研究目的
To synthesize carbon and oxygen dual-doped graphitic carbon nitride (MACN) for visible-light photocatalytic mineralization of bisphenol A (BPA), aiming to improve degradation efficiency and mineralization rates compared to pristine CN.
研究成果
The carbon and oxygen dual-doped g-C3N4 (MACN) photocatalyst, synthesized via a facile one-step method, exhibited enhanced visible-light photocatalytic activity for BPA degradation and mineralization due to optimized band structure, improved charge separation, and generation of reactive species. The 1MACN sample showed the highest performance, with a mineralization rate of 52% and efficient degradation, attributed to synergistic effects of C and O doping. This approach provides a promising strategy for environmental remediation of organic pollutants.
研究不足
The study may have limitations in scalability for industrial applications, potential variability in synthesis conditions, and the need for further optimization of doping levels to avoid excessive defects that can act as recombination centers. Environmental factors and long-term stability under real-world conditions were not extensively tested.
1:Experimental Design and Method Selection:
A facile thermal polymerization method was used to synthesize MACN with malonic acid and urea as precursors. The synthesis involved heating in a muffle furnace to 550°C for 4 hours with a heating rate of 2°C/min. Photocatalytic experiments were conducted using a photochemical reactor with a 500 W Xe lamp as the light source, equipped with a 420 nm cutoff filter for visible light experiments.
2:Sample Selection and Data Sources:
Samples included pristine CN and xMACN (x =
3:5, 1, 3, 10, representing weight ratios of malonic acid to urea). Bisphenol A (BPA) at 15 ppm concentration was used as the pollutant. List of Experimental Equipment and Materials:
Equipment included a muffle furnace, photochemical reactor (Xujiang Electromechanical plant), Xe lamp (500 W), high-performance liquid chromatography (HPLC, e2685, Waters), UV-Vis detector (2489, Waters), TEM, SEM, XRD, FT-IR, XPS, UV-Vis DRS, PL, EPR, BET surface area analyzer, and Mott-Schottky measurements. Materials included urea (Sinopharm Chemical Reagent Co., Ltd), malonic acid (TCI), t-butylalcohol (Chengdu Kelon Chemical Reagent Co., Ltd), KI (Shanghai Hushi Laboratorial Equipment Co., Ltd), TEMPOL (Shanghai Hansi Chemical Co., Ltd), DMPO (Sigma-Aldrich Co. LLC), and BPA (Shanghai Aladdin Biochemical Technology Co., Ltd).
4:Experimental Procedures and Operational Workflow:
For synthesis, urea and malonic acid were ground and heated. For photocatalytic tests,
5:02 g catalyst was dispersed in 50 mL BPA solution, stirred for 1 h in dark for adsorption equilibrium, then irradiated. Samples were collected at intervals, filtered, and analyzed by HPLC. Trapping experiments used scavengers for active species. Recycling tests involved centrifugation, washing, and drying of catalyst. Data Analysis Methods:
Data were analyzed using pseudo-first-order kinetic model for degradation rates, Kubelka-Munk method for bandgap calculation, and various characterization techniques for structural and optical properties.
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High performance liquid chromatography
e2685
Waters
Used to evaluate the concentration of BPA in the filtrate during photocatalytic experiments.
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Xe lamp
500 W
Xujiang Electromechanical plant
Served as the light source for photocatalytic experiments, equipped with filters for specific wavelengths.
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Muffle furnace
Used for thermal polymerization synthesis of CN and MACN samples by heating to 550°C.
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TEM
Used to investigate the morphology of CN and MACN samples through transmission electron microscopy.
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SEM
Used to observe the morphologies of CN and MACN samples through scanning electron microscopy.
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XRD
Used to analyze the crystal structure of CN and MACN samples through X-ray diffraction.
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FT-IR
Used to research the chemical bonds and functional groups in CN and MACN samples through Fourier-transform infrared spectroscopy.
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XPS
Used to characterize the oxidation state of elements in CN and MACN samples through X-ray photoelectron spectroscopy.
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UV-Vis DRS
Used to measure the light absorption properties of CN and MACN samples through ultraviolet-visible diffuse reflectance spectroscopy.
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PL
Used to study the photoluminescence properties of CN and MACN samples to understand charge recombination.
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EPR
Used to detect unpaired electrons and active species in CN and MACN samples under light irradiation through electron paramagnetic resonance spectroscopy.
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BET surface area analyzer
Used to measure the specific surface areas of CN and MACN samples.
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Mott-Schottky measurement system
Used to determine the flat band potential and carrier density of CN and MACN samples.
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