研究目的
To design and investigate conjugated donor-acceptor polymer photocatalysts with electron-output 'tentacles' for efficient hydrogen evolution from water, focusing on the role of dibenzothiophene-S,S-dioxide units in enhancing photocatalytic performance.
研究成果
The introduction of dibenzothiophene-S,S-dioxide units as electron-output 'tentacles' in donor-acceptor conjugated polymers significantly enhances photocatalytic hydrogen evolution, with P-FSO achieving a high rate of 400 μmol h?1 and an AQY of 8.5%. DFT calculations confirm the sulphonyl group's role in efficient electron output, highlighting the importance of this strategy for optimizing polymer photocatalysts, with potential for further improvements towards overall water splitting.
研究不足
The study uses insoluble polymer solids with no crystallinity, which may limit processability and scalability; residual palladium acts as a co-catalyst, potentially introducing impurities; and the focus is on hydrogen evolution with sacrificial agents, not overall water splitting.
1：Experimental Design and Method Selection:
The study employs a molecular engineering strategy to synthesize donor-acceptor conjugated polymers using Suzuki-Miyaura polycondensation, with DFT calculations for theoretical insights.
2：Sample Selection and Data Sources:
Polymers are synthesized with varying contents of dibenzothiophene-S,S-dioxide (FSO) units, using monomers like pyrene and benzene derivatives.
3：List of Experimental Equipment and Materials:
Instruments include Bruker D8 Advance diffractometer for XRD, BioRad FTS 6000 spectrometer for FTIR, HITACHI SU8010 SEM for morphology, Thermo ESCALAB250 for XPS, Varian Cary 500 Scan for UV-Vis DRS, Edinburgh FI/FSTCSPC 920 spectrophotometer for PL, Micromeritics ASAP 3020 for nitrogen sorption, Bruker Advance III 500 for NMR, and Gaussian 03 for DFT calculations. Materials include various chemicals from Sigma-Aldrich, TCI, and Alfa Aesar.
4：Experimental Procedures and Operational Workflow:
Polymers are synthesized via polycondensation, characterized using the above instruments, and tested for photocatalytic hydrogen evolution in a Pyrex top-irradiation vessel with a 300 W Xe lamp and gas chromatography analysis.
5：Data Analysis Methods:
Data are analyzed using DFT calculations for electronic properties, and photocatalytic performance is evaluated based on hydrogen evolution rates and apparent quantum yields.
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Bruker Advance III 500 spectrometer
Advance III 500
Bruker
Carrying out solid-state Cross-Polarization Magic Angle Spinning 13C NMR experiments.
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Bruker D8 Advance diffractometer
D8 Advance
Bruker
Performing X-ray diffraction measurements with Cu Kα1 radiation.
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HITACHI SU8010 field emission scanning electron microscopy
SU8010
HITACHI
Investigating the morphology of samples.
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Thermo ESCALAB250 instrument
ESCALAB250
Thermo
Obtaining X-ray photoelectron spectroscopy data with a monochromatized Al Kα line source.
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Edinburgh FI/FSTCSPC 920 spectrophotometer
FI/FSTCSPC 920
Edinburgh
Acquiring photoluminescence spectra and time-resolved PL.
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BioRad FTS 6000 spectrometer
FTS 6000
BioRad
Recording Fourier transform infrared spectra.
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Varian Cary 500 Scan UV-visible system
Cary 500 Scan
Varian
Performing UV-Vis diffuse reflectance spectra.
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Micromeritics ASAP 3020 equipment
ASAP 3020
Micromeritics
Conducting nitrogen sorption measurements at 77 K.
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Gaussian 03 program package
03
Gaussian
Performing density functional theory calculations.
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300 W Xe-lamp
Providing light irradiation for photocatalytic tests.
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Newport 2936-R optical power meter
2936-R
Newport
Measuring light intensities for AQY calculations.
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