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1.
In present work, we report a facile fabrication process to improve the photoelectrochemical (PEC) performance of ZnO-based photoelectrodes. In order to achieve that, the Cu2O nanocubes are cathodic-deposited on the as-prepared ZnO nanorods. Then rGO nanosheets are electrodeposited on the ZnO/Cu2O heterostructures. The fabricated photoelectrodes are systematically studied in detail by different characterization techniques such as powder X-ray diffraction, micro-Raman, X-ray photoelectron spectroscopy, ultraviolet diffused reflectance spectroscopy and photoluminescence spectroscopy analysis. Morphologies of the fabricated photoelectrodes are investigated through electron microscopy in scanning and transmission mode. To evaluate the PEC performance of the fabricated photoelectrodes, the line scan voltammetry (LSV) measurement is performed using a three-electrode system in 0.5-M Na2SO4 electrolyte solution under stimulated light illumination at 100 mW/cm2 from a 300-W Xenon Arc lamp coupled with an AM 1.5G filter using a three-electrode system. The photocurrent measurement demonstrates that the photoelectrodes based on ZnO/Cu2O/rGO possess enhanced PEC performance compared to the pristine ZnO and ZnO/Cu2O photoelectrodes. The photocurrent density of ZnO/Cu2O/rGO-15 photoelectrode (10.11 mA/cm2) is ∼9 and ∼3 times higher than the photoelectrodes based on pristine ZnO (1.06 mA/cm2) and ZnO/Cu2O (3.22 mA/cm2). The enhanced PEC performance of ZnO/Cu2O/rGO photoelectrode is attributed to the excellent light absorption properties of Cu2O and excellent catalytic and charge transport properties of rGO. Experimental results reveal that the proposed functional nanomaterials have a great potential in water splitting applications.  相似文献   

2.
Ultrathin hematite (α-Fe2O3) film deposited on a TiO2 underlayer as a photoanode for photoelectrochemical water splitting was described. The TiO2 underlayer was coated on conductive fluorine-doped tin oxide (FTO) glass by spin coating. The hematite films were formed layer-by-layer by repeating the separated two-phase hydrolysis-solvothermal reaction of iron(III) acetylacetonate and aqueous ammonia. A photocurrent density of 0.683 mA cm−2 at +1.5 V vs. RHE (reversible hydrogen electrode) was obtained under visible light (>420 nm, 100 mW cm−2) illumination. The TiO2 underlayer plays an important role in the formation of hematite film, acting as an intermediary to alleviate the dead layer effect and as a support of large surface areas to coat greater amounts of Fe2O3. The as-prepared photoanodes are notably stable and highly efficient for photoelectrochemical water splitting under visible light. This study provides a facile synthesis process for the controlled production of highly active ultrathin hematite film and a simple route for photocurrent enhancement using several photoanodes in tandem.  相似文献   

3.
Iron oxide n-Fe2O3 nanowire photoelectrodes were synthesized by thermal oxidation of Fe metal sheet (Alfa Co. 0.25 mm thick) in an electric oven then tested for their photoactivity. The photoresponse of the n-Fe2O3 nanowires was evaluated by measuring the rate of water splitting reaction to hydrogen and oxygen, which is proportional to photocurrent density, Jp. The optimized electric oven-made n-Fe2O3 nanowire photoelectrodes showed photocurrent densities of 1.46 mA cm−2 at measured potential of 0.1 V/SCE at illumination intensity of 100 mW cm−2 from a Solar simulator with a global AM 1.5 filter. For the optimized carbon modified (CM)-n-TiO2 synthesized by thermal flame oxidation the photocurrent density for water splitting was found to increase by two fold to 3.0 mA cm−2 measured at the same measured potential and the illumination intensity. The carbon modified (CM)-n-Fe2O3 electrode showed a shift of the open circuit potential by −100 mV/SCE compared to undoped n-Fe2O3 nanowires. A maximum photoconversion efficiency of 2.3% at applied potential of 0.5 V/Eaoc was found for CM-n-Fe2O3 compared to 1.69% for n-Fe2O3 nanowires at higher applied potential of 0.7 V/Eaoc. These CM-n- Fe2O3 and n- Fe2O3 nanowires thin films were characterized using photocurrent density measurements under monochromatic light illumination, UV-Vis spectra, X-ray diffraction (XRD) and scanning electron microscopy (SEM).  相似文献   

4.
Arrayed porous iron-doped TiO2 with controllable pore size was prepared by using polystyrene spheres and its structure, morphology, composition and photoelectrochemical properties were characterized with X-ray diffraction, scanning electron microscope, inductively coupled plasma-atomic emission spectrometer and electrochemical methods. It is found that the photoelectrochemical properties of the arrayed porous TiO2 can be improved by doping adequate amount of iron in the lattice of TiO2 and the sample doped with 0.01 wt% Fe (based on Ti) exhibits the best photoelectrochemical performance. With doping 0.01 wt% Fe in TiO2, the photocurrent density of the sample is improved from 2.0 μA cm−2 to 10.0 μA cm−2 and its flat-band potential shifts from −0.38 V to −0.55 V (vs. SCE).  相似文献   

5.
It is demonstrated for the first time that significant enhancement of photoelectrochemical performance could be achieved by using microwave-assisted annealing for the fabrication of α-Fe2O3 thin films. The process can also lead to significant energy savings (>60% when compared with conventional methods). Different types of Fe thin films were oxidized using both microwave and conventional heating techniques. The photoelectrochemical performance of electrodeposited, undoped and Si-doped iron oxide samples showed that microwave-annealing resulted in superior structural and performance enhancements. The photocurrent densities obtained from microwave annealed samples are among the highest values reported for α-Fe2O3 photoelectrodes fabricated at low temperatures and short times; the highest photocurrent density at 0.55 V vs. VAg/AgCl, before the dark current onset, was 450 μA cm−2 for the Si-doped films annealed at 270 °C for 15 min using microwave irradiation (and 180 μA cm−2 at 0.23 V vs. VAg/AgCl) while conventional annealing at the same temperature resulted in samples with negligible (3 μA cm−2) photoactivity. In contrast, a 450 °C/15 min conventional heat treatment only resulted in a film with 25% lower photocurrent density than that of the microwave annealed sample. The improved performance is attributed to the lower processing temperatures and rapidity of the microwave method that help to retain the nanostructure of the thin films whilst restricting the grain growth to a minimum. The lower processing temperature requirements of the microwave process can also open up the possibility of fabricating hematite thin films on conducting, flexible, plastic electronic substrates.  相似文献   

6.
Nanoporous Zn0.5Cd0.5S nanosheets/reduced graphene oxide (Zn0.5Cd0.5S/RGO) composites were prepared by a facile in-situ photoreduction method of graphene oxide (GO) in the presence of nanoporous Zn0.5Cd0.5S single-crystal-like nanosheets under visible light irradiation. The Zn0.5Cd0.5S/RGO photoelectrodes was characterized by TEM, IR and Raman spectra. Electrochemical measurements demonstrated that Zn0.5Cd0.5S/RGO photoelectrodes own a higher anodic photocurrent density, a lower zero current potential, and a higher photoelectrochemical response than that of pure Zn0.5Cd0.5S photoelectrodes under visible light irradiation under the same conditions. This high photochemical activity is predominately ascribed to the presence of RGO, which serves as the electron collector to efficiently prolong the lifetime of photoinduced electrons from the excited Zn0.5Cd0.5S nanosheets. In addition, the content of RGO in the composites had a remarkable influence on the photoelectrochemical behaviors of the photoelectrodes and the optimal RGO content was found to be 5 wt%. Zn0.5Cd0.5S/RGO composites at RGO content of 5 wt% reached a stable hydrogen production rate of 12.05 μmol h−1 cm−2 at an externally applied bias of 0.6 V. Furthermore, the Zn0.5Cd0.5S/RGO composites as photoelectrodes were found to be highly stable for hydrogen evolution reaction. The electrons stored in RGO are readily discharged or scavenged on demand by the applied positive bias to the counter electrode, and thus rectify the flow of electrons. Importantly, this work may open up a facile in-situ method for using RGO scaffold to create a stable photoelectrode with enhanced photoelectrochemical activities.  相似文献   

7.
Photoelectrochemical water splitting using solar energy is a highly promising technology to produce hydrogen as an environmentally friendly and renewable fuel with high-energy density. This approach requires the development of appropriate photoelectrode materials and substrates, which are low-cost and applicable for the fabrication of large area electrodes. In this work, hematite photoelectrodes are grown by aerosol assisted chemical vapour deposition (AA-CVD) onto highly-conductive and bulk porous SnO2 (Sb-doped) ceramic substrates. For such photoelectrodes, the photocurrent density of 2.8 mA cm-2 is achieved in aqueous 0.1 M NaOH under blue LED illumination (λ = 455 nm; 198 mW cm-2) at 1.23 V vs. RHE (reversible hydrogen electrode). This relatively good photoelectrochemical performance of the photoelectrode is achieved despite the simple fabrication process. Good performance is suggested to be related to the three-dimensional morphology of the porous ceramic substrate resulting in excellent light-driven charge carrier harvesting. The porosity of the ceramic substrate allows growth of the photoactive layer (SnO2-grains covered by hematite) to a depth of some micrometers, whereas the thickness of Fe2O3-coating on individual grains is only about 100–150 nm. This architecture of the photoactive layer assures a good light absorption and it creates favourable conditions for charge separation and transport.  相似文献   

8.
The design of photoanode with highly efficient light harvesting and charge collection properties is important in photoelectrochemical (PEC) cell performance for hydrogen production. Here, we report the hierarchical In2O3:Sn/TiO2/CdS heterojunction nanowire array photoanode (ITO/TiO2/CdS-nanowire array photoanode) as it provides a short travel distance for charge carrier and long light absorption pathway by scattering effect. In addition, optical properties and device performance of the ITO/TiO2/CdS-nanowire array photoanode were compared with the TiO2 nanoparticle/CdS photoanode. The photocatalytic properties for water splitting were measured in the presence of sacrificial agent such as SO32− and S2− ions. Under illumination (AM 1.5G, 100 mW/cm2), ITO/TiO2/CdS-nanowire array photoanode exhibits a photocurrent density of 8.36 mA/cm2 at 0 V versus Ag/AgCl, which is four times higher than the TiO2 nanoparticle/CdS photoanode. The maximum applied bias photon-to-current efficiency for the ITO/TiO2/CdS-nanowire array and the TiO2 nanoparticle/CdS photoanode were 3.33% and 2.09%, respectively. The improved light harvesting and the charge collection properties due to the increased light absorption pathway and reduced electron travel distance by ITO nanowire lead to enhancement of PEC performance.  相似文献   

9.
The utilization of solar energy for the conversion of water to hydrogen and oxygen has been considered to be an efficient strategy to solve crisis of energy and environment. Here, we report the synthesis of reduced graphene oxide–TiO2 nanoparticle composite system through the photocatalytic reduction of graphite oxide using TiO2 nanoparticles. Photoelectrochemical characterizations and hydrogen evolution measurements of these nanocomposites reveal that the presence of graphene enhances the photocurrent density and hydrogen generation rate. The optimum photocurrent density and hydrogen generation rate has been found to be 3.4 mA cm−2 and 127.5 μmole cm−2h−1 in 0.5 M Na2SO4 electrolyte solution under 1.5AM solar irradiance of white light with illumination intensity of 100 mW cm−2. In graphene–TiO2 nanocomposite, photogenerated electrons in TiO2 are scavenged by graphene sheets and percolate to counter electrode to reduce H+ to molecular hydrogen thus increasing the performance of water-splitting reaction.  相似文献   

10.
Tungsten oxide (WO3) photoelectrodes with the surface tuned by Fe(Ⅲ) for photoelectrochemical water splitting were successfully synthesized. Nanostructured WO3 films were prepared using doctor blade method, then a facile and economical deposition-annealing process was employed to fabricate Fe(Ⅲ) modified WO3 films. The resulting composite's structural and optical properties were analyzed by SEM, EDX, XRD, UV–Vis spectrometry and XPS. The photoelectrochemical properties were evaluated by photocurrent density under 500 W Xe lamp with an intensity of 100 mW/cm2. The Fe(Ⅲ) modified WO3 electrode exhibited a larger photocurrent than the pure WO3 electrode. Significantly, the optimized Fe(Ⅲ) modified WO3 film achieved the maximum photocurrent density of 1.18 mA/cm2 at 0.8 V vs. Ag/AgCl in the 0.2 M Na2SO4. The enhanced photocurrent was attributed to the extension of the light response and the electron hole separation at the interface Fe(Ⅲ)/WO3 which was confirmed by Mott–Schottky and electrochemical impedance spectroscopy.  相似文献   

11.
Efficient photoelectrochemical oxygen separation from water was demonstrated using a nano-wall like carbon modified n-type titanium oxide (CM-n-TiO2) electrode during water splitting reaction. The CM-n-TiO2 electrode was synthesized by flame-oxidation of Ti metal sample. The combustion products of natural gas flame acted as the carbon source. The oxygen separation rate during water splitting was evaluated in terms of anodic photocurrent density, Jp, under solar simulated light illumination of 1 sun. Upon incorporation of carbon within the titanium oxide, the photocurrent density was enhanced to 4.97 mA cm−2 at CM-n-TiO2 electrode compared to 0.66 mA cm−2 at regular of n-TiO2 both at the same measured potential of - 0.6 V/SCE. Such a multiple-fold increase in photocurrent density at CM-n-TiO2 thin film electrode was attributed to its enhanced absorption in the UV region, red-shift to visible region due to carbon incorporation and as well as due to pronounced nano-wall like surface morphology generated under the harsh conditions of flame oxidation. CM-n-TiO2 photoelectrodes were characterized in terms of photocurrent measurements under white light and as well as under monochromatic light illuminations, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), the valence band X-ray photoelectron spectroscopy (XPS) and the AC-impedance measurements.  相似文献   

12.
Highly efficient water splitting electrode based on uniform platinum (Pt) nanoparticles on self-organized TiO2 nanotube arrays (TNTAs) was prepared by a combination of multi-step electrochemical anodization with facile photoreduction process. Uniform platinum (Pt) nanoparticles with an average diameter of 8 nm are distributed homogeneously on nanoporous top layer and underneath TiO2 nanotube wall. In comparison to pristine TNTAs, Pt@TNTAs show substantially enhanced photocurrent density and the incident photon-to-current conversion efficiency (IPCE) in the entire wavelength window. The maximum photocurrent density and IPCE from the optimized Pt@TNTAs photoelectrode (Pt, ~1.57 wt%) were about 24.2 mA cm−2 and 87.9% at 350 nm, which is much higher than that of the pure nanotubes sample (16.3 mA cm−2 and 67.3%). The resultant Pt@TNTAs architecture exhibited significantly enhanced photoelectrochemical activities for solar water splitting with hydrogen evolution rate up to 495 μmol h−1 cm−2 in 2 M Na2CO3 + 0.5 M ethylene glycol under the optimal external bias of −0.3 VSCE.  相似文献   

13.
An integrated solar water splitting tandem cell without external bias was designed using a FeOOH modified TiO2/BiVO4 photoanode as a photoanode and p-Cu2O as a photocathode in this study. An apparent photocurrent (0.37 mA/cm2 at operating voltage of +0.36 VRHE) for the tandem cell without applied bias was measured, which is corresponding to a photoconversion efficiency of 0.46%. Besides, the photocurrent of FeOOH modified TiO2/BiVO4–Cu2O is much higher than the operating point given by pure BiVO4 and Cu2O photocathode (∼0.07 mA/cm2 at +0.42 VRHE). Then we established a FeOOH modified TiO2/BiVO4–Cu2O two-electrode system and measured the current density-voltage curves under AM 1.5G illumination. The unassisted photocurrent density is 0.12 mA/cm−2 and the corresponding amounts of hydrogen and oxygen evolved by the tandem PEC cell without bias are 2.36 μmol/cm2 and 1.09 μmol/cm2 after testing for 2.5 h. The photoelectrochemical (PEC) properties of the FeOOH modified TiO2/BiVO4 photoanode were further studied to demonstrate the electrons transport process of solar water splitting. This aspect provides a fundamental challenge to establish an unbiased and stabilized photoelectrochemical (PEC) solar water splitting tandem cell with higher solar-to-hydrogen efficiency.  相似文献   

14.
Combining WO3 with suitable materials to form heterojunction is essential to overcome the limitations of WO3 to enhance its photoelectrochemical (PEC) water splitting activity. Moreover, a clear understanding of photo-response and charge behavior of materials could lead to the rational design of efficient photoelectrodes. Given this, an efficient strategy is applied to fabricate WO3 heterojunction with nitrogen-doped carbon dots (NCDs) and in-depth characterization to investigate the surface charge dynamics using nano imaging in a relation to the enhanced PEC water splitting activity. The optimized NCDs loading to the WO3 NRs exhibited the enhanced photocurrent density of 1.54 mA cm−2 at 1.23V vs RHE under AM 1.5 G illumination, highest IPCE of ~82 % (at 308.32 nm). The Kelvin probe force microscopy and electrostatic force microscopy reveal that after loading NCDs to the WO3, a relatively smooth charge transport has been observed, which improves the PEC. Furthermore, this work demonstrates the effect of photogenerated charges caused by the NCDs that assist in enhancing the increased photocurrent, hydrogen production efficiency, and stability of the PEC water splitting system. Significantly, the nano imaging characterization utilized in this work could be extended to various photoanodes to study the surface charge dynamics.  相似文献   

15.
This paper deals with a study on the effect of 120 MeV Ag9+ ion irradiation on photoelectrochemical properties of SrTiO3 thin films deposited on Indium doped Tin Oxide (ITO) coated glass by sol-gel spin-coating technique. The structural evolution in the pristine and irradiated films was determined by X-ray diffraction and X-ray photoelectron spectroscopy. Surface morphology was studied by Atomic Force Microscopy (AFM) and optical measurements were done by UV-visible absorption spectroscopy. Irradiation of SrTiO3 thin films was found to be effective in improving its photoelectrochemical properties. A noticeable decrease in the average grain diameter from 36 to 26 nm, reduction in bandgap from 3.55 to 3.43 eV and increase in roughness after irradiation contributed in enhancing photoelectrochemical activity of SrTiO3 thin films. Thin films irradiated at fluence 3 × 1012 ions cm−2, when used in PEC cell exhibited enhanced photocurrent of 0.16 mA cm−2 at zero bias conditions, which was four times higher than that of the unirradiated sample.  相似文献   

16.
Fe2O3 nanostructures photoanodes were prepared via sol–gel spin-coating method onto fluorine-doped tin oxide glass substrates using six different surfactants: polyethylene glycol (PEG-300), Triton X-100, pluronic F127, cetyltrimethylammonium bromide (CTAB), octadecyltrimethylammonium bromide (OTAB) and tetradecyltrimethylammonium bromide (TTAB). The resulting films have thickness from 520 ± 10 to 980 ± 10 nm after calcinations at 450 °C in the air. A comparative study of photocatalytic activity of thin films was performed. The photo-generated samples were determined by measuring the currents and voltages under illumination of UV–vis light. The highest photocurrent density of 1.77 mA/cm2 at 1 V/SCE, under illumination intensity of 100 mW cm−2 from a solar simulator with a global AM 1.5 filter, were produced by TTAB treated sample. The optical properties, morphology, surface roughness and structure of the films were also characterized by UV–visible spectroscopy, SEM, AFM and XRD. The results are consistent with photocatalytic performance: TTAB treated sample has the highest grain size and optical absorption. The improved performance of this sample can be attributed to the crystallinity process of TTAB, which leads to the larger grain size and highest photocatalytic activity. The study demonstrates that photoelectrochemical performance of metal oxide can be improved by simply changing surfactant. The results highlighted the superior performance of cationic surfactants over non-ionic surfactants in preparing Fe2O3 photoanodes by sol–gel method. Moreover, the study showed that decreasing hydrocarbon tail of cationic surfactants can increase the crystallite size and improve photocatalytic activity.  相似文献   

17.
Hematite is a prospective semiconductor in photoelectrochemical (PEC) water oxidation field due to its suitable bandgap for the solar spectrum absorption. Nevertheless, the low transfer and separation efficiency of the charge carriers are restricted by its diffusion length of hole which is 2–4 nm and further reduce the PEC performance. Here, we report an innovative method, by introducing nanocavities into the α-Fe2O3 nanorod arrays photoanodes through helium ions implantation, to improve the charge carriers' transfer and separation efficiency and further to enhance water oxidation performance. The result indicates that, the photocurrent density of nanocavities embedded α-Fe2O3 photoanode (S2-A sample) reaches 1.270 mA/cm2 at 1.6 V vs. RHE which is 1-fold higher than that of the pristine α-Fe2O3 (0.688 mA/cm2) and the photocurrent density of S2-A sample reaches 0.652 mA/cm2 at 1.23 V vs. RHE. In this work, the ion implantation combined with post annealing method is found to be a valid method to improve the photoelectrochemical performance, and it also can be further used to modify the other semiconductor photoelectrodes materials.  相似文献   

18.
InGaN nanorods are highly desirable candidates for photoelectrochemical water splitting photoelectrodes because of their inherent material properties. However, their use is hindered by their low carrier separation efficiency and high production cost. Therefore, in this work, InGaN nanorods were grown by a low-cost HCVD method, and, p-n heterojunction n-InGaN/p-Cu2O photoanodes were successfully constructed by electrodeposition to address the low carrier separation efficiency. The optimized InGaN/Cu2O photoelectrodes with uniform morphology have a maximum photocurrent density of 4.2 mA cm?2 at 1.23 V vs. RHE, which is 8.4 times that of pure InGaN nanorod photoelectrodes. A comprehensive experimental study showed that this approach of constructing p-n heterojunctions greatly enhances the carrier separation efficiency and alleviates the charge transfer kinetic bottleneck at photoelectrodes.  相似文献   

19.
A highly stable photoelectrocatalytic electrode made of CdS-modified short, robust, and highly-ordered TiO2 nanotube array for efficient visible-light hydrogen generation was prepared via sonoelectrochemical anodization and sonoelectrochemical deposition method. The short nanotube electrode possesses excellent charge separation and transfer properties, while the sonoelectrochemical deposition method improves the combination between CdS and TiO2 nanotubes, as well as the dispersion of CdS nanoparticles. Different characterization techniques were used to study the nanocomposite electrode. UV-vis absorption and photoelectrochemical measurements proved that the CdS coating extends the visible spectrum absorption and the solar spectrum-induced photocurrent response. Comparing the photoactivity of the CdS/TiO2 electrode obtained using sonoelectrochemical deposition method with others that synthesized using plain electrochemical deposition, the current density of the former electrode is ∼1.2 times higher that of the latter when biased at 0.5 V. A ∼7-fold enhancement in photocurrent response is obtained using the sonoelectrochemically fabricated CdS/TiO2 electrode in comparison with the pure TiO2 nanotube electrode. Under AM1.5 illumination the composite photoelectrode generate hydrogen at a rate of 30.3 μmol h−1 cm−2, nearly 13 times higher than that of pure titania nanotube electrode. Recycle experiments demonstrated the excellent stability and reliability of CdS/TiO2 electrode prepared by sonoelectrochemical deposition. This composite electrode, with its strong mechanical stability and excellent combination of CdS and TiO2 nanotubes, offers promising applications in visible-light-driven renewable energy generation.  相似文献   

20.
In this work, a heterostructure CdS/TiO2 nanotubes (TNT) photoelectrode is decorated with Ni nanoparticles (NPs) to enhance hydrogen generation via the photoelectrochemical method. Herein, we report a systematic study of the effect of Ni NPs heterostructure photoelectrode to improve light absorption and photoelectrochemical (PEC) performance. The fabricated photoelectrodes were evaluated for photoelectrochemical hydrogen generation under simulated sunlight. The optimized Ni/CdS/TNT photoelectrode exhibited an improved photocurrent density of 6.5 mA cm?2 in poly-sulfide aqueous media at a low potential of 0 V. Owing to the enhanced photocurrent density, Ni NPs also played a significant role in improving the stability of the photoelectrode. The synergistic effect with semiconductor ternary junction incites the surface plasmon resonance (SPR) for light-harvesting to enhance photoelectrochemical hydrogen generation.  相似文献   

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