研究目的
To design an efficient Si-based photocathode for solar-light-driven conversion of N2 to NH3 under mild conditions, addressing the limitations of poor conversion efficiency and low production rate in photoelectrochemical nitrogen reduction reaction.
研究成果
The aerophilic-hydrophilic heterostructured Si-based photocathode achieves high ammonia yield rate (18.9 mg cm^{-2} hr^{-1}) and faradic efficiency (37.8%) under ambient conditions, demonstrating enhanced N2 reduction by enriching N2 concentration and suppressing HER, with DFT calculations supporting reduced energy barriers.
研究不足
The photocathode shows degradation after long-term electrolysis (e.g., 24 hours) due to loss of Au-PTFE layer and photooxidation of Si substrate. The faradic efficiency decreases with increased reaction time beyond 4 hours, and the system requires specific conditions like acid electrolyte and illumination.
1：Experimental Design and Method Selection:
The study involves fabricating a Si-based photocathode with an aerophilic-hydrophilic heterostructure using Au nanoparticles dispersed in a PTFE porous framework. Methods include magnetron sputtering for Ti and Au deposition, vacuum evaporation for PTFE coating, and various characterization techniques.
2：Sample Selection and Data Sources:
A p-type Si wafer is used as the base material. Samples are prepared with different PTFE thicknesses and Au nanoparticles for comparison.
3：List of Experimental Equipment and Materials:
Equipment includes magnetron sputtering apparatus, vacuum evaporation system, XRD, FTIR, XPS, FESEM, HRTEM, UV-vis spectrophotometer, CA apparatus, PEC system, electrochemical workstation, and DFT calculation tools. Materials include Si wafer, Ti target, PTFE powder, Au target, H2SO4, Na2SO3, and standard solutions for quantification.
4：Experimental Procedures and Operational Workflow:
Steps involve cleaning Si, depositing Ti layer, evaporating PTFE, sputtering Au nanoparticles, encapsulating electrodes, and conducting PEC NRR measurements under illumination with N2 bubbling and stirring.
5：Data Analysis Methods:
Data analysis includes using calibration curves for NH3 and N2H4 quantification, FTIR and NMR for confirmation, and DFT calculations for energy barrier assessment.
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X-ray Diffractometer
Rigaku Ultima IV
Rigaku
Used for XRD analysis to confirm crystalline structure of samples.
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FTIR Spectrometer
Thermo Nicolet is10
Thermo
Used for FTIR analysis to assess compositions and interfacial water molecules.
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XPS Spectrometer
Thermo escalab 250XI
Thermo
Used for XPS analysis to study elemental features and states.
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UV-vis-NIR Spectrophotometer
Hitachi UV-4100
Hitachi
Used for optical transmittance and reflectance measurements.
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ICP-MS
Thermo Scientific iCAP-Q
Thermo Scientific
Used for inductively coupled plasma mass spectrometry to confirm Pt concentration.
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NMR Spectrometer
Bruker AvanceIII HD500
Bruker
Used for 1H nuclear magnetic resonance measurements in isotopic labeling experiments.
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Magnetron Sputtering Apparatus
MSP-3200
Chuangshiweina Co. Ltd.
Used for depositing Ti and Au layers on the Si wafer.
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Vacuum Evaporation System
GSL-1800X-ZF4
Shenyang Kejing Co. Ltd.
Used for fabricating PTFE porous framework by evaporating PTFE powder.
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FESEM
Magellan 400
Not specified
Used for field emission scanning electron microscopy to observe surface and cross section.
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HRTEM
Tecnai G2 F20 S-Twin
Not specified
Used for high-resolution transmission electron microscopy to analyze Au nanoparticles.
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CA Apparatus
JY-82A
Chengde Dingsheng Testing Machine Co. Ltd
Used for contact angle measurements of droplets and bubbles.
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PEC System
PEC 1000
PerfectLight Co. Ltd.
Used for photoelectrochemical measurements under illumination.
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Electrochemical Workstation
CHI 630E
Not specified
Used for controlled potential electrolysis and other electrochemical measurements.
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Ammonia-ammonium ISE
NH3-US
Bante Instruments
Used for ammonia quantification with ion selective electrode.
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