Catalytic performance of CuO/g-C3N4 composites for carbamazepine degradation
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摘要: 本研究采用煅烧法制备了CuO/g-C3N4复合材料，利用SEM-EDS、FT-IR、XRD、XPS分析其表面形貌、晶体结构以及元素价态等特征。选择卡马西平为目标污染物，探究CuO/g-C3N4复合材料应用于类芬顿体系的催化性能。试验结果显示，当卡马西平初始浓度为20 mg/L，在Cu的复合量7%，CuO/g-C3N4投加量2 g/L，H2O2投加量147 mmol/L的条件下，卡马西平的去除率最高，约为96.59%。该类Fenton体系不受溶液pH的限制，且CuO/g-C3N4材料具有较好的稳定性，五次重复实验后卡马西平的去除率仍高达94.23%。∙OH和1O2是催化过程的主要活性物种。CuO/g-C3N4与H2O2之间的电子交换导致Cu(II)/Cu(I)氧化还原过程的持续发生，进而分解H2O2产生大量的活性基团攻击CBZ分子，促进其降解。Abstract: In this study, CuO/g-C3N4 composites were prepared by a calcination method, and were characterized by Scanning Electron Microscope (SEM)-Energy Dispersive Spectrometer (EDS), Fourier Transform Infrared spectroscopy (FT-IR), X-Ray Diffraction (XRD) and X-ray Photoelectron Spectroscopy (XPS) to analyze the surface morphology, crystal structure and valence state of CuO/g-C3N4, respectively. Carbamazepine was selected as the target pollutant to explore the catalytic performance of CuO/g-C3N4 composites in Fenton-like systems. The results show that when the initial concentration of CBZ is 20 mg/L, Cu composite amount is 7%, CuO/g-C3N4 dosage is 2 g/L and H2O2 dosage is 147 mmol/L, the removal rate of CBZ is the highest, which is about 96.59%. The Fenton-like reaction is not limited by solution pH, and the catalyst presents good stability. After five cycles, the removal rate of CBZ is still as high as 94.23%. ∙OH and 1O2 are the main active species detected in the catalytic process. The electron exchanges between CuO/g-C3N4 and H2O2 lead to the continuous occurrence of Cu (II)/Cu (I) redox process, which in turn decompose H2O2 to produce a large number of active groups to attack CBZ molecules and promote their degradation.
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Key words:
- CuO /
- carbon nitride /
- Fenton-like reaction /
- carbamazepine /
- molecular simulation
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图 1 (a) CuO/g-C3N4材料的SEM图；(b) CuO/g-C3N4材料的EDS图
Figure 1. (a) Scanning Electron Microscope of CuO/g-C3N4 composites; (b) Energy Dispersive Spectrometer diagram of CuO/g-C3N4 composites
图 2 (a) g-C3N4和CuO/g- C3N4的FT-IR谱图；(b) XRD谱图
Figure 2. (a) Fourier Transform Infrared Spectroscopy spectra; (b) X-ray Diffraction pattern of g-C3N4 and CuO/g-C3N4
图 4 Cu复合量对CBZ去除率的影响
Figure 4. The effect of Cu composite amount on the removal rate of CBZ
(Experimental condition: CBZ: 20 mg/L; CuO/g-C3N4 dosage: 2 g/L; H2O2 dosage: 147 mmol/L; solution pH: unadjusted; reaction time: 60 min)
图 5 CuO/g-C3N4投加量对CBZ去除率的影响
Figure 5. The effect of CuO/g-C3N4 dosage on the removal rate of CBZ
(Experimental condition: CBZ: 20 mg/L; H2O2 dosage: 147 mmol/L; solution pH: unadjusted; reaction time: 60 min)
图 6 H2O2投加量对CBZ去除率的影响
Figure 6. The effect of H2O2 dosage on the removal rate of CBZ
(Experimental condition: CBZ: 20 mg/L; CuO/g-C3N4 dosage: 2 g/L; solution pH: unadjusted; reaction time: 60 min)
图 7 溶液pH对CBZ去除率的影响
Figure 7. The effect of solution pH on the removal rate of CBZ
(Experimental condition: CBZ: 20 mg/L; CuO/g-C3N4 dosage: 2 g/L; H2O2 dosage: 147 mmol/L; reaction time: 60 min)
图 8 CuO/g-C3N4复合材料的稳定性
Figure 8. Stability of CuO/g-C3N4 composites
(Experimental condition: CBZ: 20 mg/L; CuO/g-C3N4 dosage: 2 g/L; H2O2 dosage: 147 mmol/L; solution pH: unadjusted; reaction time: 60 min)
图 9 (a) CuO/g-C3N4的降解动力学曲线；(b) CuO/g-C3N4的TOC测试浓度
Figure 9. (a) Kinetics of CBZ degradation of CuO/g-C3N4; (b) TOC concentration of CuO/g-C3N4
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