研究目的
To apply co-modification of ALD-coated MgO and photodeposited Ag nanoparticles on porous TiO2 and investigate the correlations between the nanostructure of MgO/Ag co-modification and the photocatalytic activity on CO2 reduction.
研究成果
The co-modification of porous TiO2 with ALD-coated MgO and photodeposited Ag nanoparticles synergistically enhances CO2 photoreduction activity, with up to 14 times improvement over pristine TiO2. The sequence of modification affects performance, with Ag on the outermost layer (Ag/MgO/TiO2) being more active due to better Ag distribution. The work highlights the importance of nanostructure optimization for efficient photocatalysis.
研究不足
The study is limited by the inability to detect MgO or Ag phases clearly in XRD and TEM due to low amounts or amorphous nature. The Ag nanoparticle size and distribution were challenging to characterize, and the optimal MgO thickness was trade-off dependent, potentially limiting generalization. The experiments were conducted under specific conditions (e.g., UV-vis light, fixed Ag content), which may not cover all operational scenarios.
1:Experimental Design and Method Selection:
The study involved synthesizing porous TiO2 from MIL-125 MOF, modifying it with MgO via ALD and Ag nanoparticles via photodeposition in different sequences (Ag/MgO/TiO2 and MgO/Ag/TiO2). The rationale was to explore synergistic effects on CO2 photoreduction. Methods included ALD for uniform MgO coating and photodeposition for Ag nanoparticle deposition.
2:2). The rationale was to explore synergistic effects on CO2 photoreduction. Methods included ALD for uniform MgO coating and photodeposition for Ag nanoparticle deposition. Sample Selection and Data Sources:
2. Sample Selection and Data Sources: Samples included pristine TiO2, single-modified TiO2 (with MgO or Ag), and co-modified TiO2 with varying MgO layers (1-10 ALD cycles) and fixed Ag content (5 wt.%). Data sources were experimental measurements from characterization and performance tests.
3:List of Experimental Equipment and Materials:
Equipment included ALD system (Ultratech Savannah S200), UV lamp (100 W, 365 nm), Xe lamp (450 W), XRD (Bruker-AXS D8 Advance), SEM (JEOL JSM7500F), TEM (FEI Tecnai G2 F20 ST), XPS (Omicron XPS system), UV-vis spectrophotometer (Hitachi U4100), photoluminescence spectrometer (PTI QuantaMaster), GC (Shimadzu GC-2014ATF), potentiostat (Gamry Reference 3000). Materials included TiO2, Mg precursor (bis(ethylcyclopentadienyl) magnesium), AgNO3, glass fiber filter paper, CO2 gas, etc.
4:0). Materials included TiO2, Mg precursor (bis(ethylcyclopentadienyl) magnesium), AgNO3, glass fiber filter paper, CO2 gas, etc. Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: Procedures included synthesis of TiO2, ALD coating of MgO, photodeposition of Ag, calcination, characterization (XRD, SEM, TEM, XPS, UV-vis, PL), CO2 photoreduction testing (with gas flow and irradiation), and electrochemical measurements (photocurrent, EIS).
5:Data Analysis Methods:
Data analysis involved calculating product yields, promotion factors, electron numbers, and using techniques like Rietveld refinement for XRD, deconvolution for XPS, and impedance analysis for EIS.
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X-ray Diffractometer
D8 Advance
Bruker-AXS
Used for XRD analysis of photocatalyst samples.
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Field-Emission Scanning Electron Microscope
JSM7500F
JEOL
Used for morphology analysis of samples.
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Transmission Electron Microscope
Tecnai G2 F20 ST
FEI
Used for high-resolution TEM analysis of nanostructures.
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UV-vis-NIR Spectrophotometer
U4100
Hitachi
Used for UV-vis diffuse reflectance spectra measurements.
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Gas Chromatograph
GC-2014ATF
Shimadzu
Used for measuring effluent gas composition during CO2 photoreduction.
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Atomic Layer Deposition System
Savannah S200
Ultratech
Used for coating an ultrathin MgO layer on pristine TiO2 powder.
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UV Lamp
100 W, 365 nm
Used for photodeposition of Ag nanoparticles on TiO2.
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X-ray Photoelectron Spectroscopy System
Omicron
Used for surface chemical states and compositions analysis.
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Spectrofluorometer
QuantaMaster series
PTI
Used for photoluminescence spectra to investigate charge recombination.
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Potentiostat
Reference 3000
Gamry
Used for transient photocurrent density and electrochemical impedance spectroscopy measurements.
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Xe Lamp
450 W
Newport, Inc.
Used as light source for CO2 photoreduction and electrochemical measurements.
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Glass Fiber Filter Paper
Pall Corporation
Used as support for powder photocatalyst in CO2 photoreduction tests.
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CO2 Gas
Ultra-high purity, 99.999%
Airgas
Used as reactant gas for CO2 photoreduction.
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Mg Precursor
Bis(ethylcyclopentadienyl) magnesium, min. 98%
Strem Chemicals Inc.
Used as Mg precursor in ALD process for MgO coating.
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