研究目的
To investigate the use of sulfur and nitrogen codoped graphene oxide dots (SNGODs) as environmentally benign photocatalysts for reforming sugar and glucose into hydrogen under visible light irradiation, aiming to achieve a sustainable carbon cycle and enhance catalytic activity through structural tuning.
研究成果
The SNGODs, with quaternary nitrogen repairing defects and peripheral groups enhancing charge separation, demonstrated high photocatalytic activity for H2 production from sugar and glucose, with AQYs up to 11% under 420 nm light. This work establishes carbon-based photocatalysts as superior, environmentally benign alternatives for biomass reforming, offering a sustainable approach for hydrogen energy production.
研究不足
The study is limited to laboratory-scale experiments with specific biomass substrates (sugar and glucose); scalability and applicability to other biomass types or real-world conditions are not addressed. The use of Pt cocatalyst adds cost, and long-term stability beyond 80 hours is not thoroughly tested. The quantum yield decreases with longer wavelengths, indicating inefficiency in broader solar spectrum utilization.
1:Experimental Design and Method Selection:
The study involved synthesizing SNGODs through sequential annealing of graphene oxide with sulfur and ammonia, exfoliation into dots, and autoclaving in ammonia solution. Photocatalytic activity was assessed in a gas-enclosed system under visible light irradiation.
2:Sample Selection and Data Sources:
Catalysts included SNGODs, NGODs (nitrogen-doped only), and SGODs (sulfur-doped only) for comparison. Sugar and glucose aqueous solutions (0.35 mol L?1) were used as biomass substrates.
3:35 mol L?1) were used as biomass substrates. List of Experimental Equipment and Materials:
3. List of Experimental Equipment and Materials: Equipment included XPS (AXIS Ultra DLD, Kratos), TEM (Jeol 2100F), Raman microscope (DXR, Thermo Fisher), FTIR spectrometer (Nicolet 6700, Thermo Fisher), UV-Vis spectrophotometer (Hitachi U-4100), UPS (Sigma Probe, Thermo VG Scientific), EPR spectrometer (Magnettech MS5000), PL spectrophotometer (F-700, Hitachi), spectrofluorometer (FS5, Edinburgh Instruments), gas chromatography (Hewlett-Packard 7890), and photocatalytic reaction system with Xenon lamp (Oriel Instruments, model 66901). Materials included natural graphite powder (Bay carbon, SP-1), sulfur powder (Acros), ammonia solution (Sigma-Aldrich), H2PtCl6·6H2O (Alfa Aesar), and chemicals from various suppliers.
4:1). Materials included natural graphite powder (Bay carbon, SP-1), sulfur powder (Acros), ammonia solution (Sigma-Aldrich), H2PtCl6·6H2O (Alfa Aesar), and chemicals from various suppliers. Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: Synthesis involved modified Hummers' method for GO, annealing at 600°C with S and NH3, oxidation with HNO3, ultrasonication, autoclaving in ammonia, and Pt deposition. Photocatalytic reactions were conducted at pH 10 with light irradiation (420–800 nm or monochromatic), and H2 production was measured over time.
5:Data Analysis Methods:
XPS spectra were decomposed using Gaussian fitting, PL decay curves were fitted with bi-exponential functions, and AQY was calculated based on incident photons and evolved H2 molecules.
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XPS
AXIS Ultra DLD
Kratos
Quantitative analysis of chemical composition
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TEM
Jeol 2100F
Jeol
Determination of microstructure
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Raman microscope
DXR
Thermo Fisher Scientific
Recording Raman spectra
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FTIR spectrometer
Nicolet 6700
Thermo Fisher Scientific
Recording FTIR spectra
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UV-Vis spectrophotometer
Hitachi U-4100
Hitachi
Optical absorption analysis
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PL spectrophotometer
F-700
Hitachi
Measuring PL spectra
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Spectrofluorometer
FS5
Edinburgh Instruments
PL lifetime determination
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UPS
Sigma Probe
Thermo VG Scientific
Determination of valence band edges
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EPR spectrometer
Magnettech MS5000
Magnettech
Recording EPR spectra
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Gas chromatography
Hewlett-Packard 7890
Hewlett-Packard
Determination of H2 quantity
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Xenon lamp
Oriel Instruments model 66901
Oriel Instruments
Light source for photocatalytic reactions
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Photodetector
Oriel Instrument model 71964
Oriel Instrument
Determining light intensity
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Natural graphite powder
SP-1
Bay carbon
Starting material for GO synthesis
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Sulfur powder
Acros
Doping agent
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Ammonia solution
Sigma-Aldrich
Doping and autoclaving agent
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H2PtCl6·6H2O
Alfa Aesar
Source for Pt cocatalyst deposition
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