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FTO-TiO2 photoelectrocatalytic degradation of triphenyltin chloride coupled to photoelectro-Fenton: A mechanistic study
摘要： A powerful, simple and stable transparent photoanode based on TiO2 nanoparticles deposited on fluorine-doped tin oxide (FTO) was synthesized for the photoelectrocatalytic degradation of the organometallic pollutant triphenyltin chloride (TPTCl). Contrasting with most of the works on photoelectrocatalysis (PEC), FTO-TiO2 was found to be an excellent anode material for the degradation/mineralization of organic pollutants at high anodic potentials through the formation of electrochemically-induced hVB+ (dark PEC), showing a similar behavior as the so-called 'non-active' anodes like the powerful boron doped diamond electrode (BDD). The electrocatalytic efficiency was enhanced by the photoexcitation of TiO2 under UV light (PEC) and by coupling with photoelectro-Fenton (PEC-PEF): this resulted in complete degradation of TPTCl in 15 min (kapp = 0.274 min-1) and total mineralization in 2 h. The mechanisms governing the photoelectrocatalytic processes are investigated in detail by means of electrochemical measurements and chemical probes, and a mineralization pathway for TPTCl is proposed.
关键词： photoelectro-Fenton,photoelectrocatalysis,fluorine-doped tin oxide,organotin pollutants,Dark PEC
更新于2025-09-23 15:21:01
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Thermal degradation behavior of self-assembled monolayer surfactant on silicon substrate
摘要： In nanoimprint lithography, a release agent on the mold surface is usually necessary for easy demolding between the mold and the imprinted (thermal) resist. In this work, the thermal stability of 1H,1H,2H,2H-perfluorodecyltrichlorosilane (FDTS) monolayers is studied using x-ray photoelectron spectroscopy. The FDTS monolayers are deposited on Si (100) substrates via vapor phase reactions. Significant fluorine desorption of the monolayers is observed for samples annealed at 250 and 300 °C in air. The fluorine coverage decreases as a function of annealing time at a given annealing temperature. The desorption is proposed to be dependent on the monolayer packing details and may be influenced by the intermolecular heat transfer. Removal of the CF3 groups is found to be faster than that of the CF2 group as evidenced by the CF2/CF3 peak area ratios that increase with the annealing time. Sessile drop water contact angle and fluorine coverage evolution results show that the estimated useful coating lifetime is 180 min when the samples are annealed at 300 °C and ～560 min when annealed at 250 °C. The peak position of the binding energy of the F 1s spectral line is related to the monolayer fluorine coverage and it may be a result of the interactions between the molecular chain and the negatively charged silicon substrate. Furthermore, nearly no chain desorption is detected for samples annealed in an inert environment, which may be attributed to the elimination of reactive oxygen and moisture molecules. The thermal degradation behaviors in ambient and inert atmosphere provide useful information for designing a nanoimprint process for the commercial manufacturing of polymeric microstructure and nanostructure.
关键词： fluorine desorption,x-ray photoelectron spectroscopy,thermal stability,FDTS monolayers,nanoimprint lithography
更新于2025-09-23 15:21:01
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Cadmium Sulfide Quantum-Dot-Photocatalyzed Cascade Cyclization of Functionalized Difluoromethyl Chlorides with Unactivated Olefins
摘要： A cadmium sulfide quantum-dot-photocatalyzed C(sp3)?Cl bond cleavage of ethyl chlorodifluoroacetate and cascade cyclization with unactivated olefins is described herein. This reaction provides a cost-efficient method for synthesizing a wide range of CF2-containing azaheterocycles from functionalized difluoromethyl chlorides. Furthermore, the results of a preliminary anti-proliferative activity study indicate an in vitro anti-proliferative activity superior to that of doxorubicin with IC50 values of 1.140 μM on triple negative breast cancer (MDA-MB-231) and 2.129 μM on lung (A549) carcinoma cells.
关键词： anti-proliferative activity,photocatalysis,C(sp3)-Cl activation,fluorine,cadmium sulfide quantum dots
更新于2025-09-23 15:21:01
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Effects of CF<sub>4</sub> Surface Etching on 4H-SiC MOS Capacitors
摘要： Effects of CF4 etching on 4H-SiC MOS capacitor were investigated. Fluorine atoms were introduced to surface of 4H-SiC using CF4 dry etching process as a surface treatment, and 4H-SiC MOS capacitors with dry-oxide were fabricated with this treatment. As a result, the breakdown electric field of the MOS capacitors was increased and variation of the characteristics became lower than that of MOS capacitor without this treatment.
关键词： MOS Capacitor,Oxide/4H-SiC Interface,Dry Etching,Fluorine
更新于2025-09-23 15:21:01
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Thermally Durable Nonfullerene Acceptor with Nonplanar Conjugated Backbone for Higha??Performance Organic Solar Cells
摘要： A nonfullerene acceptor (NFA) with acceptor–donor–acceptor (A–D–A) architecture, i-IEICO-2F, based on 4,9-dihydro-s-indaceno[1,2-b:5,6-b′]dithiophene as an electron-donating core and 2-(6-fluoro-2,3-dihydro-3-oxo-1H-inden-1-ylidene)-propanedinitrile as electron-withdrawing end groups, is designed and synthesized. i-IEICO-2F has a twist structure in the main conjugated chain, which causes blueshifted absorption and leads to harmonious absorption with a high bandgap donor. The bandgap of i-IEICO-2F compliments the bandgap of suitable wide bandgap donor polymers such as J52, leading to complete light absorption throughout the visible spectrum. Devices based on i-IEICO-2F exhibit optimized photovoltaic performance including an open-circuit voltage of 0.93 V, a short-circuit current density of 16.61 mA cm?2, and a fill factor of 73%, and result in a power conversion efficiency (PCE) of 11.28%. The i-IEICO-2F-based devices reach PCEs of >11% without using any additives or post-treatments. Devices are found to be thermally stable and maintain 44% of their initial PCE after 184.5 h of continuous thermal annealing (TA) treatment at 150 °C. Based on UV, atomic force microscopy (AFM), and grazing incidence wide angle X-ray scattering (GIWAXS) results, i-IEICO-2F devices show almost identical morphology and molecular orientation throughout the TA treatment and excellent stability compared to other IEICO derivatives.
关键词： twist structure,solar cells,nonfullerene acceptors,synthesis,fluorine
更新于2025-09-23 15:19:57
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Modular medical imaging agents based on azidea??alkyne Huisgen cycloadditions: Synthesis and prea??clinical evaluation of 18Fa??labeled PSMAa??tracers for prostate cancer imaging.
摘要： The seminal contribution of Rolf Huisgen to develop the [3+2]-cycloaddition of 1,3-dipolar compounds, its azide-alkyne variant has established itself as the key step in numerous organic syntheses and bioorthogonal processes in materials science and chemical biology. In the present study, the copper(I)-catalyzed azide-alkyne cycloaddition was applied for the development of a modular molecular platform for medical imaging of the prostate specific membrane antigen (PSMA), using positron emission tomography. This process is shown from molecular design, through synthesis automation and in vitro studies, all the way to preclinical in vivo evaluation of fluorine-18– labeled PSMA-targeting ‘F-PSMA-MIC’ radiotracers (t? = 109.7 min). Preclinical data indicate that the modular PSMA-scaffold has similar binding affinity and imaging properties to the clinically used [68Ga]PSMA-11. Furthermore, we demonstrated that targeting the arene-binding in PSMA, facilitated through the [3+2]-cycloaddition, can improve binding affinity, which was rationalized by molecular modeling. The here presented PSMA-binding scaffold potentially facilitates easy coupling to other medical imaging moieties, enabling future developments of new modular imaging agents.
关键词： prostate specific membrane antigen,positron emission tomography,fluorine-18,azide-alkyne Huisgen cycloaddition,modular imaging agents
更新于2025-09-23 15:19:57
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Neon plasma for effective ionisation of oxygen and fluorine in pulsed glow discharge – high ionisation energy elements quantification in potassium titanyl phosphate single crystals
摘要： Neon glow discharge was tested for the direct analysis of solid dielectric materials by pulsed glow discharge time-of-flight mass spectrometry with an emphasis on the elements with high ionisation energy. The findings for neon were compared to conventional argon glow discharge. Fluorine doped potassium titanyl phosphate (KTP) single crystals were used for analysis. The following parameters were optimised: repelling pulse delay, discharge duration and voltage and pressure in the discharge cell. Relative sensitivity factors were used for quantification; titanium was used for normalisation. Similar to argon glow discharge, the most effective mechanism for fluorine and oxygen ionisation was found to be attributed to high-energy electrons under short repelling pulse delays. Penning ionisation of oxygen in neon glow discharge was found to be less efficient. Overall, the use of neon significantly benefited fluorine and oxygen determination; the limits of detection for oxygen (0.0005 mass %) and fluorine (0.0002 mass %) decreased several times compared to argon glow discharge (0.001 and 0.01 mass %, respectively) as a result of more effective ionisation. The improvement was especially pronounced for fluorine, due to the alleviation of plasma-based interferences. However, for other KTP constituents – potassium, phosphorus and titanium – the analytical performance was expectedly lower, due to the lower sputtering rates in neon glow discharge. The limits of detection for potassium and phosphorus were significantly increased, being 0.008 mass % and 0.01 mass %, respectively. Notably, the performance for non-high ionisation energy elements was adequate for their single-run quantification along with oxygen and fluorine at non-trace levels. Thus, the use of neon as discharge medium for pulsed glow discharge mass spectrometry is clearly justified for the determination of high ionisation energy elements such as oxygen and fluorine in non-conducting matrices.
关键词： oxygen,mass spectrometry,neon,direct determination,fluorine,pulsed glow discharge
更新于2025-09-19 17:15:36
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Effect of Sodium and Fluorine Co-Doping on the Properties of Fluorite-Like Rare-Earth Molybdates of Nd5Mo3O16 type
摘要： Fluorite-like oxyfluorides NaLn4Mo3O15F (Ln = La, Pr, Nd), which relate to the Nd5Mo3O16 structural type, were obtained by solid-phase synthesis in the air. Codoping of the Nd5Mo3O16+δ family with sodium and fluorine led to the appearance of a piezoelectric effect and a reversible phase transition in oxyfluorides, accompanied by a jump in the conductivity and an anomaly of the permittivity of the compounds. In contrast to Nd5Mo3O16+δ, which possess mixed oxide-ion/electronic interstitial conductivity, the NaLn4Mo3O15F compounds can have oxygen conductivity of vacancy type. The highest conductivity offered by these materials is 3.2×10–2 S/cm at 700 °C. NaLn4Mo3O15F compounds were found to be hygroscopic and can be considered as potential proton conductors.
关键词： rare earths,sodium,phase transitions,fluorine,solid-phase synthesis
更新于2025-09-19 17:15:36
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Multi-functional MnO <sub/>2</sub> nanomaterials for photo-activated applications by a plasma-assisted fabrication route
摘要： Supported MnO2-based nanomaterials were fabricated on fluorine-doped tin oxide substrates using plasma enhanced-chemical vapor deposition (PE-CVD) between 100 °C and 400 °C, starting from a fluorinated Mn(II) diamine diketonate precursor. Growth experiments yielded β-MnO2 with a hierarchical morphology tuneable from dendritic structures to quasi-1D nanosystems as a function of growth temperature, whose variation also enabled a concomitant tailoring of the system fluorine content, and of the optical absorption and band gap. Preliminary photocatalytic tests were aimed at the investigation of photoinduced hydrophilic (PH) and solid phase photocatalytic (PC) performances of the present nanomaterials, as well as at the photodegradation of Plasmocorinth B azo-dye aqueous solutions. The obtained findings highlighted an attractive system photoactivity even under visible light, finely tailored by fluorine content, morphological organization and optical properties of the prepared nanostructures. The results indicate that the synthesized MnO2 nanosystems have potential applications as advanced smart materials for anti-fogging/self-cleaning end uses and water purification.
关键词： anti-fogging,photoactivated applications,fluorine doping,photocatalysis,water purification,self-cleaning,plasma-assisted fabrication,MnO2 nanomaterials
更新于2025-09-19 17:15:36
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Identification, Characterization, and Optimization of Integrin αvβ6-Targeting Peptides from a One-Bead One-Compound (OBOC) Library: Towards the Development of Positron Emission Tomography (PET) Imaging Agents
摘要： The current translation of peptides identified through the one-bead one-compound (OBOC) technology into positron emission tomography (PET) imaging agents is a slow process, with a major delay between ligand identification and subsequent lead optimization. This work aims to streamline the development process of 18F-peptide based PET imaging agents to target the integrin αvβ6. By directly identify αvβ6–targeting peptides from a 9-mer 4-fluorobenzoyl peptide library using the on-bead two-color (OBTC) cell-screening assay, a total of 185 peptide beads were identified and 5 beads sequenced for further evaluation. The lead peptide 1 (VGDLTYLKK(FB), IC50 = 0.45 ± 0.06 μM, 25% stable in serum at 1 h) was further modified at the N-, C-, and bi-termini. C-terminal PEGylation increased the metabolic stability (>95% stable), but decreased binding affinity (IC50 = 3.7 ± 1 μM) was noted. C-terminal extension (1i, VGDLTYLKK(FB)KVART) significantly increased binding affinity for integrin αvβ6 (IC50 = 0.021 ± 0.002 μM), binding selectivity for αvβ6-expressing cells (3.1 ± 0.8:1), and the serum stability (>99% stable). Our results demonstrate the challenges in optimizing OBOC-derived peptides, indicate both termini of 1 are sensitive to modifications, and show that further modification of 1 is necessary to demonstrate utility as an 18F-peptide imaging agent.
关键词： Fluorine-18,integrin αvβ6,affinity,one-bead one-compound (OBOC),library screening,solid-phase radiolabeling,positron emission tomography (PET),selectivity
更新于2025-09-19 17:15:36