研究目的
To develop a cost-efficient photocatalytic oxidative denitrogenation and desulfurization system for fuels under visible light using Na doped g-C3N4 nanosheets catalyst, with molecular O2 as oxidant, for removing small molecules like pyridine and thiophene.
研究成果
Na doped g-C3N4 nanosheets effectively enhance photocatalytic oxidative denitrogenation and desulfurization under visible light using O2 as oxidant, with holes as major active species. The catalyst shows good recyclability and stability, making it a promising low-cost alternative to traditional methods.
研究不足
The study focuses on model fuels with specific contaminants (pyridine and thiophene) and may not cover all real fuel compositions. The scalability and long-term stability in industrial applications are not fully addressed. The use of a Xe lamp may not perfectly simulate natural sunlight conditions.
1:Experimental Design and Method Selection:
The study involved synthesizing Na doped g-C3N4 nanosheets via a mixed-calcination method using melamine and NaCl, followed by characterization and photocatalytic activity tests for oxidative denitrogenation and desulfurization under visible light irradiation with O2 as oxidant.
2:Sample Selection and Data Sources:
Model fuels were prepared by dissolving pyridine or thiophene in n-octane with specific concentrations of N and S elements. Catalysts included pure g-C3N4 and Na doped variants with varying NaCl/melamine ratios.
3:List of Experimental Equipment and Materials:
Equipment included Rigaku D/Max 2400 diffractometer for XRD, ASAP 2420 surface area analyzer for BET, Nicolet Thermo 360 spectrometer for FT-IR, THERMO instrument for XPS, Pyris 1 thermal analyzer for TGA, JEM-2100HR TEM, JSM-7500F SEM, ZetaPALS Brookhaven instrument for zeta potential, JASCO V-770 spectrometer for UV-vis, EDAX Orbis PC for PL, CHI650D electrochemical workstation for photocurrent, 300 W Xe lamp with cut-off filter for light source, Agilent GC-7890B gas chromatograph for analysis, and ICS-600 ion-chromatograph for product analysis. Materials included melamine, NaCl, n-octane, pyridine, thiophene, triethanolamine, dimethyl sulphoxide, and various chemicals for characterizations.
4:Experimental Procedures and Operational Workflow:
Catalysts were prepared by grinding mixtures of melamine and NaCl, calcining at 520°C, washing, and drying. Characterizations involved XRD, BET, FT-IR, XPS, TGA, TEM, SEM, zeta potential, UV-vis, PL, and photocurrent measurements. Photocatalytic tests were conducted by adding catalyst to model fuel, charging with O2, irradiating with visible light, sampling at intervals, and analyzing with GC or ion chromatography.
5:Data Analysis Methods:
Data were analyzed using standard techniques for each characterization method, with photocatalytic activity evaluated based on removal efficiency of contaminants.
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X-ray diffractometer
D/Max 2400
Rigaku
Recorded powder X-ray diffraction patterns for structural analysis of catalysts.
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FT-IR spectrometer
Nicolet Thermo 360
Thermo
Recorded Fourier transform infrared spectra for chemical bonding analysis.
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Thermal analyzer
Pyris 1
PerkinElmer
Performed thermogravimetric analysis for thermal stability assessment.
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Transmission electron microscope
JEM-2100HR
JEOL
Took TEM images and EDS for morphological and elemental analysis.
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Scanning electron microscope
JSM-7500F
JEOL
Observed SEM images for surface morphology.
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UV-vis spectrometer
JASCO V-770
JASCO
Obtained UV-vis diffuse reflectance spectra for band gap analysis.
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Gas chromatograph
GC-7890B
Agilent
Analyzed reacting solutions for contaminant removal efficiency.
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Surface area analyzer
ASAP 2420
Micrometrics Instruments
Measured BET surface area and BJH pore volume using nitrogen adsorption-desorption method.
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XPS instrument
THERMO
Analyzed elemental compositions and electronic states of elements.
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Zeta potential instrument
ZetaPALS
Brookhaven
Measured zeta potential for surface charge analysis.
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Fluorescence spectrometer
EDAX Orbis PC
EDAX
Recorded photoluminescence spectra for charge carrier recombination analysis.
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Electrochemical workstation
CHI650D
Performed transient photocurrent measurements for photoresponse analysis.
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Xe lamp
300 W
Used as visible light source for photocatalytic reactions.
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Ion-chromatograph
ICS-600
Analyzed inorganic ions in products for mechanistic studies.
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