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Opposite Self-Folding Behavior of Polymeric Photoresponsive Actuators Enabled by a Molecular Approach
摘要： The ability to obtain 3D polymeric objects by a 2D-to-3D shape-shifting method is very appealing for polymer integration with different materials, from metals in electronic devices to cells in biological studies. Such functional reshaping can be achieved through self-folding driven by a strain pattern designed into the molecular network. Among polymeric materials, liquid crystalline networks (LCNs) present an anisotropic molecular structure that can be exploited to tailor internal strain, resulting in a natural non-planar geometry when prepared in the form of flat films. In this article, we analyze the influence of different molecular parameters of the monomers on the spontaneous shape of the polymeric films and their deformation under different stimuli, such as heating or light irradiation. Modifying the alkilic chains of the crosslinkers is a simple and highly effective way to increase the temperature sensitivity of the final actuator, while modifying ester orientation on the aromatic core interestingly acts on the bending direction. Combining such effects, we have demonstrated that LCN stripes made of different monomeric mixtures originate complex non-symmetric deformation under light activation, thus opening up new applications in photonic and robotics.
关键词： photonic actuators,liquid crystalline networks,curvature design,photoresponsive polymers,shape-changing materials
更新于2025-11-21 11:24:58
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Tailoring the collagen film structural properties via direct laser crosslinking of star-shaped polylactide for robust scaffold formation
摘要： Application of restructured collagen-based biomaterials is generally restricted by their poor mechanical properties, which ideally must be close to those of a tissue being repaired. Here, we present an approach to the formation of a robust biomaterial using laser-induced curing of a photosensitive star-shaped polylactide. The created collagen-based structures demonstrated an increase in the Young’s modulus by more than an order of magnitude with introduction of reinforcing patterns (from 0.15±0.02 MPa for the untreated collagen to 51.2±5.6 MPa for the reinforced collagen). It was shown that the geometrical configuration of the created reinforcing pattern affected the scaffold’s mechanical properties only in the case of a relatively high laser radiation power density, when the effect of accumulated thermomechanical stresses in the photocured regions was significant. Photo-crosslinking of polylactide did not compromise the scaffold’s cytotoxicity and provided fluorescent regions in the collagen matrix, that create a potential for noninvasive monitoring of such materials’ biodegradation kinetics in vivo.
关键词： mechanical properties,collagen,reinforcements,photopolymerization,biocompatible polymers,riboflavin
更新于2025-11-21 11:24:58
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Effect of processing conditions on additive DISC patterning of P3HT films
摘要： There is a critical need to develop a method to pattern semiconducting polymers for device applications on the sub-micrometer scale. Dopant induced solubility control (DISC) patterning is a recently published method for patterning semiconductor polymers that has demonstrated sub-micron resolution. DISC relies on the sequential addition of molecular dopants (here 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ)) to the conjugated polymer. In doped areas, the conjugated polymer is protected from dissolution while in undoped areas, the polymer dissolves into solution. Here we examine factors that affect the resolution of the developed pattern. Two factors are determined to be critical to pattern resolution, the initial crystallinity of the polymer, here poly(3-hexylthiophene) (P3HT), and the quality of the development solvent. We find that dopants diffuse more readily in highly crystalline films than in amorphous films of P3HT and that dopant diffusion reduces the fidelity of the resulting pattern. We also find that the choice of development solvent affects both the fidelity of the pattern and dopant distribution within the patterned polymer domains. Finally, we show that a dopant that diffuses more slowly than F4TCNQ in the P3HT film can be used to pattern the film with higher fidelity. These results together provide a road map for optimizing additive DISC patterning for any polymer/dopant pair.
关键词： crystallinity,semiconducting polymers,development solvent,pattern fidelity,P3HT,DISC patterning,F4TCNQ
更新于2025-11-21 11:08:12
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Conjugated Polymer–Assisted Grain Boundary Passivation for Efficient Inverted Planar Perovskite Solar Cells
摘要： Grain boundaries in lead halide perovskite films lead to increased recombination losses and decreased device stability under illumination due to defect-mediated ion migration. The effect of a conjugated polymer additive, poly(bithiophene imide) (PBTI), is investigated in the antisolvent treatment step in the perovskite film deposition by comprehensive characterization of perovskite film properties and the performance of inverted planar perovskite solar cells (PSCs). PBTI is found to be incorporated within grain boundaries, which results in an improvement in perovskite film crystallinity and reduced defects. The successful defect passivation by PBTI yields reduces recombination losses and consequently increases power conversion efficiency (PCE). In addition, it gives rise to improved photoluminescence stability and improved PSC stability under illumination which can be attributed to reduced ion migration. The optimal devices exhibit a PCE of 20.67% compared to 18.89% of control devices without PBTI, while they retain over 70% of the initial efficiency after 600 h under 1 sun illumination compared to 56% for the control devices.
关键词： halide perovskites,conjugated polymers,grain boundary passivation,nickel oxide
更新于2025-11-20 15:33:11
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Vanadium salt assisted solvothermal reduction of graphene oxide and the thermoelectric characterisation of the reduced graphene oxide in bulk and as composite
摘要： The solvothermal reduction of graphene oxide (GO), modified by the addition of vanadium chloride, resulted in an increased reduction degree of the reduced graphene oxide (rGO), which is reflected by a remarkably increased electrically conductivity of up to 8.5 S/cm, a value 30 times higher than that of rGO prepared without vanadium salt addition. Parallel with this increase, the thermoelectrical properties of rGO are improved, with a reached maximum Seebeck coefficient of 13.7 μV/K. The rGOs were used as fillers in flexible styrene-butadiene-styrene triblock copolymer composites prepared by solution mixing. Compared to the traditionally prepared reduced graphene oxide, the new product provides up to 60 times higher conductivity to the composite, while the Seebeck coefficient is nearly the same. The highest power factor of 4.6 x 10-4 μW/(m·K2) was achieved at 100 °C with 30 wt% loading, which is 30 times higher than that of the traditional reduced graphene oxide containing composite.
关键词： nanomaterials,functional materials,energy materials,composites,polymers
更新于2025-11-19 16:56:35
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Multi-scale ordering in highly stretchable polymer semiconducting films
摘要： Stretchable semiconducting polymers have been developed as a key component to enable skin-like wearable electronics, but their electrical performance must be improved to enable more advanced functionalities. Here, we report a solution processing approach that can achieve multi-scale ordering and alignment of conjugated polymers in stretchable semiconductors to substantially improve their charge carrier mobility. Using solution shearing with a patterned microtrench coating blade, macroscale alignment of conjugated-polymer nanostructures was achieved along the charge transport direction. In conjunction, the nanoscale spatial confinement aligns chain conformation and promotes short-range π–π ordering, substantially reducing the energetic barrier for charge carrier transport. As a result, the mobilities of stretchable conjugated-polymer films have been enhanced up to threefold and maintained under a strain up to 100%. This method may also serve as the basis for large-area manufacturing of stretchable semiconducting films, as demonstrated by the roll-to-roll coating of metre-scale films.
关键词： charge carrier mobility,conjugated polymers,solution shearing,stretchable semiconductors,roll-to-roll coating,multi-scale ordering
更新于2025-11-19 16:56:35
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Synthesis of π-conjugated poly(arylene)s by polycondensation of 1,4-bis(3-methylpyridin-2-yl)benzene and aryl dibromides through regiospecific C-H functionalization process
摘要： On the basis of the Ru-catalyzed regiospeci?c direct double arylation of benzene rings possessing 3-methylpyridin-2-yl substituents to produce 1-aryl-2-(3-methylpyridin-2-yl)benzene derivatives, the synthesis of poly(p-phenylene) derivatives having 2,5-bis(3-methylpyridin-2-yl) substituents is described. The reaction of 1,4-bis(3-methylpyridin-2-yl)benzene with bromobenzene (2 equiv) was carried out in the presence of [RuCl2(η6-C6H6)]2 (5 mol %) in 1-methyl-2-pyrrolidone at 120°C for 24 h to produce 1,4-bis(3-methylpyridin-2-yl)-2,5-diphenylbenzene in 99% yield as a sole product. Neither 2,6-diphenylated nor further phenylated products was produced under the examined conditions. This regiospeci?c double arylation process was then applied to the synthesis of π-conjugated polymers by use of aryl dibromides such as 1,4-dibromobenzene, 2,7-dibromo-9,9-dihexyl?uorene, and 2,5-dibromothiophene. For example, a polymer was obtained in 73% yield by using 1,4-dibromobenzene, whose Mn and Mw/Mn were estimated to be 3300 and 1.51, respectively. The bathochromic shift of the ultraviolet (UV)–visible absorption spectrum with respect to that of the model compound, 1,4-bis(3-methylpyridin-2-yl)-2,5-diphenylbenzene, indicated the extension of the π-conjugation. The blue ?uorescence was also observed for the polymer upon the UV irradiation.
关键词： C-H functionalization,direct double arylation,poly(arylene)s,π-conjugated polymers
更新于2025-11-19 16:46:39
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Photo-Controlled Release of Metal Ions Using Triazoline-Containing Amphiphilic Copolymers
摘要： Photo-controlled release that shows quick response and high spatial/temporal accuracy has become attractive given its potential applications for biomedicines. A few metal complexes are known for detoxification, sterilization, diagnosis and treatment of diseases; but, the encapsulation and control release of those metal ions using polymer micelles are challenging. We report an interesting photo-controlled release of metal ions via photo-responsible triazoline-containing amphiphilic polymers. Amphiphilic random copolymers of glycidyl methacrylate and oligo(ethylene oxide) methyl ether methacrylate were prepared through free radical copolymerization. The glycidyl pendants were converted to azide, followed by a 1,3-dipolar cycloaddition reaction to form triazoline with norbornene. The resulting random copolymers containing triazoline formed micelles with a critical micellar concentration (CMC) of 7.68×10-3 mg/mL. The triazoline moieties could coordinate to transition metal ions, e.g. Co2+, thus to encapsulate the metal ions to the core of micelles. Photo-induced denitrogenation of triazoline was able to disrupt the coordination of Co2+ and triazoline, therefore leading to the release of Co2+. Solution viscosity, UV-vis/NMR spectroscopy and TEM were used to show that the coordination and release of Co2+ ions were successful upon exposure to light. The photo-controlled release profile was found to be linearly dependent on the irradiation time, which is potentially useful for the delivery of essential ions in vivo.
关键词： Light responsive,Amphiphilic polymers,Micelles,Triazoline,Photo-controlled release
更新于2025-11-19 16:46:39
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Novel fluorescent sensor using molecularly imprinted silica microsphere‐coated CdSe@CdS quantum dots and its application in the detection of 2,4,6‐trichlorophenol from environmental water samples
摘要： In this study, a high fluorescence sensitivity and selectivity, molecularly imprinted nanofluorescent polymer sensor (MIP@SiO2@QDs) was prepared using a reverse microemulsion method. 2,4,6-Trichlorophenol (2,4,6-TCP) was detected using fluorescence quenching. Tetraethyl orthosilicate (TEOS), quantum dots (QDs) and 3-aminopropyltriethoxysilane (APTS) were used as cross-linker, signal sources and functional monomer respectively. The sensor (MIP@SiO2@QDs) and the non-imprinted polymer sensor (NIP@SiO2@QDs) were characterized using infra-red (IR) analysis, X-ray diffraction (XRD), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The selectivity of MIP@SiO2@QDs was examined by comparing 2,4,6-TCP with other similar functional substances including 2,4-dichlorophenol (2,4-DCP), 2,6-dichlorophenol (2,6-DCP) and 4-chlorophenol (4-CP). Results showed that MIP@SiO2@QDs had better selectivity for 2,4,6-TCP than the other compounds. Fluorescence quenching efficiency displayed a good linear response at the 2,4,6-TCP concentration range 5–1000 μmol/L. The limit of detection (LOD) was 0.9 μmol/L (3σ, n = 9). This method was equally applicable for testing actual samples with a recovery rate of 98.0–105.8%. The sensor had advantages of simple pretreatment, good sensitivity and selectivity, and wide linear range and could be applied for the rapid detection of 2,4,6-TCP in actual samples.
关键词： quantum dots,2,4,6-trichlorophenol,fluorescence,molecularly imprinted polymers
更新于2025-11-19 16:46:39
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Reorientational dynamics of organic cations in perovskite-like coordination polymers
摘要： Here we report the dynamics of organic cations as guest molecules in a perovskite host-framework. The molecular motion of CH3NH3+ (MAFe), (CH3)2NH2+ (DMAFe) and (CH3)3NH+ (TrMAFe) in the cage formed by KFe(CN)63? units was studied using a combination of experimental methods: (i) thermal analysis, (ii) dielectric and electric studies, (iii) optical observations, (iv) EPR and 1H NMR spectroscopy and (v) quasielastic neutron scattering (QENS). In the case of MAFe and TrMAFe, the thermal analysis reveals one solid-to-solid phase transition (PT) and two PTs for the DMAFe crystal. A markedly temperature-dependent dielectric constant indicates the tunable and switchable properties of the complexes. Also, their semiconducting properties are confirmed by a dc conductivity measurement. The broadband dielectric relaxation is analyzed for the TrMAFe sample in the frequency range of 100 Hz–1 GHz. QENS shows that we deal rather with the localized motion of the cation than a diffusive one. Three models, which concern the simultaneous rotation of the CH3 and/or NH3 group, π-flips and free rotations of the organic cation, are used to fit the elastic incoherent structure factor. The 1H NMR spin–lattice relaxation time for all compounds under study, as well as the second moments, has been measured in a wide temperature range. In all studied samples, the temperature dependence of the second moment of the proton NMR line indicated the gradual evolution of the molecular movements from the rigid state up to a highly disordered one.
关键词： quasielastic neutron scattering,phase transitions,perovskite,coordination polymers,dielectric properties,NMR spectroscopy,dynamics,organic cations
更新于2025-11-14 17:28:48