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Stoichiometric and non-stoichiometric tungsten doping effect in bismuth vanadate based photoactive material for photoelectrochemical water splitting
摘要： In photoelectrochemical (PEC) water splitting, BiVO4 has attracted attention due to its favorable band gap but it suffers low PEC performance due to poor conductivity. The vast majority of publications on this system has examined doping of stoichiometric composition of tungsten (W) on this system to increase bulk and interfacial conductivity while managing the contaminant generation of crystallographic defects and recombination sites. In this paper, a deep investigation was carried out to examine the effect of non-stoichiometric W doping in BiVO4 system. Stoichiometric and non-stoichiometric W-doped monoclinic BiVO4 (i.e. Bi1-(xtd)V1-xWxtdO4; BiV1-xWxtdO4 and BiV1-yWyO4; x ? 0.008; y ? 0.03 and d ? 0.005) were prepared using a facile dip coating technique. The stoichiometric composition contains charge balanced Bi, V and W atoms whereas non-stoichiometric compositions contain excess Bi and excess Bi and W. The non-stoichiometric composition BiV1-xWxtdO4 has shown better photoelectrochemical water splitting performance with respect to other compositions at 1.23 V vs RHE, under one sun illumination of electrode. The XRD and XPS results shows that non-stoichiometric doping with excess Bi or with excess Bi and W can possibly create an environment where V5t ions are substitutional replaced by W6t ions without generating other defects. But there was no signi?cant difference in band gap of different compositional samples observed. Further electrochemical impedance technique was used to analyze change in bulk and surface charge mobility with W-doping in BiVO4. The electrochemical impedance analysis showed the presence of low interfacial resistance, lower charge transfer resistance and high charge donor/surface state density for non-stoichiometric composition BiV1-xWxtdO4 electrode. It is evident from and cyclic voltammetry that the addition of excess Bi and W from its stoichiometric quantity ef?ciently suppressed the formation of hole-electron pair recombination sites. The electrochemical analytical results lead us to believe that the particular non-stoichiometric composition of BiV1-xWxtdO4 can signi?cantly lower trap sites and enhances kinetics of charge transfer, leading to the better photoelectrochemical water splitting performance.
关键词： Oxygen evolution,Photoelectrochemical cell,Water splitting,Bismuth vanadate,Tungsten doping
更新于2025-09-23 15:23:52
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Novel design of photocatalyst coaxial ferromagnetic core and semiconducting shell microwire architecture
摘要： We report a novel design of coaxial core-shell magnetic-semiconductor microwire, as a catalyst under sunlight irradiation. The nano/micro hierarchical architecture-like device is comprised of a coaxial core-shell microwire where the core is the ferromagnetic Fe metal and the shell is formed by a semiconducting hematite layer. The fabrication process of our substrate-free device is simply based on controlled thermal oxidation process revealing a simple and low-cost method. The hematite outer microlayer has a mesoporous structure decorated with nanowires. The ferromagnetic and metallic core assume fundamental importance as to mechanical stability, collect the generated photoelectrons, and to be removed back from the dye solution by a magnetic field gradient or simply a magnet. This nano/micro device has exhibited photocatalytic activity to degrade the methylene blue dye under simulated sunlight irradiation. Additionally, the coaxial magnetic/semiconducting can also be designed as a photoanode to drive water oxidation reaction. The coaxial magnetic/semiconducting photoanode response has shown good chemical stability and long activity under simulated sunlight radiation. In fact, this designed architecture gives novel perspective in the development of substrate free photocatalyst.
关键词： Photoelectrochemical performance,Hematite photoanodes,Photodegradation,Micro/nano architecture,Core-shell microstructures,Thermal oxidation
更新于2025-09-23 15:23:52
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Synthesis and annealing process of ultra-large SnS nanosheets for FTO/SnS/CdS/Pt photocathode
摘要： SnS has been widely used in photoelectric devices due to its special band gap of 1.2–1.5 eV. Here, we reported on the fabrication of SnS nanosheets and the effect of synthesis condition together with heat treatment on its physical properties. The obtained band gap of the SnS nanosheets is in the rage of 1.37–1.41 eV. It was found that the photo-current density of a thin film comprised of SnS nanosheets could be enhanced significantly by annealing treatment. The maximum photo-current density of the stack structure of FTO/SnS/CdS/Pt was high as 389.5 μA cm-2, rendering its potential application in high efficiency solar hydrogen production.
关键词： SnS nanosheets,Water splitting,Photoelectrochemical properties
更新于2025-09-23 15:23:52
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Modulated anodization synthesis of Sn-doped iron oxide with enhanced solar water splitting performance
摘要： Modulated anodization synthesis is introduced here for the fabrication of porous Sn-doped iron oxide. Continuous square-wave modulation consisting of highly positive (+50 to +80 V range) and slightly negative potentials (-2 to -10 V range) at 100 Hz allowed the etching anodization of the metallic Fe foil and incorporation of Sn-dopant from the fluoride anion-containing electrolyte, respectively. Compared with the undoped iron oxide, the surface-enriched Sn-dopant (in the form of Sn4+) alleviates the trapping and recombination of surface holes, while enhancing the hole transfer at the surface states. As such, the overpotential for photoelectrochemical (PEC) water oxidation was reduced by 110 mV and photocurrent density doubled. The incorporation of Co-Pi co-catalyst further improved the hole transfer efficiency, resulting in further reduction in overpotential by another 330 mV with respect to the bare Sn-doped iron oxide and significant improvement in photocurrent density at potentials below +1.23 V vs. reversible hydrogen electrode. Lastly, the iron oxide electrodes exhibit highly stable PEC water oxidation with no degradation in activity throughout the 10 h assessment under simulated solar irradiation and Faradaic efficiency of 90%. We envisage that the modulated anodization technique can be conveniently incorporated for a wide range of other dopants in search of efficient solar water splitting electrodes.
关键词： Doping,Hematite,Hydrogen,Photoelectrochemical water splitting,Charge transport
更新于2025-09-23 15:23:52
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A dual TiO2/Ti-stainless steel anode for the degradation of orange G in a coupling photoelectrochemical and photo-electro-Fenton system
摘要： A dual-anode consists of stainless steel and TiO2/Ti electrodes is used to study the kinetics of the degradation of hazardous chemicals exemplified by azo dye orange G (OG) using a coupling photoelectrochemical catalytic and photoelectro-Fenton (PEC/PEF) system. Concurrent generation of hydroxyl radicals on the TiO2/Ti photocatalyst and in-situ generation of Fenton reagents on the stainless steel electrode greatly enhances the performance of the PEC/PEF electrodes over that of the PEC and the PEF alone process. The efficiency of the PEC/PEF process is a function of Fe2+ and H2O2 concentration OH? in the solution bulk, which promotes the oxidative degradation of OG and its byproducts. The mean carbon oxidation state (COS) is estimated to reflect the degree of mineralization. Based on the pseudo first-order kinetics with respect to OH?, OG, Fe2+, the corresponding reaction rates is established. UV–Vis spectrometry reveals the presence of four major intermediates, which helps establish the OG degradation pathways.
关键词： Photoelectrochemical catalytic oxidation,Orange G,Electro-Fenton,Photoelectro-Fenton,Electrochemical oxidation
更新于2025-09-23 15:23:52
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Facile synthesis of two-dimensional tailored graphitic carbon nitride with enhanced photoelectrochemical properties through a three-step polycondensation method for photocatalysis and photoelectrochemical immunosensor
摘要： Graphitic carbon nitride (g-C3N4) is an ideal alternative two-dimensional (2D) nanostructure for photocatalysis and photoelectrochemical (PEC) application, while controllably fabricating 2D shaped g-C3N4 nanolayers/nanosheets is still facing challenges. On the basis of temperature-dependent polymorphic characters, herein, a 2D extending g-C3N4 (g-CNS3) is synthesized from dicyandiamide as the precursor by operating the condensation temperature in a continuously three-step thermal polycondensation procedure. The g-CNS3 with film-like morphology showed improved visible-light absorption ability and enhanced PEC performance compared to g-CNS1 synthesized via the traditional one-step thermal polymerization method. Benefiting from its excellent PEC properties, the g-CNS3 exhibited high photocatalytic activity to removal MB with fast kinetics and served as the photoactive layer to construct a PEC immunosensor with high sensitivity and specificity for subgroup J avian leukosis virus detection. A linear range from 102.14 to 103.35 TCID50/mL and a detection limit of 102.08 TCID50/mL were obtained for the PEC immunoassay of the target virus. This work might provide a novel protocol for tailoring shaped 2D g-C3N4 nanosemiconductor with superior properties and shed light on its promising PEC applications.
关键词： Two-dimensional material,Photocurrent response,Graphitic carbon nitride,Photocatalysis,Photoelectrochemical immunosensor
更新于2025-09-23 15:23:52
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Operando observation of chemical transformations of iridium oxide during photoelectrochemical water oxidation
摘要： Iridium oxide is one of the few catalysts capable of catalyzing the oxygen evolution reaction (OER) in both acidic and basic conditions. Understanding the mechanism of IrOx under realistic photoelectrochemical conditions is important for the development of integrated water splitting systems. Herein, we have developed a highly efficient OER photoanode in pH 1 aqueous solutions based on a sputtered IrOx film and a p+n-Si light absorber, interfaced with sputtered Au layer. Operando high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS) was employed to monitor the oxidation state changes of IrOx during both electrochemical and photoelectrochemical (PEC) water oxidation reactions in pH 1 aqueous solutions. We observed a gradual increase of the average oxidation state of Ir with increasing anodic potential in the pre-catalytic region, followed by a reduction of Ir under O2 evolution conditions. Consistent results were obtained on dark anodes and illuminated photoanodes. However, when the thickness of IrO2 was increased to 2 and 3 nm, the spectral changes became much less pronounced and the reduction of Ir oxidation state after the OER onset was not observed. This is due to the lower surface to bulk ratio, where lattice oxygen sites in the bulk are not accessible for the formation of hydroxide. More generally, the operando method developed here can be extended to other materials, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.
关键词： oxygen evolution reaction (OER),electrochemical and photoelectrochemical (PEC),high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS),iridium oxide,Operando method
更新于2025-09-23 15:23:52
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Fe Foil-Guided Fabrication of Uniform Ag@AgX Nanowires for Sensitive Detection of Leukemia DNA
摘要： Herein, we report a novel Fe foil guided, in-situ etching strategy for the preparation of highly uniform Ag@AgX (X = Cl, Br) nanowires (NWs) and applied the photoelectric-responsive materials for sensitive photoelectrochemical (PEC) detection of Leukemia DNA. The Ag@AgX NWs formation process was discussed from the redox potential and Ksp value. The fabricated PEC platform for sensing Leukemia DNA showed good assay performance with a wide linear range (0.1 pM to 50 nM) and low detection limit of 0.033 pM. We envision that our Fe foil-guided synthetic method could be applied to synthesize more photoactive materials for sensitive PEC detections.
关键词： Leukemia DNA,photoelectrochemical detection,in-situ,Br) nanowires,Ag@AgX (X = Cl,etch,Fe foil
更新于2025-09-23 15:23:52
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Ultrathin GeSe Nanosheets: from Systematic Synthesis, to Studies of Carrier Dynamics and Applications for High Performance UV-Vis Photo-Detector
摘要： Owing to the attractive energy band properties, black phosphorus (BP)-analogue semiconductor, germanium selenide (GeSe), shows a promising potential applied for optoelectronic devices. Herein, ultrathin GeSe nanosheets were systematically prepared via a facile liquid phase exfoliation (LPE) approach, with controllable nano-scale thickness. Different from BP, ultrathin GeSe nanosheets exhibits a good stability under both liquid and ambient conditions. Besides, its ultrafast carrier dynamics was probed by transient absorption spectroscopy. We showed that the GeSe nanosheets-based photo-detector exhibits excellent photoresponse behaviors ranging from ultraviolet (UV) to the visible regime, with high responsivity and low dark current. Furthermore, the detective ability of such a device can be effectively modulated by varying the applied bias potential, light intensity and concentration of electrolyte. Generally, our present contribution could not only supply fundamental knowledge of GeSe nanosheets-based photoelectrochemical (PEC)-type device, but also offer a guidance to extend other possible semiconductor materials in the application of PEC-type photo-detector.
关键词： photoelectrochemical,photo-detector,liquid phase exfoliation,carrier dynamics,GeSe nanosheets
更新于2025-09-23 15:23:52
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Atomically Precise Bimetallic Nanoclusters as Photosensitizers in Photoelectrochemical Cells
摘要： The atomically precise bimetallic nanocluster, Au24Ag20(PhCC)20(SPy)4Cl2 (1), is for the first time employed as a stable photosensitizer for photoelectrochemical applications. The sensitization of TiO2 nanotube arrays (TNA) with 1 greatly enhances the light harvest ability of the composite, as 1 shows high molar-extinction-coefficient in the UV-Vis region. Compared to a more standard Au25(SG)18 -TNA (2-TNA, SG: Glutathione), 1-TNA shows a much better stability under illumination both in neutral and basic conditions. The precise composition of the photosensitizers enables a direct comparison of the sensitization ability between 1 and 2. With the same cluster loading, the photocurrent produced by 1-TNA is 15 times larger than 2-TNA. The superior performance of 1-TNA over 2-TNA is attributed not only to the higher light absorption ability of 1, but also to the higher charge-separation efficiency. Besides, a ligand effect on the stability of the photoelectrode and charge-transfer between the NCs and the semiconductor is revealed. Our work paves the way to study the role of metal nanoclusters as photosensitizers at the atomic level, which is essential for the design of better material for light energy conversion.
关键词： Energy Conversion,Bimetallic Nanoclusters,Photosensitizers,Nanostructured Materials,Photoelectrochemical Cells
更新于2025-09-23 15:23:52