研究目的
To develop a precursor-reforming strategy to induce g-C3N4 microtubes with spatial anisotropic charge separation for enhanced photocatalytic hydrogen evolution performance.
研究成果
The precursor-reforming strategy successfully produces g-C3N4 microtubes with spatial anisotropic charge separation, leading to significantly enhanced photocatalytic H2 evolution activity. The mg-C3N4-24 sample achieves the highest performance due to efficient charge carrier separation, with electrons migrating to the outer shell and holes to the inner shell. This work advances material design through precursor-reforming and highlights the importance of morphological control in photocatalysis.
研究不足
The study does not explicitly discuss limitations, but potential constraints include the use of specific precursors (melamine) and hydrothermal conditions, which may limit scalability or applicability to other materials. Optimization areas could involve further tuning of hydrothermal parameters or exploring other precursor systems.
1:Experimental Design and Method Selection:
The study employs a precursor-reforming strategy involving hydrothermal treatment of melamine to form melamine-cyanuric acid (MCA) precursors, followed by thermal polymerization under N2 atmosphere to produce g-C3N4 microtubes (mg-C3N4). The design rationale is to conquer hydrogen bonds during thermal exfoliation to form tubular structures with adjustable orifice closure and spatial anisotropic charge separation. Methods include hydrothermal synthesis, thermal polymerization, and photo-deposition for characterizing charge separation.
2:4). The design rationale is to conquer hydrogen bonds during thermal exfoliation to form tubular structures with adjustable orifice closure and spatial anisotropic charge separation. Methods include hydrothermal synthesis, thermal polymerization, and photo-deposition for characterizing charge separation. Sample Selection and Data Sources:
2. Sample Selection and Data Sources: Samples include bulk g-C3N4 (bg-C3N4), ultrathin g-C3N4 (ug-C3N4), and mg-C3N4 with varying hydrothermal times (16 h, 20 h, 24 h, 28 h). Precursors are melamine and MCA, selected based on hydrothermal time to study morphology evolution. Data sources are experimental characterizations and photocatalytic tests.
3:List of Experimental Equipment and Materials:
Equipment includes alumina crucible, Teflon stainless autoclave, Thermo ESCALAB 250XI (XRD, XPS), Nicolet Magna-IR 550 spectrometer (FT-IR), SEM (JSM-7001F, Jeol), TEM (JEM-2100F), UV-vis spectrophotometer (UV-2450, Shimadzu), BET/BJH surface area analyzer (3H-2000PS1), electrochemical workstation (Zahner Instruments), photoluminescence spectrometer (FLS1000, Hitachi), gas chromatograph (GC-2030), and Xe lamp with UV cut-off filter. Materials include melamine, deionized water, MnSO4·H2O, H2PtCl6, triethanolamine, and H2PtCl6·6H2O.
4:2O. Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: For bg-C3N4, melamine is heated at 550°C for 4 h. For ug-C3N4 and mg-C3N4, melamine is dissolved in water, hydrothermally treated at 180°C for varying times (16-28 h) to form MCA precursors, then thermally polymerized at 550°C for 4 h under N2. Photo-deposition of Pt and MnOx involves dispersing mg-C3N4 in solutions with metal precursors, stirring in dark, then UV illumination. Photocatalytic H2 evolution tests use 50 mg sample in 100 mL triethanolamine solution with Pt co-catalyst, under Xe lamp irradiation, with H2 concentration analyzed hourly by GC.
5:Photo-deposition of Pt and MnOx involves dispersing mg-C3N4 in solutions with metal precursors, stirring in dark, then UV illumination. Photocatalytic H2 evolution tests use 50 mg sample in 100 mL triethanolamine solution with Pt co-catalyst, under Xe lamp irradiation, with H2 concentration analyzed hourly by GC. Data Analysis Methods:
5. Data Analysis Methods: Data analysis includes XRD for crystal structure, FT-IR for chemical bonds, XPS for surface chemistry, SEM/TEM for morphology, UV-vis DRS for optical properties, BET for surface area, photocurrent and EIS for charge transfer, PL for carrier recombination, and GC for H2 quantification. Statistical techniques involve Tauc plots for band gap, Mott-Schottky for band alignment, and biexponential fitting for PL lifetime.
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X-ray diffractometer
Thermo ESCALAB 250XI
Thermo
Used for X-ray diffraction (XRD) analysis to investigate crystal structures of samples.
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Scanning electron microscope
JSM-7001F
Jeol
Used for SEM analysis to observe morphology and microstructure.
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Transmission electron microscope
JEM-2100F
Jeol
Used for TEM analysis to examine microstructures and element mapping.
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UV-vis spectrophotometer
UV-2450
Shimadzu
Used for UV-vis diffuse reflectance spectra (DRS) to study optical properties.
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Photoluminescence spectrometer
FLS1000
Hitachi
Used for PL spectra and time-resolved fluorescence decay analysis.
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Fourier transform infrared spectrometer
Nicolet Magna-IR 550
Nicolet
Used for FT-IR spectra analysis to study chemical bonds and functional groups.
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X-ray photoelectron spectrometer
ESCALAB250XI
VG Scientific
Used for XPS analysis to determine surface chemical states and composition.
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Surface area analyzer
3H-2000PS1
Used for BET/BJH surface area and pore size distribution analysis.
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Electrochemical workstation
Zahner Instruments
Used for transient photocurrent and electrochemical impedance spectroscopy (EIS) measurements.
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Gas chromatograph
GC-2030
Used to analyze H2 concentrations during photocatalytic tests.
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Xe lamp
300 W
Used as light source for photocatalytic H2 evolution experiments.
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Autoclave
100 mL Teflon stainless
Used for hydrothermal synthesis of precursors.
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Alumina crucible
50 mL
Used for thermal polymerization of melamine.
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