研究目的
To explore efficient photocatalysts for N2 reduction reaction (NRR) by building Z-scheme heterostructures of 0D AgInS2 nanoparticles and 2D MXene (Ti3C2) nanosheets.
研究成果
The 0D/2D AgInS2/Ti3C2 Z-scheme nanosheets, particularly with 30 wt% AgInS2, achieved high photocatalytic N2 fixation rates (38.8 μmol/(g·h)) under visible light, attributed to efficient charge separation, Schottky junction formation, and enhanced N2 adsorption. DFT calculations confirmed N2 activation with high adsorption energy and bond elongation. This work demonstrates MXene's potential as a cost-effective co-catalyst for N2 reduction, with implications for sustainable ammonia production.
研究不足
The study notes that the efficiency of N2 reduction is low due to high energy requirements for N≡N bond cleavage and poor interfacial charge transfer. The photocatalytic performance decreased after multiple cycles, indicating stability issues. The band gap of Ti3C2 is too low for sufficient N2 reduction energy, and excess AgInS2 led to reduced performance due to photosensitization effects.
1:Experimental Design and Method Selection:
The study involved designing 0D/2D AgInS2/Ti3C2 Z-scheme heterojunctions via hydrothermal synthesis to enhance charge separation and N2 fixation. Theoretical models included DFT calculations for adsorption energies and band alignment analysis.
2:Sample Selection and Data Sources:
Samples were synthesized with varying mass ratios of AgInS2 to Ti3C2 (10-50 wt%), labeled AT-10 to AT-50. Data sources included experimental measurements of photocatalytic performance and computational simulations.
3:Data sources included experimental measurements of photocatalytic performance and computational simulations. List of Experimental Equipment and Materials:
3. List of Experimental Equipment and Materials: Equipment included X-ray diffractometer (XRD, D8 Advance), XPS (Thermo ESCALAB 250XI), FESEM (Hitachi SU8010), TEM (JEOL 2100), UV-vis spectrophotometer (JASCO UV-550), PL spectrophotometer (Hitachi F-4500), FS5 fluorescence lifetime spectrophotometer (Edinburgh Instruments), CHI 760E electrochemical workstation, and 300 W Xe lamp (CEL-HXF300). Materials included Ti3AlC2 powder, AgNO3, In(OAC)3·6H2O, thioacetamide, L-cysteine, HF, methanol, and others as listed.
4:0). Materials included Ti3AlC2 powder, AgNO3, In(OAC)3·6H2O, thioacetamide, L-cysteine, HF, methanol, and others as listed. Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: Ti3C2 nanosheets were prepared by etching Ti3AlC2 with HF, followed by hydrothermal synthesis of AgInS2/Ti3C2 composites. Photocatalytic tests involved dispersing samples in methanol solution under N2 atmosphere, irradiating with visible light, and measuring NH4+ concentration via indophenol blue method. Characterization included XRD, XPS, TEM, UV-Vis DRS, PL, EIS, and photocurrent measurements.
5:Data Analysis Methods:
Data analysis involved Tauc's plot for band gap calculation, exponential decay kinetics for PL lifetime, Nyquist plots for EIS, and DFT simulations for adsorption energies and charge density differences using CASTEP with PBE-GGA and PAW potential.
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X-ray photoelectron spectroscopy
Thermo ESCALAB 250XI
Thermo
Analyzing surface compositions and valence states
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Field emission scanning electron microscopy
SU8010
Hitachi
Analyzing morphology of synthesized samples
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Transmission electron microscopy
JEOL 2100
JEOL
Observing microstructures of samples
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UV-vis absorption spectrophotometer
UV-550
JASCO
Recording UV-Vis diffuse reflection spectra
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Fluorescence spectrophotometer
F-4500
Hitachi
Investigating photoluminescence properties
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Fluorescence lifetime spectrophotometer
FS5
Edinburgh Instruments
Measuring time-resolved transient PL decay curves
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X-ray diffractometer
D8 Advance
Determining crystal structure of samples
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Electrochemical workstation
CHI 760E
Shanghai Chenhua
Performing electrochemical measurements
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Xe lamp
CEL-HXF300
Providing visible light irradiation for photocatalytic tests
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Teflon-lined autoclave
Used for hydrothermal synthesis of composites
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