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oe1(光电查) - 科学论文

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Solar cells sensitized with porphyrin dyes with a carbazole donor: The effects of an auxiliary benzothiadiazole acceptor and bulky substituents on the donor

摘要： Three porphyrin sensitizers XW54–XW56 containing a carbazole donor have been designed and synthesized by introducing a benzothiadiazole (BTD) unit as the auxiliary electron acceptor to extend the absorption spectra and/or bulky dihexyloxyphenyl groups into the carbazole unit to suppress dye aggregation and improve the photovoltage (Voc). The BTD unit incorporated in XW54 obviously broadens and red-shifts the absorption threshold to ca. 700 nm, as compared with that of 650 nm observed for XW1. Thus, XW54 exhibits a much broader monochromatic photon-to-electron conversion efficiency (IPCE) spectrum with an extremely red-shifted onset wavelength of 780 nm, resulting in a photocurrent density (Jsc) of 11.60 mA cm?2, higher than that of XW1. Unfortunately, the Voc value was decreased owing to the more severe dye aggregation caused by the large conjugation framework induced by the presence of the BTD unit. As a result, XW54 shows an efficiency of 6.26%, slightly higher than that of 6.11% obtained for XW1. On the other hand, with the bulky dihexyloxyphenyl donor groups introduced to XW55, a highest Voc of 860 mV was achieved, which can be ascribed to the efficient prevention of charge recombination and suppression of dye aggregation. Thus, XW55-based cells exhibit an improved e?ciency of 6.60%. On the basis of XW54 and XW55, two bulky dihexyloxyphenyl groups and a BTD unit were simultaneously introduced to XW56, affording a highest efficiency of 7.03%, with the Jsc and Voc values of 12.5 mA cm?2 and 785 mV, respectively. These results compose a novel approach for developing e?cient dye-sensitized solar cells (DSSCs) by simultaneously introducing bulky dihexyloxyphenyl groups and a benzothiadiazole unit, which may synergistically broaden the absorption spectra and suppress the dye aggregation, resulting in improved photocurrent and photovoltage.

关键词： Dye-sensitized solar cells,Sensitizers,Porphyrin,Bulky groups,Carbazole

更新于2025-11-19 16:56:42
Sensitized photochemical CO2 reduction by hetero-Pacman compounds linking a Re(I) tricarbonyl with a porphyrin unit

摘要： The hetero-Pacman architecture places two different metal coordination sites in close proximity, which can support efficient energy and/or electron transfer and allow for cooperative activation of small molecules. Herein, we present the synthesis of dyads consisting of a porphyrin unit as photosensitizer and a rhenium unit as catalytically active site, which are held together by the rigid xanthene backbone. Mononuclear [(NN)Re(CO)3(Cl)] complexes for CO2 reduction where NN represents a bidentate diimine ligand (e.g. bipyridine or phenanthroline) lack light absorption in the visible region, resulting in poor photocatalysis upon illumination with visible light. In order to improve their visible light absorption, we have focused on the incorporation of a strongly absorbing free base or zinc porphyrin unit. Resulting photocatalytic experiments showed a strong dependence of catalytic performance on both the type of photosensitizer and also the excitation wavelengths. Most notably, the intramolecular hetero-Pacman system containing a zinc porphyrin unit showed much better catalytic activity in the visible region (excitation wavelengths >450 nm) than the free base version, the corresponding mononuclear rhenium compound or an intermolecular system comprised of a 1:1 mixture of the mononuclear analogues.

关键词： photocatalysis,CO2 reduction,electron transfer,porphyrin,rhenium

更新于2025-11-19 16:56:35
Cationic porphyrins with large side arm substituents as resonance light scattering ratiometric probes for specific recognition of nucleic acid G-quadruplexes

摘要： Specific G-quadruplex-probing is crucial for both biological sciences and biosensing applications. Most reported probes are focused on fluorescent or colorimetric recognition of G-quadruplexes. Herein, for the first time, we reported a new specific G-quadruplex-probing technique—resonance light scattering (RLS)-based ratiometric recognition. To achieve the RLS probing of G-quadruplexes in the important physiological pH range of 7.4-6.0, four water soluble cationic porphyrin derivatives, including an unreported octa-cationic porphyrin, with large side arm substituents were synthesized and developed as RLS probes. These RLS probes were demonstrated to work well for ratiometric recognition of G-quadruplexes with high specificity against single- and double-stranded DNAs, including long double-stranded ones. The working mechanism was speculated to be based on the RLS signal changes caused by porphyrin protonation that was promoted by the end-stacking of porphyrins on G-quadruplexes. This work adds an important member in G-quadruplex probe family, thus providing a useful tool for studies on G-quadruplex-related events concerning G-quadruplex formation, destruction and changes in size, shape and aggregation. As a proof-of-concept example of applications, the RLS probes were demonstrated to work well for label-free and sequence-specific sensing of microRNA. This work also provides a simple and useful way for the preparation of cationic porphyrins with high charges.

关键词： G-quadruplex,ratiometric recognition,microRNA sensing,resonance light scattering,cationic porphyrin

更新于2025-11-19 16:56:35
POSS: A Morphology-Tuning Strategy to Improve the Sensitivity and Responsiveness of Dissolved Oxygen Sensor

摘要： Dissolved oxygen (DO) plays a crucial role in environment, food processing, and biotechnology. Although several physical-doping DO probes have been developed, a sensitive and reliable sensor for real-time and non-invasive DO detection in bioprocess is still challenging. Here we demonstrate a morphology-tuning strategy to improve the sensitivity and responsiveness of DO polymeric sensors (P(Pt-TPP-TFE-Ad) and P(Pt-TPP-TFE-POSS)) by decorating with the same platinum(II) porphyrins and different morphology-tunable moieties in supporting matrix. Experimental results manifest the sensitivity and response of sensors increase with size effect of the morphology-tunable moiety in due that the bulky morphology-tunable moiety facilitates the formation of interconnected and porous network that can promote oxygen permeability. Additionally, P(Pt-TPP-TFE-POSS) features excellent linear Stern-Volmer quenching, superior stability, and reversible response, thereby permitting the real-time and non-invasive quantification of DO during cephalosporin C fermentation. Our work offers an ideal tool for online sensing of DO in industrial and biological applications.

关键词： porphyrin,sensors,biofermentation,morphology-tuning,dissolved oxygen

更新于2025-11-19 16:56:35
A high-performance photocatalyst of ZnTCPP sensitized porous graphitic carbon nitride for antibiotic degradation under visible light irradiation

摘要： In this paper, a highly efficient photocatalyst of ZnTCPP sensitized g-C3N4 was successfully constructed via a facile thermal polycondensation method. The FT-IR and XRD data indicated that ZnTCPP molecules were successfully condensed on the surface of g-C3N4 through amide groups as the bridging units. The optimum 10%ZnTCPP/g-C3N4 composites exhibits excellent enhanced photocatalytic activity for decomposing both methylene blue (MB) and tetracycline (TC) under visible light with long-term reusability and elimination rates of 96% and 80.3%, respectively. The superior visible light photocatalytic performance was mainly attributed to the highly efficient separation of electron-hole pairs and the enhanced solar light utilization, as demonstrated by photoluminescence (PL), electrochemical impedance spectra (EIS), photocurrent responses, and UV-vis diffuse reflectance spectroscopy (DRS). The active species trapping and terephthalic acid (TA) fluorescence experiments indicated that ·OH was the dominating reactive oxidizing species for TC degradation. Furthermore, the possible photocatalytic degradation pathways for MB and TC have been proposed based on the UPLC-MS spectrometry. The excellent degradation efficiency of ZnTCPP/g-C3N4 reveals that it has great potential as photocatalysts for practical application to eliminate recalcitrant organic contaminants.

关键词： Zn meso-tetra (4-carboxyphenyl) porphyrin,Tetracycline,Photocatalyst,Semiconductors,g-C3N4

更新于2025-11-19 16:46:39
A pH-responsive zinc (II) metalated porphyrin for enhanced photodynamic/photothermal combined cancer therapy; 一种用于增强光动力/光热协同肿瘤治疗的酸性刺激响应锌(II)金属卟啉化合物;

摘要： The acidic tumor microenvironment is triggered by glycolysis in hypoxic condition, which can motivate the pH-responsive system to build certain triggers for efficiently tumor-targeted phototherapy. Additionally, the metalated porphyrin structures are widely studied in biomedical applications due to the favorable properties of high singlet oxygen quantum yield as well as strong fluorescence imaging ability. Herein, a pH-responsive zinc (II) metalated porphyrin (P-4) was designed and synthesized for amplifying cancer photodynamic/photothermal therapy with excellent fluorescence quantum yield (67.4%), superb singlet oxygen quantum yield (84.3%) and desired photothermal conversion efficiency (30.0%). In vitro, the self-assembled P-4 nanoparticles can specifically target to lysosome subcellular site and realize protonated process of dibutaneaminophenyl (DBAP) groups with high photo toxicity. Under single 660 nm laser illumination, the tumor can be ablated completely with no side effects in vivo. This work demonstrates that the pH-responsive P-4 nanoparticles provide a new avenue for highly efficient cancer combination therapy.

关键词： porphyrin,pH-responsive,NIR absorbance,photothermal therapy,photodynamic therapy

更新于2025-11-14 15:29:11
Study of the photoresponse of a titanium anode coated with solution-processed fullerene-containing metal porphyrin/phthalocyanine films

摘要： The present paper deals with the recent studies on the preparation of porphyrin-based donor-acceptor complexes capable of photoinduced electron transfer for solution-processed organic solar cells. Here the synthesis and chemical structure of (octakis(3,5-di-tert-butylphenoxy)phthalocyaninato) cobalt(II) (1) and (2,3,7,8,12,18-hexamethyl,13,17-diethyl,5-(2-pyridyl)porphinato) manganese(III) chloride (2) are performed and self-assembly in toluene solution of 1 and 1′-N-methyl-2′-(pyridin-4-yl)pyrrolidino[3′,4′:1,2][60]fullerene (PyC60) were discussed in more details. The structure of the obtained dyad 1-PyC60 is con?rmed by means of chemical thermodynamics/kinetics, UV–vis, IR, 1H NMR spectroscopy. Photoelectrochemical studies of the phthalocyanine-fullerene dyad and its precursors were carried out by voltammetry and amperometry methods. A comparative analysis of the photoelectrochemical characteristics obtained in this paper and these for recent described cobalt(II)/manganese(III) porphyrin/phthalocyanine-fullerene dyads are introduced from which ideas for the future design of high performance organic solar cells will be developed.

关键词： donor-acceptor complexes,organic solar cells,phthalocyanine,photoinduced electron transfer,fullerene,porphyrin

更新于2025-11-14 15:14:40
Improvement of the ON/OFF Switching Performance of a pH-Activatable Porphyrin Derivative by the Introduction of Phosphorus(V)

摘要： An activatable photosensitizer for singlet oxygen is of significance due to its potential applications for high tumor-specific photodynamic therapy and diagnosis. In this study, a pH-activatable system that enables the specific photosensitization of singlet oxygen at a low pH was developed based on the complexation of a porphyrin–aniline conjugate with phosphorus(V). As a result of complexation with phosphorus, the water solubility of the porphyrin–aniline conjugate was improved by 100 times. Furthermore, this complexation strongly suppressed the singlet-oxygen-generating activity of the porphyrin photosensitizer under basic conditions, and the quantum yield of the singlet oxygen photosensitization markedly increased under acidic conditions. Based on these improvements, an extremely high ON/OFF switching ratio of the quantum yield was obtained (>400 times).

关键词： pH activatable photosensitizer,ON/OFF switching,singlet oxygen,aniline,phosphorous porphyrin,protonation,fluorescence,acid

更新于2025-09-23 15:23:52
Voltage Stimulated Anion Binding of Metallo-Porphyrin Induced Crystalline 2D Nanoflakes

摘要： Voltage stimulated redox active materials received significant attention in the field of organic electronics and sensor technology. Consequently, such stimuli responsive materials triggered the formation of crystalline nanostructures facilitates the design of efficient smart devices hitherto unknown. Thus, we reported free base and metallo- tetratolylporphyrin linked ferrocene derivatives (H2TTP-Fc and ZnTTP-Fc) undergo distinct proton/anion binding mechanism in CHCl3 during bulk electrolysis at applied voltage of 1.4 V followed by nanospheres and crystalline 2D nanoflakes formation via MVD approach. Cyclic voltammetry and UV-Vis absorption studies of H2TTP-Fc and ZnTTP-Fc revealed the cation (H+)/anion (Cl-) binding affinity towards free ‘N’ atoms and Zn leads [H4TTP-Fc]+Cl- and H+[(Cl)ZnTTP-Fc]- thereby improvement in current and charge generation compared to initial state. SEM and TEM images revealed the nanospheres and 2D nanoflakes with average diameter of 50 – 200 nm and 0.2 - 1 μm. x-ray diffraction analysis suggest that protonated H2TTP-Fc aggregates exhibit amorphous nature, while H+[(Cl)ZnTTP-Fc]- revealed crystalline nature from layer-by-layer arrangement of nanoflakes assisted by π-π stacking and ion-dipole interactions. Hence, voltage responsive anion binding of metallo-porphyrins unique observation offer remarkable design of smart organic materials for sensors and biological applications.

关键词： anion binding,crystalline nanoflakes,metallo-porphyrin,self-assembly,bulk electrolysis

更新于2025-09-23 15:23:52
Facile Synthesis and Self-assembly of Zinc (2-Diethoxy-phosphorylethynyl)porphyrins

摘要： The synthesis of zinc (2-diethoxyphosphorylethynyl)porphyrins and their self-organization in solid state and in solution are reported. Copper-cocatalyzed Sonogashira reaction of bromoporphyrins with diethyl ethynylphosphonate was used to prepare meso-substituted derivatives Zn4 and Zn5 bearing one or two ethynylphosphonate substituents at the macrocycle. In contrast, copper-free Sonogashira coupling of 2-bromoporphyrin with diethyl ethynylphosphonate is more convenient to prepare porphyrin Zn6 bearing this substituent at the b-pyrrolic position of the macrocycle. The structure of complexes Zn4a.C7H8, Zn4a.CHCl3, Zn4c and Zn5b.CH2Cl2 in crystals were elucidated by X-ray diffraction analysis. The supramolecular self-assembly through weak coordinative binding of the phosphoryl group of one porphyrin molecule to the zinc(II) ion located in the center of another macrocyclic cavity is observed in all crystals. However, Zn(II)-porphyrinates Zn4a and Zn5b exist in the solid state as mutually coordinated dimers while complex Zn4c displays a 1D polymer structure. In all dimer complexes, neighboring porphyrin rings are spatially separated, with Zn–O and P=O bond distances being similar, while the interplanar porphyrin distance is variable to depend on weak intermolecular interactions in the crystals. The self-organization of (phosphorylethynyl)porphyrins is also observed in weakly polar chloroform and detectable by NMR and UV-vis spectroscopies. The mutually coordinated dimer of electron-deficient porphyrin Zn5b was observed in 5.x.10-3 M chloroform solution even at room temperature. Kinetic lability of this supramolecular complex was proven by NMR spectroscopy. The associates of more electron-donating porphyrins Zn4a and Zn4c are less stable and self-assembled dimers become the predominant species in 5.x.10-3 M chloroform solution only below 225 K. The self-assembly of porphyrin Zn4a and Zn5b in more diluted solutions (up to 10-6 M) was also investigated by UV-vis spectroscopy.

关键词： self-organization,phosphonate,porphyrin,catalysis,acetylene linker

更新于2025-09-23 15:23:52

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