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Fluorine-phenanthroimidazole Porous Organic Polymer: Efficient Microwave Synthesis and Photocatalytic Activity
摘要： A porous polymer containing a fluorophenylphenanthroimidazole core was easily prepared via one-pot Suzuki-Miyaura cross coupling reactions under microwave heating. These new metal-free polymers have demonstrated heterogeneous photocatalytic activity toward aza-Henry reaction with reasonable recyclability. Their preparation require a minimal workup to build porous networks with control over the apparent surface area and pore volume from suitable molecular building blocks containing the 2-(1H-phenanthro[9,10-d]imidazol-2-yl)-3,5-difluorophenol (PhIm-2F), as rigid and multitopic node which afforded a conjugated porous polymer (CPP-PhIm-2F). A series of fluorinated ligands have shown their capability to preparation of soluble and supported cationic Ru(bpy)2(F-phenanthroimidazole)-complexes by reaction with Ru(bpy)2Cl2 and demonstrated a beneficial effect of two fluorine atom on the photocatalytic effect.
关键词： Conjugated polymer,Ruthenium photocatalyst,Photocatalysis,Aza-Henry,Heterogenized catalyst,Porous organic polymer,Phenanthroimidazole
更新于2025-09-23 15:19:57
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A New Benzodithiophene Based Donor-Acceptor ??-Conjugated Polymer for Organic Solar Cells
摘要： A new benzodithiophene based donor-acceptor π-conjugated polymer (P1) is designed and explored as the photoactive donor for organic solar cells (OSCs). The synthesized donor polymer, P1 displays a wide absorption profile ranging from 300-750 nm with optical band gap of 1.61 eV and moderate ionization potential of -5.30 eV. It has good solubility in non-halogenated and halogenated organic solvents. Next, we fabricated OSCs with P1 by blending with PC71BM, the pristine polymer processed from chlorobenzene showed PCE of 2.79%. Upon addition of external additive diphenyl ether to the blend showed a dramatic improvement in PCE with maximum of 5.33%. DPE tailored the active layer morphology and showed two times higher PCE than pristine films. These results clearly indicate that the new polymer has a great potentiality for enhancing efficiency upon solvent additives, which will provide new routes for the development of new class of polymers for high-performance air-stable OSCs.
关键词： benzodithiophene based π-conjugated polymer,organic solar cell,morphology,octyl side chain
更新于2025-09-23 15:19:57
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Organic-inorganic hybrid heterostructures towards long-wavelength photodetectors based on InGaZnO-Polymer
摘要： Organic-inorganic hybrid heterostructures have attracted considerable attentions due to their wide application in electronics and optoelectronics. In this study, a high-performance red light photodetector based on organic-inorganic heterostructure was successfully fabricated after a systematical optimization in material and device constitution. The conjugated polymer (P(PDI-BDT-O)) with narrow band gap used as light absorber was combined with a layer of indium gallium zinc oxide (IGZO) to construct a bi-layered phototransistor achieving a high mobility as well as high photoresponsivity. Benefiting from both the high absorption coefficient of the polymer over a wide range of wavelength and the perfect matching of band level between polymer and IGZO, the device exhibits an ultrahigh photoresponsivity (212 A/W) and specfic detectivity (2 ? 1012 Jones) for red light at the wavelength of 633 nm. These results demonstrate the great potential of organic-inorganic heterostructures in the application of long-wavelength photodetectors.
关键词： Conjugated polymer,Oxide semiconductor,Organic-inorganic heterostructures,Red light photodetector
更新于2025-09-23 15:19:57
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Direct Observation of Structure and Dynamics of Photogenerated Charge Carriers in Poly(3-hexylthiophene) Films by Femtosecond Time-Resolved Near-IR Inverse Raman Spectroscopy
摘要： The initial charge separation process of conjugated polymers is one of the key factors for understanding their conductivity. The structure of photogenerated transients in conjugated polymers can be observed by resonance Raman spectroscopy in the near-IR region because they exhibit characteristic low-energy transitions. Here, we investigate the structure and dynamics of photogenerated transients in a regioregular poly(3-hexylthiophene) (P3HT):[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) blend film, as well as in a pristine P3HT film, using femtosecond time-resolved resonance inverse Raman spectroscopy in the near-IR region. The transient inverse Raman spectrum of the pristine P3HT film at 50 ps suggests coexistence of neutral and charged excitations, whereas that of the P3HT:PCBM blend film at 50 ps suggests formation of positive polarons with a different structure from those in an FeCl3-doped P3HT film. Time-resolved near-IR inverse Raman spectra of the blend film clearly show the absence of charge separation between P3HT and PCBM within the instrument response time of our spectrometer, while they indicate two independent pathways of the polaron formation with time constants of 0.3 and 10 ps.
关键词： polaron,femtosecond inverse Raman spectroscopy,conjugated polymer,bulk heterojunction
更新于2025-09-19 17:15:36
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Photocontrolled synthesis of na??type conjugated polymers
摘要： Current approaches to synthesize π-conjugated polymers (CPs) are dominated by thermally driven, transition metal-mediated reactions. Herein we show that electron-deficient Grignard monomers readily polymerize under visible light irradiation at room temperature in the absence of a catalyst. The product distribution can be tuned by the wavelength of irradiation based on the absorption of the polymer. Conversion studies are consistent with an uncontrolled chain-growth process; correspondingly, chain extension produces all-conjugated n-type block copolymers. Preliminary results demonstrate that the polymerization can be expanded to donor-acceptor alternating copolymers. We anticipate that this method can serve as a platform to access new architectures of n-type CPs without the need for transition metal catalysis.
关键词： photopolymerization,transition-metal-free,conjugated polymer
更新于2025-09-19 17:13:59
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Molecular engineering of a conjugated polymer as a hole transporting layer for versatile p–i–n perovskite solar cells
摘要： Along with the development of perovskite materials, which have enormous potential for optoelectronics such as solar cells and light-emitting diode devices, numerous organic semiconductor polymers, which have been critically adopted into the hole and electron transporting layers, have been synthesized and studied. In neiep-structured perovskite solar cells, various outstanding polymer materials have been successfully applied. However, in peien-structured solar cells, the hydrophobic nature of the polymers makes the sequential deposition of a perovskite thin ?lm dif?cult. Several destructive methods have been proposed; however, a more ef?cacious and fundamental method is urgently needed. Here, we present a nondestructive polymer hole-transporting layer (HTL) thin-?lm formation process based on molecular engineering via a simple solvent process. When we used various solvents with different volatilities, perovskite ?lm formation was achieved on polymer thin ?lms formed from highly volatile solvents. In addition, we elucidated the structure and orientation of the molecules in the ?lms and revealed that the molecular structure of face-on orientation for the horizontally aligned hydrophobic alkyl groups induced a lower surface energy of the ?lm, as determined by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. Furthermore, the tilt angle of the molecules, which was calculated from the results of quantitative near-edge X-ray absorption ?ne structure (NEXAFS) analysis, was found to correlate with the surface energy. This result provides guidance for polymer-orientation and surface-energy studies, and perovskite solar cells fabricated using the polymer HTL demonstrated good durability and ?exibility. We expect that our approach represents a new route for fabricating peien-structured solar cells and that numerous valuable p-type conjugated polymers will be developed via our proposed molecular engineering process.
关键词： Solvent process,Organic semiconductor,Flexible device,Conjugated polymer,Perovskite solar cell,Molecular engineering
更新于2025-09-19 17:13:59
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Enhanced Stability and Performance of Air-Processed Perovskite Solar Cells via Defect Passivation with Thiazole-Bridged Diketopyrrolopyrrole-Based ??-Conjugated Polymer
摘要： Minimization of the defects at grain boundaries and/or the film surface of organic–inorganic halide perovskites becomes increasingly important to produce highly-efficient and long-term stable perovskite solar cells (PeSCs). In this study, we present a promising strategy to enhance the performance and stability of PeSCs by using thiazole-bridged diketopyrrolopyrrole (DPP)-based semiconducting polymer poly{3-(5-([2,2′-bithiophen]-5-yl)thiazol-2-yl)-2,5-bis(2-octyldodecyl)-6-(thiazol-2-yl) pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione} (PTzDPPBTz) as the passivation layer. Our results indicate a large amount of Lewis base functional groups present in PTzDPPBTz can effectively passivate the defects and vacancies created by under-coordinated Pb atoms without significantly altering the microstructure of the perovskite film, enabling the perovskite film to exhibit superior stability while preserving their good optoelectronic properties. Meanwhile, the appropriate energy level of PTzDPPBTz can facilitate efficient charge transfer at the interface. With PTzDPPBTz passivation layer, the devices deliver power conversion efficiency (PCE) up to 20.30% (stabilized PCE = 20.39%) without photocurrent hysteresis, surpassing the efficiency of the devices without passivation layer (PCE = 16.58%). Importantly, PTzDPPBTz passivation layer can also be applicable for air-processed devices prepared under high relative humidity level (72 ± 3%), delivering almost comparable PCE (19.19%) to those obtained for the devices processed under inert atmosphere. To the best of ourknowledge, 19.19% represents the highest PCE ever reported for air-processed PeSCs prepared under the relative humidity exceeding 70%. In addition, the feasibility of using conjugated polymer-based passivation layer for monolithic all-perovskite tandem solar cells is firstly demonstrated, and a remarkably high open-circuit voltage (Voc) of 1.87 V is attained, which is much higher than those of the tandem cells without passivation (1.76 V). More encouragingly, long-term stable devices are demonstrated by simply applying UV-curable epoxy/poly[perfluoro(4- vinyloxy-1-butene)] (CYTOP) bilayer film as the encapsulation layer, rataining ≈65% of their initial PCE after 890 hours of continuous operation in ambient air. Our findings provide a new avenue to improve both the efficiency and stability of air-processed PeSCs via defect passivation.
关键词： efficiency,defect passivation,air-processed,π-conjugated polymer,stability,thiazole-bridged diketopyrrolopyrrole,perovskite solar cells
更新于2025-09-19 17:13:59
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Elevated Photovoltaic Performance in Medium Bandgap Copolymers Composed of Indacenodi-thieno[3,2-b]thiophene and Benzothiadiazole Subunits by Modulating the ??-Bridge
摘要： Two random conjugated polymers (CPs), namely, PIDTT‐TBT and PIDTT‐TFBT, in which indacenodithieno[3,2‐b]thiophene (IDTT), 3‐octylthiophene, and benzothiadiazole (BT) were in turn utilized as electron‐donor (D), π‐bridge, and electron‐acceptor (A) units, were synthesized to comprehensively analyze the impact of reducing thiophene π‐bridge and further fluorination on photostability and photovoltaic performance. Meanwhile, the control polymer PIDTT‐DTBT with alternating structure was also prepared for comparison. The broadened and enhanced absorption, down‐shifted highest occupied molecular orbital energy level (EHOMO), more planar molecular geometry thus enhanced the aggregation in the film state, but insignificant impact on aggregation in solution and photostability were found after both reducing thiophene π‐bridge in PIDTT‐TBT and further fluorination in PIDTT‐TFBT. Consequently, PIDTT‐TBT‐based device showed 185% increased PCE of 5.84% profited by synergistically elevated VOC, JSC, and FF than those of its counterpart PIDTT‐DTBT, and this improvement was chiefly ascribed to the improved absorption, deepened EHOMO, raised μh and more balanced μh/μe, and optimized morphology of photoactive layer. However, the dropped PCE was observed after further fluorination in PIDTT‐TFBT, which was mainly restricted by undesired morphology for photoactive layer as a result of strong aggregation even if in the condition of the upshifted VOC. Our preliminary results can demonstrate that modulating the π‐bridge in polymer backbone was an effective method with the aim to enhance the performance for solar cell.
关键词： 2‐b]thiophene,random conjugated polymer,modulating π‐bridge,indacenodithieno[3,photovoltaic property
更新于2025-09-19 17:13:59
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Conjugated Polymer Controlled Morphology and Charge Transport of Small-Molecule Organic Semiconductors
摘要： In this study, we report an effective approach to tune the crystallization, microstructure and charge transport of solution-processed organic semiconductors by blending with a conjugated polymer additive poly(3-hexylthiophene) (P3HT). When 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene) was used as a model semiconductor material to mix with different amount of P3HT, their intermolecular interactions led to distinctive TIPS pentacene film morphologies, including randomly-oriented crystal ribbons, elongated needles with enhanced long-range order, and grass-like curved microwires with interlinkages. Each type of morphology was found to further correlate to considerably different charge transport and device performance. As compared to pristine TIPS pentacene devices, bottom-gate, top-contact OTFTs with 2% in weight P3HT additive showed a 2-fold and 5-fold improvement of average field-effect mobility and performance consistency (defined as the ratio of average mobility to the standard deviation), respectively. The improvement in transistor electrical performance can be attributed to the combined effect of enhanced crystal orientation and uniformity, as well as increased areal coverage. This work can be applied beyond the particular example demonstrated in this study and to tune the charge transport of other small-molecule organic semiconductors in general.
关键词： OTFTs,TIPS pentacene,organic semiconductors,film morphology,P3HT,charge transport,conjugated polymer
更新于2025-09-19 17:13:59
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Donor–acceptor type black phosphorus nanosheets covalently functionalized with a conjugated polymer for laser protection
摘要： Covalent functionalization of two-dimensional black phosphorus (BP) with conjugated polymers would be favorable to improve its environmental stability and solubility in organic solvents, and thereby to open a way to explore more applications of BP in the fields of optoelectronics, electronics and photonics. As a proof-of-concept application, soluble donor–acceptor type BP nanosheets covalently functionalized with poly[(1,4-diethynyl-2,5-bis(hexyloxy)benzene)-alt-benzo[c]thiadiazole] (hereafter called PDBT-BP) were synthesized through Sonogashira–Hagihara coupling polymerization, and embedded into an optically nonactive transparent poly(methylmethacrylate) (PMMA) matrix to produce the PMMA-based PDBT-BP film for nonlinear optics. In contrast to BP/PMMA, PDBT-BP/PMMA and PDBT/BP blends/PMMA films, the annealed PDBT-BP/PMMA film, which was heated at 150 °C under dry argon for 1 h, shows more excellent reverse saturable absorption (RSA) behavior, with a larger nonlinear absorption coefficient (βeff ) of 208.16 cm GW?1 and an imaginary third-order susceptibility (Im χ(3)) of 8.89 × 10?11 esu at a pulse energy of 400 μJ. The achieved optical limiting (OL) threshold is 4.44 J cm?2 (0.74 GW cm?2), smaller than that of the non-annealed PDBT-BP/PMMA film (5.64 J cm?2). The SA (saturable absorption) to RSA transition observed at a low incident laser intensity could be used to realize all-optical intensity-dependent logic gates in the near future.
关键词： Conjugated Polymer,Laser Protection,Polymer Chemistry,Black Phosphorus,Nonlinear Optics
更新于2025-09-16 10:30:52