研究目的
Investigating the photocatalytic hydrogen production using Pd-doped mesoporous TiO2 and ethanol as an organic scavenger under near-UV light, with a focus on optimizing metal loadings and evaluating quantum yields.
研究成果
Pd-doped TiO2 photocatalysts, particularly at 1.00 wt% loading, demonstrated high hydrogen production rates and quantum yields (up to 30.8%) under near-UV light, with zero-order kinetics and no deactivation over 24 hours. The macroscopic radiation energy balance provided accurate efficiency measurements, and Pd was found to be a cost-effective alternative to Pt. Future work could focus on enhancing Pd reduction and optimizing conditions for higher efficiencies.
研究不足
The study is limited to near-UV light irradiation and specific reactor conditions (Photo-CREC Water II). Higher Pd loadings (above 1.00 wt%) showed reduced performance due to increased backscattering and poorer metal dispersion. The use of ethanol as a sacrificial agent may not be optimal for all applications, and scalability to industrial levels was not addressed.
1:Experimental Design and Method Selection:
The study employed a sol-gel method for synthesizing Pd-doped TiO2 photocatalysts using a Pluronic F-127 soft template to enhance morphological properties. Photocatalytic experiments were conducted in the Photo-CREC Water II reactor system to measure hydrogen production under near-UV light irradiation, with macroscopic radiation energy balances used for precise photon absorption calculations.
2:Sample Selection and Data Sources:
Photocatalysts were prepared with Pd loadings ranging from 0.25 to 5.00 wt%. Ethanol (2.0 v/v%) was used as the sacrificial agent. Data were collected from repeated experiments (at least three times) to ensure reproducibility, with gas and liquid samples analyzed using gas chromatography and HPLC.
3:25 to 00 wt%. Ethanol (0 v/v%) was used as the sacrificial agent. Data were collected from repeated experiments (at least three times) to ensure reproducibility, with gas and liquid samples analyzed using gas chromatography and HPLC. List of Experimental Equipment and Materials:
3. List of Experimental Equipment and Materials: Equipment includes the Photo-CREC Water II reactor, BET surface area analyzer (Micromeritics ASAP 2010), pulse chemisorption unit (Micromeritics AutoChem II Analyzer), X-ray diffractometer (Rigaku Rotating Anode), UV-VIS-NIR spectrophotometer (Shimadzu UV-3600), XPS analyzer, gas chromatograph (Shimadzu GC2010), and HPLC system (Shimadzu UFLC). Materials include ethanol, hydrochloric acid, Pluronic F-127, citric acid, titanium(IV) isopropoxide, palladium(II) chloride, and argon gas.
4:Experimental Procedures and Operational Workflow:
Photocatalysts were synthesized via sol-gel method, calcined at 500°C, and characterized for surface area, pore size, crystallite size, band gap, and chemical composition. Hydrogen production experiments were conducted in the Photo-CREC Water II reactor with controlled conditions (photocatalyst concentration, ethanol concentration, pH, atmosphere). Radiation measurements were taken using a spectrometer, and samples were analyzed periodically over 6 hours of irradiation.
5:Data Analysis Methods:
Data were analyzed using BET and BJH methods for surface area and pore size, Scherrer equation for crystallite size, Tauc plot for band gap, and macroscopic radiation energy balance for photon absorption rates. Quantum yields were calculated based on hydrogen production rates and absorbed photons, with statistical analysis for standard deviations.
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X-ray diffractometer
Rotating Anode X-Ray Diffractometer
Rigaku
Identifying crystalline phases and determining crystallite sizes of photocatalysts using XRD analysis.
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UV-VIS-NIR spectrophotometer
UV-3600
Shimadzu
Measuring band gaps of photocatalysts using UV-VIS absorption spectroscopy with BaSO4 as reference.
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Gas chromatograph
GC2010
Shimadzu
Analyzing gas phase products (e.g., H2, CO2, CH4) from photocatalytic reactions using FID and TCD detectors.
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HPLC system
UFLC
Shimadzu
Characterizing liquid phase components (e.g., ethanol concentration) using refractive index detection.
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UV lamp
BLB
Ushio
Providing near-UV light irradiation (300-420 nm range) for photocatalytic reactions in the reactor.
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BET surface area analyzer
ASAP 2010
Micromeritics
Determining specific surface area and pore size distribution of photocatalysts using nitrogen adsorption-desorption isotherms.
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Pulse chemisorption unit
AutoChem II Analyzer
Micromeritics
Calculating metal dispersion and average crystallite size for doped photocatalysts.
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Spectrometer
EPP2000-25
StellarNet
Measuring emitted radiation spectra of the near-UV lamp for photon energy calculations.
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Photo-CREC Water II reactor
CREC-UWO
Conducting photocatalytic water splitting experiments with hydrogen storage and symmetrical irradiation capabilities.
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