研究目的
To achieve direct overall pure water splitting using visible light excited graphitic carbon nitride incorporated with conjugated aromatic rings without sacrificial agents.
研究成果
Benzene-doped g-C3N4 shows enhanced photocatalytic performance for overall water splitting under visible light due to extended conjugation, reduced band gap, improved charge separation, and higher surface area, with stable activity over multiple cycles.
研究不足
The hydrogen yield from BD-CN is very poor, and the study is limited to specific aromatic ring incorporations; scalability and practical application challenges may exist.
1:Experimental Design and Method Selection:
The study involved synthesizing modified graphitic carbon nitride (g-C3N4) polymers by copolymerizing melamine with 2,4,6-triaminopyrimidine (TAP) or 1,3,5-triaminobenzene (TAB) to incorporate pyrimidine and benzene rings, respectively. The synthesis was conducted at 550°C for 5 hours. Characterization included structural, morphological, optical, and electronic analyses using various techniques. Photocatalytic water splitting experiments were performed under visible light irradiation without sacrificial reagents, with Pt as a cocatalyst. Computational methods using DFT were employed to understand electronic properties and reaction mechanisms.
2:Sample Selection and Data Sources:
Samples included unmodified g-C3N4 (CN), pyrimidine-doped CN (PD-CN), and benzene-doped CN (BD-CN). Data were obtained from experimental measurements and theoretical calculations.
3:List of Experimental Equipment and Materials:
Equipment included Bruker AXS D8 advanced diffractometer for XRD, JEOL JEM 3010 for HRTEM, BRUKER RFS 27 for Raman spectroscopy, JASCO FT-IR-4100 for FTIR, JASCO V-660 UV-vis spectrophotometer for UV-Vis DRS, Micrometrics ASAP 2020 for BET surface area, JEOL model JES FA200 for EPR, JASCO FT-6300 for photoluminescence, Scienta R3000HP for XPS, Oriel 300 W Xe lamp for photocatalytic experiments, and Shimadzu GC-2014 chromatograph for gas analysis. Materials included melamine, TAP, TAB, H2PtCl6·6H2O, and pure water.
4:Experimental Procedures and Operational Workflow:
Synthesis involved grinding and heating mixtures of melamine with TAP or TAB. Characterization steps included XRD, SEM, TEM, Raman, FTIR, UV-Vis, BET, EPR, PL, XPS, and photocatalytic testing with light irradiation and gas chromatography.
5:Data Analysis Methods:
Data were analyzed using software like QUANTUM ESPRESSO and Gaussian 09 for DFT calculations, with statistical methods for photocatalytic efficiency calculations such as AQY, TON, and TOF.
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Bruker AXS D8 advanced diffractometer
D8
Bruker
Used for powder XRD analysis to determine crystal structure.
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JEOL JEM 3010
JEM 3010
JEOL
Used for high resolution transmission electron microscopy (HRTEM) to analyze morphology.
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BRUKER RFS 27 laser confocal FT-Raman spectrometer
RFS 27
BRUKER
Used for Raman spectroscopy to examine molecular structures.
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JASCO FT-IR-4100 spectrophotometer
FT-IR-4100
JASCO
Used for FTIR analysis to confirm chemical bonds.
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JASCO V-660 UV-vis spectrophotometer
V-660
JASCO
Used for UV-visible diffused reflectance spectra to determine optical properties.
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JEOL model JES FA200 ESR spectrometer
JES FA200
JEOL
Used for electron paramagnetic resonance (EPR) spectra to analyze electron mobility.
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JASCO FT-6300 spectrophotometer
FT-6300
JASCO
Used for photoluminescence measurements.
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Shimadzu GC-2014 chromatograph
GC-2014
Shimadzu
Used for gas chromatography to analyze evolved hydrogen and oxygen gases.
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Micrometrics ASAP 2020 apparatus
ASAP 2020
Micrometrics
Used for BET surface area analysis.
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Scienta R3000HP
R3000HP
Scienta
Used for X-ray photoelectron spectra (XPS) to analyze chemical environment.
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Oriel 300 W Xe lamp
300 W
Oriel
Used as light source for photocatalytic experiments.
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