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Photocontrolled Iodine-Mediated Green Reversible-Deactivation Radical Polymerization of Methacrylates: Effect of Water in the Polymerization System
摘要： Photocontrolled iodine-mediated reversible-deactivation radical polymerization (RDRP) is a facile and highly efficient access to precision polymers. Herein, a facile photocontrolled iodine-mediated green RDRP strategy was successfully established in water by using 2-iodo-2-methylpropionitrile (CP-I) as the initiator and water-soluble functional monomers including poly(ethylene glycol) methyl ether methacrylate (PEGMA), 2-hydroxyethyl methacrylate (HEMA), and 2-hydroxypropyl methacrylate (HPMA) as the model monomers under blue-light-emitting diode (LED) irradiation at room temperature. Well-defined polymers (PPEGMA, PHEMA, PHPMA) with narrow polydispersities (1.09?1.21) were obtained, and amphiphilic block copolymers which can form nanospheres in situ in water (PPEGMA-b-poly(benzyl methacrylate) (PPEGMA-b-PBnMA) and PPEGMA-b-PHPMA) were prepared. To explore the role of water in our polymerization, control experiments were successfully carried out by using oil-soluble monomer methyl methacrylate (MMA) with the help of trace amounts of water. Notably, the green solvent—water—has an additionally positive effect in accelerating the polymerization and makes our polymerization system an environmentally friendly polymerization system. Therefore, this simple strategy conducted in the presence of water enables the green preparation of well-defined water-soluble or water-insoluble polymers and clean synthesis of amphiphilic copolymer nanoparticles in situ.
关键词： blue-light-emitting diode,water-soluble functional monomers,amphiphilic block copolymers,green solvent,RDRP,Photocontrolled iodine-mediated reversible-deactivation radical polymerization
更新于2025-09-19 17:13:59
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Effect of chlorination and fluorination of benzothiadiazole on the performance of polymer solar cells
摘要： In order to explore the effects of chlorine and fluorine on photophysical properties and the differences, in this work, we synthesized five new polymers, P1–P5, in which benzo[1,2-b:4,5-b]dithiophene as the electron donating and benzothiadiazole as electron withdrawing. Analysis of these five polymers showed that the introduction of Cl and F atoms can deeper the highest occupied molecular orbital of these polymers and enhance the absorption of light by the species, thereby improving Voc and Jsc. Chlorination has a stronger ability to reduce energy levels and broaden the absorption spectrum compared to fluorination. Among them, P2 showed an efficiency of 4.08% with Jsc of 11.28 mA/cm2, Voc of 0.79 V, and fill factor (FF) of 0.45. Since chlorination is easier than fluorination in terms of synthesis, it is advantageous for practical applications. Therefore, we think that chlorination should not be ignored when designing high efficiency photovoltaic materials, especially when their fluorinated counterparts have proven to have good properties.
关键词： optical properties,copolymers,optical and photovoltaic applications
更新于2025-09-19 17:13:59
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Asymmetric Siloxane-Functional Side Chains Enable High-Performance Donor Copolymers for Photovoltaic Applications
摘要： In this work, three benzodithiophene (BDT)-benzotriazole (BTA) alternated wide bandgap (WBG) copolymers attaching symmetric or asymmetric conjugated side chains, namely PDBTFBTA-2T, PBDTFTBA-TSi and PBDTFBTA-2Si, were developed for efficient nonfullerene polymer solar cells. The symmetry effect of the side chains was investigated in detail on the overall properties of these donor polymers. The results demonstrated that the introduced siloxane functional groups showed less effect on the absorptions and frontier orbital levels of the prepared polymers but had significant effect on the miscibility between these polymer donors and nonfullerene acceptor. If increasing the content of siloxane functional groups, the miscibility of the polymer donors and Y6 would be improved, leading to the decreased domain size and more mixed domains. Interestingly, the active blend based on PBDTFTBA-TSi with asymmetric side chains exhibited more balanced miscibility, carrier mobility and phase separation, benefiting exciton diffusion and dissociation. Therefore, a champion power conversion efficiency (PCE) of 14.18% was achieved finally in PBDTFTBA-TSi devices, which was 20.6% and 19.0% higher than the symmetric counterparts of PBTFBTA-2T devices (PCE = 11.76%) and PBDTFBTA-2Si devices (PCE = 11.92%), respectively. This work highlights that the asymmetric side chain engineering based on siloxane functional groups is a promising design strategy for high-performance polymer donor semiconductors.
关键词： molecular design strategy,nonfullerene polymer solar cells,siloxane functional group,wide bandgap copolymers,asymmetric side chains
更新于2025-09-19 17:13:59
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Macroscopic Alignment of Block Copolymers on Silicon Substrates by Laser Annealing
摘要： Laser annealing is a competitive alternative to conventional oven annealing of block copolymer (BCP) thin films enabling rapid acceleration and precise spatial control of the self-assembly process. Localized heating by a moving laser beam (zone annealing), taking advantage of steep temperature gradients, can additionally yield aligned morphologies. In its original implementation it was limited to specialized germanium-coated glass substrates, that absorb visible light and exhibit low-enough thermal conductivity to facilitate heating at relatively low irradiation power density. Here, we demonstrate a recent advance in laser zone annealing, which utilizes a powerful fiber-coupled near-IR laser source allowing rapid BCP annealing over a large area on conventional silicon wafers. The annealing coupled with photothermal shearing yields macroscopically-aligned BCP films which are used as templates for patterning metallic nanowires. We also report a facile method of transferring laser-annealed BCP films onto arbitrary surfaces. The transfer process allows patterning substrates with a highly corrugated surface and single-step rapid fabrication of multilayered nanomaterials with complex morphologies.
关键词： laser annealing,photothermal processing,block copolymers,nanopatterning,directed self-assembly,multilayers
更新于2025-09-19 17:13:59
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Electrospraying the Triblock Copolymer SEBS: The Effect of Solvent System and the Embedding of Quantum Dots
摘要： This work reports on ABA triblock copolymer microparticles encoded with CdSe/CdS core–shell quantum dots (QDs) realized by electrospraying. This method allows for simple but efficient embedding of QDs in polymer beads while retaining the fluorescent properties of the original QDs. The creation of poly(styrene-ethylene-butylene-styrene) (SEBS) monodisperse spherical microparticles with a tunable morphology for applications of the final QD-loaded product is attainable via solvent variation. By varying the selectivity of the solvent for one of the distinct blocks in the polymer, the final particle morphology can be selectively altered while maintaining the same overall process conditions, allowing to tailor the particles from homogeneously flat in a nonselective solvent to dense spherical particles in an endblock selective solvent system. The mechanism responsible for this transition in morphology can be related to differences in mass transfer in the droplets and thus solvent evaporation rates arising from particular microphase structures. Finally, fluorescence characteristics of the final QD-embedded polymer particles and photodegradation stability are investigated by spectrophotometry and are compared to the temporal evolution of the original QDs, indicating significant stability improvement and well-dispersed QDs in an optimized polymer matrix morphology.
关键词： colloids,block copolymers,polymeric materials,electrospraying,quantum dots
更新于2025-09-16 10:30:52
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Synthesis and properties of hyperbranched polymers for white polymer light-emitting diodes
摘要： In this work, a series of hyperbranched copolymers with fluorene-alt-carbazole as the branches, three-dimensional-structured spiro[3.3]heptane-2,6-dispirofluorene (SDF) as the core, and iridium 1-(4-bromophenyl)-isoquinoline (acetylacetone) (Ir(Brpiq)2acac) as the dimming group were synthesized by one-pot Suzuki polycondensation for white emission. All copolymers show great thermal stabilities and high hole-transporting ability due to the introduction of the carbazole unit. The hyperbranched structures for copolymers can suppress the interchain interactions efficiently, and help to form amorphous films. The fabricated polymer light-emitting devices (PLEDs) based on the above synthesized copolymers realize good white light emission, and achieve high electroluminescence (EL) performance. For example, for the optimized PLED, the maximum luminance and current efficiency reach 6210 cd m?2 and 6.30 cd A?1, respectively, indicating the synthesized hyperbranched copolymers have potential application in solution-processable white polymer light-emitting diodes.
关键词： hyperbranched copolymers,electroluminescence,white emission,Suzuki polycondensation,polymer light-emitting devices
更新于2025-09-16 10:30:52
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Polyfluorene Copolymers as High‐Performance Hole Transport Materials for Inverted Perovskite Solar Cells
摘要： Inverted perovskite solar cells (PSCs) that can be entirely processed at low temperatures have attracted growing attention owing to their cost-effective production. Hole-transport materials (HTMs) play an essential role in achieving efficient inverted PSCs, as they determine the effectiveness of charge extraction and recombination at interfaces. In this study, three polyfluorene copolymers (TFB, PFB and PFO) were investigated as HTMs for construction of inverted PSCs. It is found that the photovoltaic performance of the solar cells is closely correlated with the electronic properties of the HTMs. Owing to its high mobility along with the favored energy level alignment with perovskite, TFB showed superior charge extraction and suppressed interfacial recombination than PFB- and PFO-based devices, which delivers a high efficiency of 18.48% with an open-circuit voltage (VOC) of up to 1.1 V. In contrast, the presence of a large energy barrier in the PFO-based devices resulted in substantial losses in both VOC and photocurrent. These results demonstrate that TFB could serve as a superior HTM for inverted PSCs. Moreover, we anticipate that the performance of the three HTMs identified here might guide molecular design of novel HTMs for the manufacture of highly efficient inverted PSCs.
关键词： hole-transport materials,charge extraction,polyfluorene copolymers,photovoltaic performance,inverted perovskite solar cells
更新于2025-09-12 10:27:22
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Semiconductor Quantum Dots Are Efficient and Recyclable Photocatalysts for Aqueous PET-RAFT Polymerization
摘要： This Letter describes the use of CdSe quantum dots (QDs) as photocatalysts for photoinduced electron transfer reversible addition?fragmentation chain transfer (PET-RAFT) polymerization of a series of aqueous acrylamides and acrylates. The high colloidal solubility and photostability of these QDs allowed polymerization to occur with high efficiency (>90% conversion in 2.5 h), low dispersity (PDI < 1.1), and ultralow catalyst loading (<0.5 ppm). The use of protein concentrators enabled the removal of the photocatalyst from the polymer and monomer with tolerable metal contamination (8.41 ug/g). These isolated QDs could be recycled for four separate polymerizations without a significant decrease in efficiency. By changing the pore size of the protein concentrators, the QDs and polymer could be separated from the remaining monomer, allowing for the synthesis of block copolymers using a single batch of QDs with minimal purification steps and demonstrating the fidelity of chain ends.
关键词： block copolymers,CdSe quantum dots,photocatalysts,aqueous acrylamides,acrylates,protein concentrators,PET-RAFT polymerization
更新于2025-09-12 10:27:22
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Design of arrayed-waveguide optical switch employing window function for crosstalk reduction
摘要： Nanosheets have thicknesses on the order of nanometers and planar dimensions in the micrometer range. Nanomaterials that are capable of converting reversibly between 2D nanosheets and 3D structures in response to specific triggers can enable construction of nanodevices. Supra-molecular lipid nanosheets and their triggered conversions to 3D structures including vesicles and cups are reported. They are produced from lipid vesicles upon addition of amphiphilic peptides and cationic copolymers that act as peptide chaperones. By regulation of the chaperoning activity of the copolymer, 2D to 3D conversions are reversibly triggered, allowing tuning of lipid bilayer structures and functionalities.
关键词： graft copolymers,amphiphilic peptides,2D–3D conversion,lipid nanosheets
更新于2025-09-11 14:15:04
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Metal Oxide Heterostructure Array via Spatially Controlled–Growth within Block Copolymer Templates
摘要： Nanofabrication is continuously searching for new methodologies to fabricate 3D nanostructures with 3D control over their chemical composition. A new approach for heterostructure nanorod array fabrication through spatially controlled–growth of multiple metal oxides within block copolymer (BCP) templates is presented. Selective growth of metal oxides within the cylindrical polymer domains of polystyrene-block-poly methyl methacrylate is performed using sequential infiltration synthesis (SIS). Tuning the diffusion of trimethyl aluminum and diethyl zinc organometallic precursors in the BCP film directs the growth of AlOx and ZnO to different locations within the cylindrical BCP domains, in a single SIS process. BCP removal yields an AlOx-ZnO heterostructure nanorods array, as corroborated by 3D characterization with scanning transmission electron microscopy (STEM) tomography and a combination of STEM and energy-dispersive X-ray spectroscopy tomography. The strategy presented here will open up new routes for complex 3D nanostructure fabrication.
关键词： block copolymers,sequential infiltration synthesis,heterostructures,nanofabrication
更新于2025-09-11 14:15:04