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Adsorption and photocatalytic oxidation of ibuprofen using nanocomposites of TiO2 nanofibers combined with BN nanosheets: Degradation products and mechanisms
摘要： This study investigated the adsorption and photocatalytic activity of TiO2-boron nitride (BN) nanocomposites for the removal of contaminants of emerging concern in water using ibuprofen as a model compound. TiO2 nanofibers wrapped by BN nanosheets were synthesized by electrospinning method. Characterization of the nanocomposite photocatalysts indicated the BN nanosheets improved the light absorbance and reduced the recombination of the photoexcited charge carriers (e- and h+). The photocatalytic oxidation products and mechanisms of ibuprofen by the TiO2-BN catalysts were elucidated using a multiple analysis approach by high performance liquid chromatography, ultraviolet absorbance, dissolved organic carbon, fluorescence excitation-emission matrices, and electrospray ionization–liquid chromatography–tandem mass spectrometry. The experimental results revealed that the photocatalytic oxidation by the TiO2-BN nanocomposites is a multi-step process and the interactions between ibuprofen molecules and the TiO2-BN nanocomposites govern the adsorption process. The increasing BN nanosheet content in the TiO2 nanofibers facilitated the breakdown of ibuprofen degradation intermediates (hydroxyibuprofen, carboxyibuprofen, and oxypropyl ibuprofen). Kinetic modeling indicated both adsorption and photocatalytic oxidation of ibuprofen by the TiO2-BN nanocomposites followed the first-order kinetic model. The photocatalytic oxidation rate increased with the increasing BN content in the nanocomposite catalysts, which was attributed to the enhanced light absorption capacity and the separation efficiency of the photoexcited electron (e-)-hole (h+) pairs. Multiple photocatalytic cycles were conducted to investigate the reusability and regeneration of the nanofibers for ibuprofen degradation.
关键词： adsorption,titanium dioxide boron-nitride nanocomposites,photocatalytic degradation mechanisms,degradation intermediates,photocatalytic oxidation
更新于2025-09-23 15:23:52
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A comparison of water photo-oxidation and photo-reduction using photoelectrodes surface-modified by deposition of co-catalysts: Insights from photo-electrochemical impedance spectroscopy
摘要： The purpose of this research paper is to highlight the similarities in the kinetic treatment between water photo-oxidation into molecular oxygen and water photo-reduction into molecular hydrogen, using photoelectrodes surface modified by deposition of co-catalysts. Photo-anodes made of TiO2 nanorods surface-covered by crystals of cobalt Zeolitic Imidazolate Framework (ZIF-67), and photo-cathodes made of Rh:SrTiO3 particles surface-modified by adsorption of molecules of trisdioximate hexa-chlorine cobalt (II) clathrochelate (Co(Cl2Gm)3(BCH3)2), have been prepared and used for water photo-oxidation and photo-reduction experiments, respectively. Both photoelectrodes have been characterized by SEM and cyclic voltammetry under illumination conditions. Charge transfer mechanisms have been investigated by photo-electrochemical impedance spectroscopy (PEIS). It is shown that for both systems, the presence of a co-catalyst increases the charge transfer kinetics, and that the trapping resistance is larger than the charge transfer resistance, at any operating potential.
关键词： Water photo-oxidation,Titanium dioxide nanorods,Strontium titanate,Water photo-reduction,ZIF-67 MOF
更新于2025-09-23 15:23:52
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Heat-Assisted Photoacidic Oxidation Method for Tailoring the Surface Chemistry of Polymer Dielectrics for Low-Power Organic Soft Electronics
摘要： The use in low-power soft electronics of the appropriate insulating polymer materials with a high dielectric constant (k) is considered a practical alternative to that of inorganic dielectric materials, which are brittle and have high processing temperatures. However, the polar surfaces of typical high-k polymer insulators are problematic. Further, it is a huge challenge to control their surface properties without damage because of their soft and chemically fragile nature. Here, a heat-assisted photoacidic oxidation method that can be used to effectively oxidize the outermost surfaces of high-k rubbery polymer films without degradation is presented. The oxidized surfaces prepared with the developed method contain large numbers of hydroxyl groups that enable the subsequent growth of dense and ordered self-assembled monolayers (SAMs) consisting of organosilanes. The whole process modifies the surface characteristics of polymer dielectrics effectively. The mechanisms of the oxidation of polymer surfaces and the subsequent SAM growth process are investigated. The resulting surface-tailored rubbery dielectrics exhibit superior electrical characteristics when used in organic transistors. These results demonstrate that this method can be used to realize practical soft organic electronics based on high-k polymer dielectrics.
关键词： self-assembled monolayers,organic semiconductors,polymer gate dielectric,polymer oxidation,surface chemistry
更新于2025-09-23 15:23:52
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Manipulation of Charge Transport by Metallic V <sub/>13</sub> O <sub/>16</sub> Decorated on Bismuth Vanadate Photoelectrochemical Catalyst
摘要： Conductive metal oxides represent a new category of functional material with vital importance for many modern applications. The present work introduces a new conductive metal oxide V13O16, which is synthesized via a simplified photoelectrochemical procedure and decorated onto the semiconducting photocatalyst BiVO4 in controlled mass percentages ranging from 25% to 37%. Owing to its excellent conductivity and good compatibility with oxide materials, the metallic V13O16-decorated BiVO4 hybrid catalyst shows a high photocurrent density of 2.2 ± 0.2 mA cm?2 at 1.23 V versus reversible hydrogen electrode (RHE). Both experimental characterization and density functional theory calculations indicate that the superior photocurrent derives from enhanced charge separation and transfer, resulting from ohmic contact at the interface of mixed phases and superior electrical conductivity from V13O16. A Co–Pi coating on BiVO4–V13O16 further increases the photocurrent to 5.0 ± 0.5 mA cm?2 at 1.23 V versus RHE, which is among the highest reported for BiVO4-based photoelectrodes. Surface photovoltage and transient photocurrent measurements suggest a charge-transfer model in which photocurrents are enhanced by improved surface passivation, although the barrier at the Co–Pi/electrolyte interface limits the charge transfer.
关键词： charge transport,bismuth vanadate,Co–Pi passivation,water oxidation,metallic V13O16
更新于2025-09-23 15:23:52
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TiO2/Schwertmannite nanocomposites as superior co-catalysts in heterogeneous photo-Fenton process
摘要： The heterogeneous photo-Fenton reaction is an effective technique in combating organic contaminants for both soil and water remediation, and extensive studies have focused on enhancing its efficiency and reducing its costs. In this work, we developed novel photo-Fenton catalysts by simply milling commercially available TiO2 (P25) with Schwertmannite (Sh), a natural iron-oxyhydroxysulfate nanomineral. We expect that the photo-generated electrons from TiO2 could continuously migrate to Sh, which then could enhance the separation of electron-hole pairs on TiO2 and accelerate the reduction of Fe(III) to Fe(II) on Sh, leading to high degradation efficiency of the target organic contaminants. SEM and TEM results showed the distribution of TiO2 on Sh surface for the nanocomposites (TiO2/Sh). Under simulated sunlight irradiation, the much higher content of Fe(II) was determined on TiO2/Sh than on Sh via a common method in the iron ore, and the consumption of H2O2 and the production of ?OH were more significant in the TiO2/Sh system than those in the TiO2 and Sh systems. These results well support our hypothesis that the photo-generated electrons could migrate from TiO2 to Sh on the composites, and can also explain the much higher degradation efficiency of Rhodamine B (RhB) in the TiO2/Sh system. Besides, TiO2/Sh had lower Fe dissolution as compared with Sh, and retained high catalytic stability after four repeated cycles. Above merits of the TiO2/Sh composites, in combining with their simple synthesis method and low-cost property, indicated that they should have promising applications as heterogeneous photo-Fenton catalysts.
关键词： Advanced oxidation,Photo-Fenton reaction,Semiconductor,Schwertmannite
更新于2025-09-23 15:23:52
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Introduction of oxygen vacancies into hematite in local reducing atmosphere for solar water oxidation
摘要： Sn Doping and creation of oxygen vacancies have been adopted universally to overcome the poor electric conductivity and unfavorable hole diffusion length of α-Fe2O3 photoanodes. Generally, Sn doping is realized via longitudinal migration of tin element from FTO (fluorine-doped tin oxide) substrates into α-Fe2O3 at high temperature. To introduce oxygen vacancies along with Sn into hematite for further promoting its electric conductivity, we have created a local reducing atmosphere via partial oxidation of graphite while doping hematite with Sn. The donor density of the resultant Fe2O3 photoanode annealed on graphite (G-Fe2O3) at 770 °C for 20 min is increased to ～1.7 times that of the counterpart annealed on SiO2 powders (S-Fe2O3), indicating that the electric conductivity of hematite is improved after introduction of oxygen vacancies. Moreover, oxygen vacancies have been demonstrated to significantly reduce the charge transfer resistance of Sn doped hematite. Consequently, the photocurrent density of G-Fe2O3 is enhanced remarkably (～70%) compared with S-Fe2O3. However, the improvement in photocurrent density due to oxygen vacancies becomes less significant when more Sn is doped into hematite. The strategy for creation of oxygen vacancies reported here can be extended to other photoanodes for better understanding the effect of oxygen vacancies on PEC performance.
关键词： Oxygen vacancies,Sn doping,Solar water oxidation,Hematite
更新于2025-09-23 15:23:52
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Enhanced solar light driven activity of p-n heterojunction for water oxidation induced by deposition of Cu2O on Bi2O3 microplates
摘要： As an important half reaction in solar-driven water splitting, it is more challenging to develop low-cost and highly efficient photocatalysts for water oxidation. The enhancement of sunlight harvesting and inhibition of charge-carrier recombination are keys to fabricating efficient semiconductor-based photocatalysts for energy conversion from solar light to chemicals. Herein, we reported highly dispersive Cu2O/Bi2O3 composites prepared by a facile and benign synthetic route, where n-type Bi2O3 microplates and nano-sized p-type Cu2O were coupled together to construct heterojunctions to improve the transportation efficiency of photoinduced charge carriers, benefited from the intimate interactions at the interfaces between Bi2O3 and Cu2O. The electrochemical properties of charge-transportation and population of charge carriers were investigated in the heterojunctions. The hybrid materials exhibit both enhanced photocatalytic performances in water oxidation and photodegradation of dyes compared with sole Bi2O3 or Cu2O under artificial solar light irradiation. The initial O2 evolution rate of the heterojunction system is 1.4- and 8-fold higher than the pure Bi2O3 and Cu2O, respectively. This study provides new protocols for synthesizing novel hybrid materials with insights into heterojunction-based photocatalysis for green energy production and wastewater purification.
关键词： Nanocomposite,Water oxidation,Photocatalysis,Heterojunction,Wastewater purification
更新于2025-09-23 15:23:52
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CO and H2 activation over g-ZnO layers and w-ZnO(0001)
摘要： Graphene-like ZnO (g-ZnO) nanostructures (NSs) and thin films were prepared on Au(111) and their reactivities towards CO and H2 were compared with that of wurtzite ZnO (w-ZnO) (0001) single crystal. The interaction and reaction between CO/H2 and the different types of ZnO surfaces were studied using near-ambient-pressure scanning tunneling microscopy (NAP-STM), X-ray photoelectron spectroscopy (XPS) and Density functional theory (DFT) calculations. The reactivity of the w-ZnO(0001) surface towards CO and H2 was found to be more prominent than those on the surfaces of g-ZnO/Au(111). CO oxidation took place primarily at the edge sites of w-ZnO(0001) and the interface between g-ZnO NSs and Au(111), while g-ZnO thin films on Au(111) appeared inert at below 600 K. Similarly, the w-ZnO(0001) surface could dissociate H2 at 300 K, accompanied by a substantial surface reconstruction, while g-ZnO on Au(111) appeared inert for H2 activation at 300 K. DFT calculations showed that the reactivities of ZnO surfaces towards CO could be related to the formation energy of oxygen vacancy (EOvf), which could be related to the charge transfer to lattice oxygen atoms or surface polarity.
关键词： CO oxidation,NAP-STM,ZnO,XPS,surface polarity,oxygen vacancy
更新于2025-09-23 15:23:52
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Photocatalytic removal of phenanthrene and algae by a novel Ca-Ag3PO4 composite under visible light: Reactivity and coexisting effect
摘要： In this study, the feasibility of a novel Ca-Ag3PO4 composite with visible light irradiation for the phenanthrene (PHE) degradation and algae inactivation in artificial seawater was firstly investigated. The experimental findings revealed that Ag3PO4 phase was sucessfully formed on the Ca-based material, and the presence of Ca-based material could effectively keep Ag3PO4 particles stable. An excellent performance on PHE degradation or algae inactivation was observed from Ca-Ag3PO4 composite under visible light irradiation. The degradation of PHE or inactivation of algae not only could be efficiently achieved in the single mode, but also could be successfully achieved in the coexisting mode. Above 96 % of PHE and algae were simultaneously removed within 12 h in the Ca-Ag3PO4/visible light system. It was further observed that the degradation of PHE and/or inactivation of algae increased with the increase of Ca-Ag3PO4 dosage. HO? was the primary radical responsible for PHE degradation, whereas HO? and Ag+ released from Ca-Ag3PO4 mainly contributed to the algae inactivation. A possible mechanism involving the catalytic removal of PHE and algae by Ca-Ag3PO4 under visible light irradiation was proposed. This study provides helpful guide for the simultaneous removal of various pollutants in real seawater.
关键词： Ag3PO4,Algae,Photocatalytic,Advanced oxidation processes (AOPs),Visible light,Phenanthrene (PHE)
更新于2025-09-23 15:23:52
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Experimental data on the degradation of caffeine by photo-electro-fenton using BDD electrodes at pilot plant
摘要： Emerging contaminants (EC) are an imminent risk due to potential toxicity to aquatic ecosystems and human beings. This type of contaminants is found in low concentrations and usually present incomplete or inefficient removal by conventional treatments, which entail its permanence and constant increase. Advanced Oxidation Processes (AOP) are an alternative for the elimination of dangerous and resistant substances in wastewater. So, this research evaluates the caffeine degradation in aqueous solution by AOP, such as: Fenton, Electro-Oxidation (EO) with boron doped diamond (BDD) electrodes, Electro-Fenton (EF) and Photo-Electro-Fenton (PEF). The influences of pH, concentration of the supporting electrolyte and specific electric charge were investigated using a Taguchi's factorial design, which allowed to identify the contribution of each variable in the process. The data obtained in this work can be useful for scaling process and cost analysis because it provide the information at pilot plant scale.
关键词： Chemical engineering,Taguchi design,BDD electrodes,Advanced oxidation process,Caffeine degradation
更新于2025-09-23 15:23:52