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1.
Small ; 19(43): e2302980, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37376838

RESUMO

A feasible nanoscale framework of heterogeneous plasmonic materials and proper surface engineering can enhance photoelectrochemical (PEC) water-splitting performance owing to increased light absorbance, efficient bulk carrier transport, and interfacial charge transfer. This article introduces a new magnetoplasmonic (MagPlas) Ni-doped Au@Fex Oy nanorods (NRs) based material as a novel photoanode for PEC water-splitting. A two stage procedure produces core-shell Ni/Au@Fex Oy MagPlas NRs. The first-step is a one-pot solvothermal synthesis of Au@Fex Oy . The hollow Fex Oy nanotubes (NTs) are a hybrid of Fe2 O3 and Fe3 O4 , and the second-step is a sequential hydrothermal treatment for Ni doping. Then, a transverse magnetic field-induced assembly is adopted to decorate Ni/Au@Fex Oy on FTO glass to be an artificially roughened morphologic surface called a rugged forest, allowing more light absorption and active electrochemical sites. Then, to characterize its optical and surface properties, COMSOL Multiphysics simulations are carried out. The core-shell Ni/Au@Fex Oy MagPlas NRs increase photoanode interface charge transfer to 2.73 mAcm-2 at 1.23 V RHE. This improvement is made possible by the rugged morphology of the NRs, which provide more active sites and oxygen vacancies as the hole transfer medium. The recent finding may provide light on plasmonic photocatalytic hybrids and surface morphology for effective PEC photoanodes.

2.
ACS Omega ; 9(1): 559-572, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38222549

RESUMO

The photodegradation of organic pollutants using metal oxide-based catalysts has drawn great attention as an effective method for wastewater treatment. In this study, zinc oxide nanoparticles (ZnO NPs) and zinc oxide/copper oxide nanocomposites (ZnO/CuO NCs) were fabricated using the leaf extract of Croton macrostachyus as a nontoxic, natural reducing and stabilizing agent. The synthesized samples were characterized by employing X-ray diffraction, microscopic, spectroscopic, and electrochemical methods. The results confirmed the successful synthesis of ZnO NPs and ZnO/CuO NCs with well-defined crystalline structures and morphologies. The prepared samples were tested for the photodegradation of methylene blue (MB) dye under visible light irradiation. Compared to ZnO NPs, ZnO/CuO NCs showed greatly improved photocatalytic performances, particularly with the sample prepared with the 20 mol % Cu precursor (97.02%). The enhancement could be related to the formed p-n heterojunction, which can suppress the recombination of charge carriers and extend the photoresponsive range. A theoretical study of the photocatalytic activity of ZnO/CuO NCs against MB dye degradation was also conducted by using COMSOL Multiphysics software. The results of the simulation are in reasonable agreement with those of the experiment. This study contributes to the development of sustainable and effective photocatalytic materials that are suitable for application in environmental remediation, particularly in the treatment of wastewater.

3.
ACS Omega ; 9(26): 28463-28475, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38973891

RESUMO

The discharge of toxic dye effluents from industry is a major concern for environmental pollution and toxicity. These toxic dyes can be efficiently removed from waste streams using a photocatalysis process involving visible light. Due to its simple synthesis procedure, inexpensive precursor, and robust stability, graphitic carbon nitride (g-C3N4, or CN) has been used as a visible light responsive catalyst for the degradation of dyes with mediocre performance because it is limited by its low visible light harvesting capability due to its wide bandgap and fast carrier recombination rate. To overcome these limitations and enhance the performance of g-C3N4, it was coupled with a narrow bandgap copper tin sulfide (CTS) semiconductor to form a p-n heterojunction. CTS and g-C3N4 were selected due to their good stability, low toxicity, ease of synthesis, layered sheet/plate-like morphology, and relatively abundant precursors. Accordingly, a series of copper tin sulfide/graphitic carbon nitride nanocomposites (CTS/g-C3N4) with varying CTS contents were successfully synthesized via a simple two-step process involving thermal pyrolysis and coprecipitation for visible-light-induced photocatalytic degradation of methyl orange (MO) dye. The photocatalytic activity results showed that the 50%(wt/wt) CTS/g-C3N4 composite displayed a remarkable degradation efficiency of 95.6% for MO dye under visible light illumination for 120 min, which is higher than that of either pristine CTS or g-C3N4. The improved performance is attributed to the extended light absorption range (due to the optimized bandgap), effective suppression of photoinduced electron-hole recombination, and improved charge transfer that arose from the formation of a p-n heterojunction, as evidenced by electrochemical impedance spectroscopy (EIS), photocurrent, and photoluminescence results. Moreover, the results of the reusability study showed that the composite has excellent stability, indicating its potential for the degradation of MO and other toxic organic dyes from waste streams.

4.
ACS Appl Mater Interfaces ; 15(29): 34883-34894, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37452743

RESUMO

In this study, a Ag/WO3/InGaN hybrid heterostructure was successfully developed by sputtering and molecular beam epitaxy techniques, to obtain unique Ag nanospheres adorned with cauliflower-like WO3 nanostructure over the InGaN nanorods (NRs). Exploiting the localized surface plasmon resonance of Ag, the Ag/WO3/InGaN heterostructure exhibited superior photoabsorption ability in the visible region (400-700 nm) of the solar spectrum, with a surface plasmon resonance band centered around 440 nm. Comprehensive analysis through photoluminescence spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy revealed that the Ag/WO3/InGaN hybrid heterostructure significantly enhances the charge carrier separation and transfer kinetics leading to improved overall photoelectrochemical (PEC) performance. The photocurrent density of the Ag/WO3/InGaN photoanode is 1.17 mA/cm2, which is about 2.72 times higher than that of pure InGaN NRs under visible light irradiation. The photoanode exhibited excellent stability for about 12 h. From the study, it has been found that the maximum applied bias photon-to-current efficiency (ABPE) is ∼1.67% at the applied bias of 0.6 V. The improved PEC water splitting efficiency of the Ag/WO3/InGaN photoanode is attributed to the synergistic effects of localized surface plasmon resonance (LSPR), efficient charge carrier separation and transport, and the presence of a Schottky junction. Consequently, the plasmonic metal-assisted heterojunction-based semiconductor Ag/WO3/InGaN demonstrates immense potential for practical applications in photoelectrochemical water splitting.

5.
ACS Appl Mater Interfaces ; 15(29): 34779-34788, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37431988

RESUMO

The rational synthesis and tailoring of metal-organic frameworks (MOFs) with multifunctional micro/nanoarchitectures have emerged as a subject of significant academic interest owing to their promising potential for utilization in advanced energy storage devices. Herein, we explored a category of three-dimensional (3D) NiCo2S4 nanospikes that have been integrated into a 1D Fe3C microarchitecture using a chemical surface transformation process. The resulting electrode materials, i.e., Fe3C@NiCo2S4 nanospikes, exhibit immense potential for utilization in high-performance hybrid supercapacitors. The nanospikes exhibit an elevated specific capacity (1894.2 F g-1 at 1 A g-1), enhanced rate capability (59%), and exceptional cycling stability (92.5% with 98.7% Coulombic efficiency) via a charge storage mechanism reminiscent of a battery. The augmented charge storage characteristics are attributed to the collaborative features of the active constituents, amplified availability of active sites inherent in the nanospikes, and the proficient redox chemical reactions of multi-metallic guest species. When using nitrogen-doped carbon nanofibers as the anode to fabricate hybrid supercapacitors, the device exhibits high energy and power densities of 62.98 Wh kg-1 and 6834 W kg-1, respectively, and shows excellent long-term cycling stability (95.4% after 5000 cycles), which affirms the significant potential of the proposed design for applications in hybrid supercapacitors. The DFT study showed the strong coupling of the oxygen from the electrolyte OH- with the metal atom of the nanostructures, resulting in high adsorption properties that facilitate the redox reaction kinetics.

6.
ACS Omega ; 7(35): 30908-30919, 2022 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-36092591

RESUMO

CuO-ZnO nanocomposites (NCs) were synthesized using an aqueous extract of Verbascum sinaiticum Benth. (GH) plant. X-ray diffraction (XRD), spectroscopic, and microscopic methods were used to explore the crystallinity, optical properties, morphology, and other features of the CuO-ZnO samples. Furthermore, catalytic performances were investigated for methylene blue (MB) degradation and 4-nitrophenol (4-NP) reduction. According to the results, CuO-ZnO NCs with 20 wt % CuO showed enhanced photocatalytic activity against MB dye with a 0.017 min-1 rate constant compared to 0.0027 min-1 for ZnO nanoparticles (NPs). Similarly, a ratio constant of 5.925 min-1 g-1 4-NP reductions was achieved with CuO-ZnO NCs. The results signified enhanced performance of CuO-ZnO NCs relative to ZnO NPs. The enhancement could be due to the synergy between ZnO and CuO, resulting in improved absorption of visible light and reduced electron-hole (e-/h+) recombination rate. In addition, variations in the CuO content affected the performance of the CuO-ZnO NCs. Thus, the CuO-ZnO NCs prepared using V. sinaiticum Benth. extract could make the material a desirable catalyst for the elimination of organic pollutants.

7.
Nanomaterials (Basel) ; 11(6)2021 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-34070272

RESUMO

Water splitting driven by renewable energy sources is considered a sustainable way of hydrogen production, an ideal fuel to overcome the energy issue and its environmental challenges. The rational design of electrocatalysts serves as a critical point to achieve efficient water splitting. Layered double hydroxides (LDHs) with two-dimensionally (2D) layered structures hold great potential in electrocatalysis owing to their ease of preparation, structural flexibility, and tenability. However, their application in catalysis is limited due to their low activity attributed to structural stacking with irrational electronic structures, and their sluggish mass transfers. To overcome this challenge, attempts have been made toward adjusting the morphological and electronic structure using appropriate design strategies. This review highlights the current progress made on design strategies of transition metal-based LDHs (TM-LDHs) and their application as novel catalysts for oxygen evolution reactions (OERs) in alkaline conditions. We describe various strategies employed to regulate the electronic structure and composition of TM-LDHs and we discuss their influence on OER performance. Finally, significant challenges and potential research directions are put forward to promote the possible future development of these novel TM-LDHs catalysts.

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