研究目的
To achieve direct functionalization of methane into ethanol over copper-modified polymeric carbon nitride via photocatalysis under mild conditions, addressing the challenge of deep mineralization and low selectivity in methane conversion.
研究成果
The introduction of Cu species into PCN enables efficient photocatalytic anaerobic methane conversion to ethanol with a productivity of 106 μmol gcat?1 h?1, avoiding deep mineralization through managed ·OH production and methane activation. The synergy between Cu species and adjacent C atoms in PCN facilitates the methane-methanol-ethanol pathway, offering a green strategy for methane valorization under mild conditions.
研究不足
The study is limited to laboratory-scale experiments under controlled conditions; scalability and long-term stability of the photocatalyst are not fully addressed. Potential coke deposition and ethanol production decay over time are noted as areas for optimization.
1：Experimental Design and Method Selection:
The study involves designing a photocatalyst by modifying polymeric carbon nitride (PCN) with Cu species to manage H2O2 generation and decomposition for ·OH production, and to serve as active sites for methane adsorption and activation. Theoretical models include radical mechanisms and band structure alignments.
2：Sample Selection and Data Sources:
Samples include PCN and Cu-X/PCN (X = theoretical weight percentage of Cu) prepared by thermal condensation of urea with copper chloride. Methane gas is used as the reactant.
3：List of Experimental Equipment and Materials:
Equipment includes X-ray diffractometer, FTIR spectrometer, TEM, XPS, ESR spectrometer, DRS spectrophotometer, in situ IR spectrometer, TPD analyzer, electrochemical workstation, gas chromatographer, and photochemical reactor with Xe-lamp. Materials include urea, copper chloride, deionized water, methane, nitrogen, and various chemicals for detection methods.
4：Experimental Procedures and Operational Workflow:
Photocatalysts are prepared, characterized, and tested for H2O2 and ·OH production, methane adsorption, and photocatalytic methane conversion in liquid-solid dynamic and gas-solid static conditions under visible light irradiation.
5：Data Analysis Methods:
Data are analyzed using XRD, FTIR, TEM, XPS, ESR, DRS, in situ IR, TPD, electrochemical measurements, gas chromatography, and spectrophotometry.
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X-ray diffractometer
MiniFlex II
Rigaku
Collecting X-ray diffraction patterns for structural characterization of photocatalysts.
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Transmission electron microscope
JEM-2100F
JEOL
Investigating morphology and microstructure of samples.
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XPS microprobe
ESCALAB 250Xi
Thermo Fisher
Performing X-ray photoelectron spectroscopy measurements for valence state and bonding analysis.
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ESR spectrometer
JES-FA200
JEOL
Achieving electron spin resonance spectra for detailed analysis of Cu species.
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Spectrophotometer
U-3010
Hitachi
Measuring diffuse reflectance spectra and absorbance for optical characterization.
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Spectrophotometer
F-4600
Hitachi
Measuring fluorescence spectra for hydroxyl radical detection.
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FTIR spectrometer
Lambda FTIR-7600
Recording Fourier transform infrared spectra for chemical structure analysis.
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FTIR spectrometer
Nicolet iS10
Recording in situ IR spectra for methane adsorption studies.
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Chemisorption analyzer
AutoChem II 2920
Performing methane temperature programmed desorption for adsorption analysis.
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Electrochemical workstation
CHI 660D
Chenhua
Conducting electrochemical analyses including Mott-Schottky plots.
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Gas chromatographer
GC7900
Techcomp
Analyzing liquid and gas phase products of photocatalytic reactions.
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Gas chromatographer
GC7890II
Techcomp
Determining hydrogen amount in gas phase products.
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Xe-lamp
500 W
Providing illumination for photocatalytic experiments.
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