Fagan Rachel, McCormack Declan E, Hinder Steven J, Pillai Suresh C
Centre for Research in Engineering Surface Technology (CREST), FOCAS Institute, Dublin Institute of Technology, Kevin St, Dublin 8, Ireland.
School of Chemical and Pharmaceutical Sciences, Dublin Institute of Technology, Kevin St., Dublin 8, Ireland.
Materials (Basel). 2016 Apr 14;9(4):286. doi: 10.3390/ma9040286.
Graphitic carbon nitride (-C₃N₄) and titanium dioxide (TiO₂) were chosen as a model system to investigate photocatalytic abilities of heterojunction system under UV and visible light conditions. The use of -C₃N₄ has been shown to be effective in the reduction in recombination through the interaction between the two interfaces of TiO₂ and -C₃N₄. A simple method of preparing -C₃N₄ through the pyrolysis of melamine was employed, which was then added to undoped TiO₂ material to form the -C₃N₄-TiO₂ system. These materials were then fully characterized by X-ray diffraction (XRD), Brunauer Emmett Teller (BET), and various spectroscopic techniques including Raman, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), diffuse absorbance, and photoluminescence analysis. Photocatalysis studies were conducted using the model dye, rhodamine 6G utilizing visible and UV light irradiation. Raman spectroscopy confirmed that a composite of the materials was formed as opposed to a mixture of the two. Using XPS analysis, a shift in the nitrogen peak to that indicative of substitutional nitrogen was detected for all doped samples. This is then mirrored in the diffuse absorbance results, which show a clear decrease in band gap values for these samples, showing the effective band gap alteration achieved through this preparation process. When -C₃N₄-TiO₂ samples were analyzed under visible light irradiation, no significant improvement was observed compared that of pure TiO₂. However, under UV light irradiation conditions, the photocatalytic ability of the doped samples exhibited an increased reactivity when compared to the undoped TiO₂ (0.130 min), with 4% -C₃N₄-TiO₂ (0.187 min), showing a 43.9% increase in reactivity. Further doping to 8% -C₃N₄-TiO₂ lead to a decrease in reactivity against rhodamine 6G. BET analysis determined that the surface area of the 4% and 8% -C₃N₄-TiO₂ samples were very similar, with values of 29.4 and 28.5 m²/g, respectively, suggesting that the actual surface area is not a contributing factor. This could be due to an overloading of the system with covering of the active sites resulting in a lower reaction rate. XPS analysis showed that surface hydroxyl radicals and oxygen vacancies are not being formed throughout this preparation. Therefore, it can be suggested that the increased photocatalytic reaction rates are due to successful interfacial interactions with the -C₃N₄-doped TiO₂ systems.
选择石墨相氮化碳(-C₃N₄)和二氧化钛(TiO₂)作为模型体系,以研究异质结体系在紫外光和可见光条件下的光催化能力。已证明使用-C₃N₄可通过TiO₂和-C₃N₄的两个界面之间的相互作用有效减少复合。采用了一种通过三聚氰胺热解制备-C₃N₄的简单方法,然后将其添加到未掺杂的TiO₂材料中以形成-C₃N₄-TiO₂体系。然后通过X射线衍射(XRD)、布鲁诺尔-埃米特-泰勒(BET)以及包括拉曼光谱、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)、漫反射吸收和光致发光分析在内的各种光谱技术对这些材料进行全面表征。使用模型染料罗丹明6G在可见光和紫外光照射下进行光催化研究。拉曼光谱证实形成了材料的复合物,而不是两者的混合物。通过XPS分析,在所有掺杂样品中均检测到氮峰向指示取代氮的方向移动。这在漫反射吸收结果中得到反映,结果显示这些样品的带隙值明显降低,表明通过该制备过程实现了有效的带隙改变。当在可见光照射下分析-C₃N₄-TiO₂样品时,与纯TiO₂相比未观察到显著改善。然而,在紫外光照射条件下,与未掺杂的TiO₂(0.130分钟)相比,掺杂样品的光催化能力表现出更高的反应活性,4%-C₃N₄-TiO₂(0.187分钟)的反应活性提高了43.9%。进一步掺杂至8%-C₃N₄-TiO₂导致对罗丹明6G的反应活性降低。BET分析确定4%和8%-C₃N₄-TiO₂样品的表面积非常相似,分别为29.4和28.5 m²/g,这表明实际表面积不是一个影响因素。这可能是由于体系过载,活性位点被覆盖,导致反应速率降低。XPS分析表明在整个制备过程中未形成表面羟基自由基和氧空位。因此,可以认为光催化反应速率的提高是由于与-C₃N₄掺杂的TiO₂体系成功的界面相互作用。