0 rating with a limiting oxygen index (LOI) of 24.0%. Subsequently, zinc ferrite (ZF) nanoparticles were synthesized via a co-precipitation method and employed as partial substitutes for ATO in ABS composites. When 50 wt% ATO was replaced by ZF, the ABS/12DBDPE/2ATO/2ZF composite exhibited an increased LOI value of 26.9%, while still achieving a UL-94 V-0 rating. Compared with neat ABS, the peak heat release rate (PHRR) and total heat release (THR) were reduced by 62.1% and 46.3%, respectively. Furthermore, incorporating 5 wt% nitrile butadiene rubber (NBR) significantly improved the toughness of the composite, increasing the impact strength from 3.8 kJ/m2 to 13.2 kJ/m2, without compromising flame retardancy. Overall, this study demonstrates an effective and practical strategy to reduce ATO usage while simultaneously enhancing the fire safety and mechanical performance of ABS.Keywords：Acrylonitrile butadiene styrene (ABS);Flame retardancy;Zinc ferrite;Antimony trioxide;Substitution2|0|0Updated：2026-07-22
- Abstract：In polymer processing, low-molecular-weight chemically identical oligomers are typically added to a polymer to improve its processability and mechanical properties by manipulating its entanglement concentration. However, the complicated semi-crystalline morphologies and melt memory effect of less entangled bimodal dispersed mixtures cannot be overlooked. In this study, we systematically examined the crystallization and self-nucleation behavior of poly(ε-caprolactone) (PCL) mixtures composed of a relatively high-molecular-weight (83 kg/mol) fraction and a low-molecular-weight PCL with a mid-chain defect (2 kg/mol). The entanglement concentrations were quantified by linear rheological measurements. Both thermal analysis and small-angle X-ray scattering (SAXS) investigations revealed that pronounced crystallization-induced phase separation (i.e., molecular segregation) occurs because of the different nucleation energy barriers. In contrast to our previous investigation using a long chain fraction with a higher molecular weight (200 kg/mol) (Macromolecules 2024, 57, 1632−1641), the low-molecular-weight oligomer tends to crystallize between adjacent crystalline lamellae composed of long PCL chains due to the lack of intra-crystalline links, for example, entanglements and tie-molecules. The correlation between the melt memory effect and the entanglement concentration was evaluated using self-nucleation experiments. The 2 kg/mol PCL oligomer (with a central defect) did not exhibit melt memory. However, the introduction of high-molecular-weight components, even below the critical entanglement concentration, leads to a wider temperature range, preserving the ordered structure. Our results provide solid evidence that the melt memory effect in polar semi-crystalline polymers originates from the intramolecular interactions of adjacent chain folding rather than entanglements or chain overlaps.Keywords：Molecular segregation;Small-angle X-ray scattering (SAXS);Melt memory3|0|0Updated：2026-07-22
- Abstract：Two pyrimidoisoindigo-based polymers were synthesized by copolymerizing thiophene-flanked pyrimidoisoindigo (T-PymII) with thiophene (T) or 3,4-difluorothiophene (2FT), and their structure–property correlations were investigated. Although both polymers exhibited ambipolar transport properties, P(PymII-TTT) was dominated by hole transport, while P(PymII-T-2FT-T) was dominated by electron transport. Among them, the highest hole mobility up to 1.66×10−2 cm2·V−1·s−1 was observed for P(PymII-TTT), while the highest electron mobility of 6.37×10−3 cm2·V−1·s−1 was observed for P(PymII-T-2FT-T). AFM and GIWAXS analyses revealed that their poor morphology and crystallinity may account for their inferior performance. Therefore, further side-chain engineering is needed to improve the crystallinity of PymII-based polymers.Keywords：Pyrimidoisoindigo;Organic field-effect transistor;Ambipolar charge transport17|6|0Updated：2026-07-20
- Abstract：As plastic pollution has become increasingly severe, the development of recyclable and rapidly degradable polyesters has significant practical value and significance. In this study, seven-membered cyclic 1,3-propylene glycol oxalate (POx) was successfully synthesized through a two-step polycondensation-depolymerization method using dimethyl oxalate (a low-cost and readily accessible bulk chemical) and bio-based 1,3-propylene glycol as the starting materials. Using Sn(Oct)2 as the catalyst, high-molecular-weight poly(1,3-propylene oxalate) (PPOx) was efficiently prepared via ring-opening polymerization (ROP) of POx. This ROP demonstrated excellent reactivity, attaining a monomer conversion up to 95% within 10 min, and PPOx had a maximum intrinsic viscosity (η) of 1.06 dL/g. Furthermore, the prepared PPOx could be catalytically depolymerized to enable efficient recovery of the POx monomer, with a yield of 60% and a purity of 98%. The degradation performance tests indicated that PPOx exhibited rapid degradation, reaching a degradation rate of up to 99% within 50 days. Owing to the innovative selection of raw materials and the design of a closed-loop process, this study provides a new economical and sustainable strategy for reducing dependence on petroleum resources, offering valuable insights into the development of recyclable and rapidly degradable polyesters.Keywords：Polyester;Oxalate;Ring-opening polymerization;Closed-loop recycling;Rapid degradation13|3|0Updated：2026-07-20
- Abstract：Incorporating different structural units into the polyester backbone constitutes a powerful strategy to tailor material performances. The integration of ether and ester moieties affords poly(ether-alt-ester)s with enhanced mechanical flexibility and tunable thermal properties. Nevertheless, the substrate scope available for the alternating copolymerization of epoxides with lactones remains considerably restricted, and the resulting polymers still suffer from inferior thermal resistance. Herein, we design a typical Bringmann’s lactone bearing a conformationally constrained biaryl axis and a helically distorted six-membered bridging scaffold. A binary catalyst system composed of simple Salen-Cr(III)-Cl and 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene (MTBD) enables strictly alternating and controlled copolymerization with meso-epoxides, effectively suppressing the formation of ether-ether or ester-ester linked homopolymer sequences. This protocol yields alternating poly(ether-alt-ester)s with a high glass transition temperature of 114 °C, an enhancement of 57 °C relative to alternating copolymer derived from the flexible 3,4-dihydrocoumarin monomer. This approach provides a facile and practical strategy for advancing the performance of alternating poly(ether-alt-ester)s.Keywords：Poly(ether-alt-ester)s;Alternating copolymerization;Biaryl lactone;Glass transition temperature10|1|0Updated：2026-07-20
- Abstract：Recently circularly polarized luminescence (CPL) generated by chiral materials have attracted tremendous attention due to its potential applications such as 3D displays, quantum communication, and information storage. Polymers have emerged as particularly promising platforms for generating and amplifying CPL, owing to their structural designability, inherent helical architectures, and excellent processability. Hence, this review provides a comprehensive overview of recent advances in polymer-based CPL materials, with a central focus on the rational construction of polymer chiral superstructures, including helical polymers bearing chiral centers on side chains for chiral transfer and amplification, helical polymers with chiral centers integrated into the main chain, achiral polymers complexed with small-molecule inducers through non-covalent interactions; and achiral polymers utilizing macromolecular inducers. By discussing representative examples, we elucidate the underlying mechanisms of chirality transfer, amplification, and luminescence that govern CPL. The review concludes by highlighting the key challenges and promising future perspectives in this field, aiming to guide further research and accelerate the practical application of polymer-based CPL materials.Keywords：Circularly polarized luminescence;Helical polymer;Achiral polymer;Chiral induction;Chiral amplification10|3|0Updated：2026-07-20
- Abstract：Information leakage and forgery continue to threaten the security of the information storage and transmission. However, most existing physical encryption materials rely on single and predictable stimulus-response mechanisms, resulting in limited security, programmability, and service life. Herein, a high-security sequential 4D encryption system is developed based on a dynamic covalent polyurethane network that integrates shape memory, self-healing, and photochromism in one system. Arylboronic acid was incorporated into the polyurethane framework to form a dynamic boron carbamate network. The resulting boroxine crosslinks act as reversible junctions, enabling thermally triggered shape memory behavior, while simultaneously providing efficient self-healing through reversible hydrolysis and reformation. The optimized polyurethane exhibited a tensile strength of about 35 MPa, a shape-fixity ratio of >99%, and a shape-recovery ratio of up to 83% while achieving a self-healing efficiency of about 81% after thermal treatment. In parallel, the incorporation of a photochromic dye enables precise time-dependent color evolution under ultraviolet irradiation. The synergistic coupling of thermal and photonic responses allows sequential and time-gated information decoding, significantly increasing the encryption complexity and resistance to unauthorized access. The resulting films function as dynamic 4D encryption carriers from which correct information can be retrieved only through a predefined sequence of shape recovery and color transformation. This study provides a versatile strategy for next-generation physical encryption materials with intrinsic damage tolerance, long-term reliability, and storage potential in optical data storage and advanced anti-counterfeiting applications.Keywords：Information encryption;Multistimuli response;Dynamic bond;Polyurethane6|0|0Updated：2026-07-20
- Abstract：The interfacial structure at the electrode-electrolyte interface is a critical determinant of the performance of electrochemical supercapacitors. Although grafting polyelectrolyte (PE) brushes onto electrodes is a promising strategy to enhance charge storage, the role of dielectric contrast and its coupling with PE microstructure remains to be studied. In this work, a classical density functional theory (cDFT) is employed to elucidate the synergistic effects of dielectric contrast and PE microstructure on supercapacitor performance. The theory explicitly accounts for image-charge interaction induced by dielectric discontinuity, chain correlation of the PE, excluded volume effect, and electrostatic correlation. The results reveal that increasing the grafting density and chain length of the PE brushes significantly enhances the capacitance by providing more immobile charge sites and expanding the effective double-layer region, which facilitates stronger counterion adsorption. It is found that the dielectric contrast between the electrode substrate and solvent, which is often oversimplified in idealized models, plays a decisive role. A higher dielectric permittivity of the substrate weakens the shielding effect of the polarization field within the electrode. Consequently, the external electric field provides a stronger influence on the electrolyte, promoting a denser accumulation of counterions at the interface. Crucially, a high-dielectric substrate mitigates the repulsive image-charge interaction, effectively transforming it into an attractive force that further adsorbs charge near the electrode. This effect becomes particularly pronounced at high surface potentials. These results provide fundamental insights into the optimization of high-performance SCs using PE coatings.Keywords：Classical density functional theory;Polyelectrolyte brushes;Dielectric contrast;Image-charge interaction;Supercapacitors6|2|0Updated：2026-07-20
- Abstract：Upgrading commercially available polyethylene to have both higher mechanical properties and surface hydrophilicity is of fundamental interest and practical importance, but the actual results usually suffer from a trade-off between mechanical performance and surface hydrophilicity. Herein, we report the preparation of eighteen high-density polyethylene (HDPE) blend materials via the simple physical blending with hydrophilic ethylene/meta-methoxystyrene (E-mMOS) copolymers (P1, P2, and P3) used as macromolecular additives. After adding low blend ratios of the E-mMOS copolymers (2 wt%, 5 wt% and 10 wt%), the tensile strength, toughness and hydrophilicity of the resultant HDPE blends simultaneously increased. HDPE(SABIC)/P3 blend showed the optimal comprehensive improvement in tensile strength (41.2 MPa versus 31.1 MPa), elongation at break (1601% versus1083%), and hydrophilicity (water contact angle, 96.2° versus 106.4°) compared with commercial HDPE. SEM tests exhibited the HDPE/E-mMOS blends had good compatibilities. These HDPE materials also exhibited good processability, as evidenced by DSC and rheological measurements.Keywords：Polyethylene;Melt blending;Hydrophilic;Compatibility;Upgrading7|1|0Updated：2026-07-20
- Abstract：The co-nonsolvency of polymers in binary mixtures of individually good solvents remains mechanistically controversial, despite extensive research over several decades. Recent theoretical analyses based on ternary solution thermodynamics suggest that the orientation of tie lines in the polymer solvent composition plane serves as a decisive signature to distinguish between preferential interaction-driven and solvent cosolvent attraction-driven mechanisms, yet direct experimental verification of this prediction has remained elusive. Here, we report the quantitative experimental determination of tie line orientations in a poly(N-isopropylacrylamide) water-methanol system through direct measurement of solvent partitioning between coexisting liquid phases. Our experimental results reveal that all measured tie lines consistently exhibit positive slopes in the polymer concentration and methanol fraction composition planes, unambiguously indicating preferential enrichment of the better solvent in the polymer-rich phase. This observation provides direct experimental evidence supporting the preferential interaction-driven mechanism and establishes tie line orientation as a robust practical experimental observable for elucidating co-nonsolvency phenomena. These findings validate theoretical predictions within the Flory-Huggins framework and bridge the gap between the mean field theory and experimental reality, offering a definitive methodology that should broadly applicable to other polymer systems exhibiting similar phase separation behavior.Keywords：Co-nonsolvency;Phase separation;Preferential solvation;Tie-line analysis5|0|0Updated：2026-07-20
- Abstract：Bone defects remain a major clinical challenge due to the slow rate of recovery, complex surgical procedures, and great impact on the lives of patients. Therefore, the development of biocompatible, durable, degradable artificial bone grafts is highly desirable. Inspired by the natural composition of human bone, this study reports the fabrication of poly(lactic acid) (PLA)/zinc-doped hydroxyapatite (Zn-HA) composite materials via the melt blending method. The chemical properties, mechanical performance, degradability, and biocompatibility of the composites were evaluated systematically. Among them, the 10 wt% PLA/Zn-HA composite exhibited optimal performance, including high tensile and flexural strengths, superior thermal stability, and the lowest degradation rate. Controlled degradation and sustained release of zinc ions further enhance osteoblast activity with low cytotoxicity. Furthermore, Alkaline Phosphatase (ALP) activity and Alizarin Red S (ARS) staining confirmed that the 10 wt% PLA/Zn-HA composite significantly promoted osteogenic differentiation. By simultaneously achieving mechanical reliability and enhanced biological properties, this study provides promising design criteria for next-generation artificial bone grafts for bone defect repair.Keywords：Bone repair;Poly(lactic acid);Zinc-doped hydroxyapatite;Composite materials8|2|0Updated：2026-07-20
- Abstract：Liquid crystal elastomers (LCEs) are compelling smart materials for soft robotics and flexible electronics. However, both conventional and dynamically crosslinked LCE systems fundamentally rely on chemically crosslinked networks, which has long been regarded as a prerequisite for their reversible actuation. While thermoplastic elastomers based on block copolymers offer a structural model for constructing robust physically crosslinked networks, it remains a significant challenge to transplant this design strategy into LCEs to realize reversible actuation in non-covalently crosslinked system. Herein, we develop a physically crosslinked thermoplastic LCE system based on ABA-type triblock copolymers (PS-b-MCLCP-b-PS). Polystyrene (PS) hard-block aggregates act as reversible physical crosslinking sites, effectively replacing permanent covalent bonds. We systematically investigated the regulatory effect of the PS block content on the microstructure, mechanical properties, and thermally responsive actuation of the materials. By achieving an optimal balance between physical network confinement and the segment mobility of the liquid crystal phase, the resultant elastomer exhibits excellent reversible thermally driven actuation, well-balanced mechanical properties and solvent recyclability with high mechanical retention. Furthermore, the material demonstrates prominent wide-temperature-range damping performance attributed to the synergistic energy dissipation of the physical network and mesogen rotation. This work offers a feasible molecular design strategy for sustainable and multifunctional LCEs to break the dependence on chemical crosslinking for reversible actuation.Keywords：Liquid crystal elastomer;Block copolymer;Soft actuator;Reversible thermo-responsive deformation5|2|0Updated：2026-07-20
- Abstract：The foam materials used in cushioning and protective applications often face a trade-off between flame retardancy and energy absorption. Ethylene–vinyl acetate (EVA) foams are lightweight, flexible, and highly flammable, which restricts their broader engineering applications. In this study, a multifunctional additive, silane-modified zinc ion–reinforced melamine phosphate (ZnMP), was developed via in situ ion complexation and surface grafting to overcome the incompatibility between flame retardancy and mechanical performance in conventional intumescent systems. Compared to pristine melamine phosphate (MPP), ZnMP forms a coordinated structure through Zn2+ interactions with nitrogen- and phosphorus-containing groups. When incorporated into the EVA foams at 15 wt%, ZnMP acted as an efficient heterogeneous nucleating agent, generating a dense microporous structure. Meanwhile, the silane coupling agent enhanced the interfacial interaction between the ZnMP and the EVA matrix, enabling effective reinforcement. Consequently, the EVA/ZnMP foam exhibited significantly improved mechanical properties, including a 144.3% increase in storage modulus, 21.4% increase in energy adsorption, and 88.6% cyclic compression retention after 10 cycles (80% strain). In addition, Zn2+ promoted the formation of a compact char layer during combustion, leading to excellent flame-retardant performance with a limiting oxygen index (LOI) of 25.3%, UL-94 V-0 rating, and a 41.0% reduction in the peak heat release rate. This ion-coordination and interfacial modification strategy offers a promising route for developing lightweight EVA foams with balanced mechanical reinforcements and flame-retardant properties for cushioning and protective applications.Keywords：Zinc ion reinforcement;Melamine phosphate;Ethylene–vinyl acetate foam;Flame retardancy;Energy absorption14|4|0Updated：2026-07-15
- Abstract：To address the limited toughness of poly(ethylene terephthalate) (PET) monofilaments arising from the inherent molecular chain rigidity, this study prepared PET/poly(butylene terephthalate) (PBT) blend monofilaments via the melt-blend spinning method to enhance their toughness. The influence of PBT content on the structural evolution and properties of the blend system was systematically investigated. These results indicate that the PBT content significantly influences the extent of transesterification and compatibility, thereby dictating the mechanical behavior of the monofilaments. At a low PBT content of 2 wt%, transesterification was negligible. The monofilaments exhibited a uniform radial gradient orientation without a distinct skin-core structure, demonstrating optimal overall mechanical performance with markedly improved strength. Specifically, the tensile, loop, and knot strengths were 611, 421, and 443 MPa, respectively. When the PBT content exceeded 5 wt%, the flexible chain segments of PBT enhanced the molecular chain mobility in the blend chips, leading to an increase in crystallite size. However, intensified transesterification concurrently reduces the crystallizability and degrades the mechanical properties. At PBT contents above 15 wt%, SEM analysis revealed phase separation and pronounced heterogeneity in the radial gradient structure of the blend monofilaments, resulting in a significant deterioration of the mechanical properties. This study elucidates the pivotal role of blending ratio in governing the “composition-structure-property” relationship of PET/PBT-blended monofilaments, revealing the underlying mechanism of transesterification and gradient structure development. These findings provide a theoretical foundation for the design of high-performance PET monofilaments.Keywords：Poly(ethylene terephthalate) monofilament;Gradient structure;Melt-blend spinning19|23|0Updated：2026-07-15
- Abstract：Protein stability is a critical factor that limits its application in biopharmaceuticals, clinical diagnostics, and industrial production. The inherent instability of proteins renders them susceptible to loss of activity and function under external environmental stresses, thus necessitating the development of novel stabilizers to improve protein stability. Inspired by sericin, we developed heterochiral poly-β-homoserine (β-HS) that combines resistance to enzymatic degradation, straightforward synthesis, and precise composition control, while exhibiting favorable in vitro safety profile. The β-HS exhibits remarkable stabilizing effects on horseradish peroxidase (HRP) and β-galactosidase (β-Gal) when subjected to elevated temperature and lyophilization, respectively. Our research indicates that β-HS stabilizes proteins by assisting in the maintenance of their conformation and preventing aggregation. Additionally, β-HS demonstrates stabilizing effects on proteins with diverse physicochemical properties. Therefore, this study suggests that the β-HS is a promising candidate for enhancing protein stability.Keywords：Silk sericin;Poly-β-homoserine;Protein protection;Stabilizer;Ring-opening polymerization18|17|0Updated：2026-07-10
- Abstract：High-temperature polymer dielectrics are critically needed for advanced power electronics; however, their performance is often compromised by charge-transfer complexes (CTC) in aromatic polyimides. To overcome this limitation, we introduced an ultra-low loading of 5,10,15,20-tetra(4-aminophenyl) porphyrin (TAPP) as a multifunctional crosslinker into a polyimide (PI) matrix. TAPP simultaneously establishes covalent crosslinking and trap engineering, and its amino groups form a robust network with PI chains, whereas the porphyrin cycle acts as an efficient deep-level charge trap, effectively suppressing CTC formation and charge migration. The optimized PCPI films exhibited a tunable non-monotonic dielectric constant while maintaining a low loss. The PCPI-0.1 sample shows a significantly enhanced breakdown strength and achieves high discharge energy densities of 8.78, 6.09, and 4.97 J·cm−3 at 25, 150, 200 °C, respectively, while maintaining an efficiency above 85%. Remarkably, PCPI-0.1 delivered superior energy density compared to most high-temperature polymer dielectrics reported in the literature, coupled with excellent cycling stability and aging resistance. This work presents a strategy based on ultra-low-loading crosslinking that integrates structural modulation with deep-trap engineering, offering a viable pathway to high-performance all-organic dielectrics for extreme-condition applications.Keywords：Ultra-low loading;Covalent crosslinking;Trap engineering;Charge-transfer complexes;Energy storage;High-temperature31|21|0Updated：2026-07-10
- Abstract：Simultaneously optimizing the optoelectronic properties and the morphology of active layer is the key to high-performance polymer solar cells. Here, we present a novel materials-processing paradigm that incorporates a thermally activated delayed fluorescence (TADF) additive into the layer-by-layer (LBL) fabrication process to concurrently optimize nanoscale morphology and mitigate non-radiative recombination. We demonstrate that the TADF additive facilitates the formation of an ideal interpenetrating network during LBL film deposition, while its intrinsic TADF properties effectively reduce non-radiative voltage loss, enhance exciton lifetimes, and facilitate charge generation and transport. Devices fabricated with this synergistic strategy achieve both high short-circuit current density and open-circuit voltage, culminating in a remarkable power conversion efficiency exceeding 20%. This work not only provides an efficient and reproducible processing route for high-performance polymer solar cells (PSCs) but also opens a new avenue for addressing fundamental optoelectronic limitations through coordinated material design and processing innovation.Keywords：Polymer solar cell;Layer-by-layer;Thermally-activated delay fluorescence;Additive engineering;High-performance organic solar cell27|29|0Updated：2026-07-10
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