研究目的
To investigate the molecular engineering of graphitic carbon nitride (g-C3N4) by copolymerization with phenyl urea to enhance its photocatalytic properties for CO2 reduction and organic dye degradation.
研究成果
Phenyl grafting significantly enhances the photocatalytic activity of g-C3N4 for CO2 reduction to methane and formic acid, and for rapid degradation of rhodamine B dye, due to improved charge carrier separation, extended light absorption, and increased surface area. The catalyst shows good stability and recyclability, suggesting potential for sustainable energy and environmental applications.
研究不足
The amount of phenyl urea dopant is critical; excess can deform the tri-s-triazine network and reduce photoactivity. High pyrolysis temperature may affect π-conjugation preservation. The study is limited to specific conditions and may not generalize to other dopants or applications.
1：Experimental Design and Method Selection:
The study involves copolymerization of phenyl urea, melamine, and urea to synthesize phenyl-grafted g-C3N4, followed by characterization and photocatalytic testing. Theoretical models include band gap calculations and reaction mechanisms for CO2 reduction and dye degradation.
2：Sample Selection and Data Sources:
Samples include pure g-C3N4 and Phx-g-C3N4 with varying phenyl urea content (x = 5, 20, 50, 100, 200 mg). Data sources are experimental measurements from synthesis and characterization techniques.
3：List of Experimental Equipment and Materials:
Equipment includes powder X-ray diffractometer (PXRD), UV-Vis diffuse reflectance spectrometer (UV-Vis DRS), Fourier transform infrared spectrometer (FT-IR), solid-state NMR spectrometer, X-ray photoelectron spectrometer (XPS), field emission scanning electron microscope (FE-SEM), transmission electron microscope (TEM), Brunauer-Emmett-Teller surface area analyzer (BET), gas chromatograph with thermal conductivity and flame ionization detectors (GC-TCD/FID), high-performance liquid chromatograph (HPLC), photoluminescence spectrometer (PL), time-resolved PL setup (TRPL), fluorescence lifetime imaging microscope (FLIM). Materials include urea, melamine, phenyl urea, N,N-dimethylformamide (DMF), water, triethanolamine (TEA), rhodamine B dye.
4：Experimental Procedures and Operational Workflow:
Synthesis of phenyl urea from urea and aniline; copolymerization with melamine and urea at 550°C; characterization using PXRD, UV-Vis DRS, FT-IR, NMR, XPS, SEM, TEM, BET; photocatalytic tests for CO2 reduction in DMF/H2O/TEA mixture under visible light irradiation with product analysis by GC and HPLC; dye degradation tests under visible light with kinetics analysis; recyclability tests; charge carrier lifetime measurements.
5：Data Analysis Methods:
Data analyzed using Kubelka-Munk plots for band gap, kinetics fitting for degradation rates, statistical analysis for product yields, and software tools for spectral deconvolution and lifetime calculations.
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Powder X-ray Diffractometer
Used for crystalline phase and structural analysis of materials.
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UV-Vis Diffuse Reflectance Spectrometer
Used to measure optical absorption properties and band gap calculations.
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Fourier Transform Infrared Spectrometer
Used for chemical bonding analysis via FT-IR spectra.
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Solid-state NMR Spectrometer
CP-MAS
Used for carbon environment analysis in solid samples.
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X-ray Photoelectron Spectrometer
Used for elemental composition and chemical state analysis.
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Field Emission Scanning Electron Microscope
FE-SEM
Used for morphological analysis and elemental composition via EDS.
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Transmission Electron Microscope
TEM
Used for microstructural analysis and interplanar distance measurement.
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Brunauer-Emmett-Teller Surface Area Analyzer
BET
Used to measure specific surface area and pore size.
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Gas Chromatograph
GC-TCD/FID
Used for analysis of gaseous products from CO2 photoreduction.
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High-Performance Liquid Chromatograph
HPLC
Used for analysis of liquid products like formic acid.
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Photoluminescence Spectrometer
PL
Used to study charge carrier recombination via emission spectra.
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Time-Resolved PL Setup
TRPL with TCSPC
Used to measure charge carrier lifetimes.
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Fluorescence Lifetime Imaging Microscope
FLIM
Used for imaging based on fluorescence lifetime.
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Visible Light Source
20W white cold LED
Used as light source for photocatalytic experiments.
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