硫化镉/石墨烯复合光催化剂的微波水热合成及DFT研究
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摘要
采用微波水热法制备了CdS/rGO纳米复合光催化剂,通过XRD、FTIR、XPS、SEM、TEM对其结构和形貌进行了表征,结合UV-Vis和密度泛函(DFT)计算对异质界面的电荷转移机制进行了研究。结果表明所得复合材料中CdS分散性好、显示出较高的可见光催化活性和光稳定性。当rGO含量为0.5 mg/mL时复合材料的光催化性能最佳,可见光照射120 min后亚甲基蓝(MB)的光降解率达到94.40%,且五次循环实验光催化效果接近。界面相互作用、差分电荷密度、平均静电势等计算结果表明CdS与rGO通过范德华弱相互作用形成稳定异质界面,电荷由CdS向rGO转移,电子和空穴在两相界面实现了有效分离,因而材料的光催化性能得到增强。
The CdS/rGO nanocomposites were prepared via microwave-hydrothermal process. The structure and morphology of CdS/rGO composites was characterized by XRD, FTIR, XPS, SEM, and TEM. The mechanism of charge transfer for CdS/rGO heterogeneous interface was investigated by UV-Vis spectra combined density functional theory(DFT) calculations. The results indicated that the CdS in CdS/rGO displayed good dispersion, high photocatalytic activity, and excellent light stability. When the content of rGO was 0.5 mg/mL, the composite exhibited the best photocatalytic activity. The photodegradation rate of methylene blue(MB) reached 94.40 % after 120 min in visible light and the composite had the similar photocatalytic performance during five cycles. The DFT calculations such as interfacial interaction, charge density difference, ave-rage electrostatic potential et al revealed that the hetero-interface between CdS and rGO formed via van der Waals' interaction, which resulted in stabilization of composites. The introduction of rGO promoted the efficient transport of photo-induced electrons from CdS to the rGO, and gave rise to spatial separation of photo-generated electrons and holes. Hence, the enhancement of photocatalytic performance was observed.
The CdS/rGO nanocomposites were prepared via microwave-hydrothermal process. The structure and morphology of CdS/rGO composites was characterized by XRD, FTIR, XPS, SEM, and TEM. The mechanism of charge transfer for CdS/rGO heterogeneous interface was investigated by UV-Vis spectra combined density functional theory(DFT) calculations. The results indicated that the CdS in CdS/rGO displayed good dispersion, high photocatalytic activity, and excellent light stability. When the content of rGO was 0.5 mg/mL, the composite exhibited the best photocatalytic activity. The photodegradation rate of methylene blue(MB) reached 94.40 % after 120 min in visible light and the composite had the similar photocatalytic performance during five cycles. The DFT calculations such as interfacial interaction, charge density difference, ave-rage electrostatic potential et al revealed that the hetero-interface between CdS and rGO formed via van der Waals' interaction, which resulted in stabilization of composites. The introduction of rGO promoted the efficient transport of photo-induced electrons from CdS to the rGO, and gave rise to spatial separation of photo-generated electrons and holes. Hence, the enhancement of photocatalytic performance was observed.
引文
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29 Vanderbilt D.Physical Review B Condensed Matter,1990,41(11),7892.
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43 Geng W,Zhao X,Liu H,et al.Journal of Physical Chemistry C,2013,117(20),10536.