Department of Chemistry, Nanchang University, Nanchang 330031, China.
Phys Chem Chem Phys. 2013 May 28;15(20):7657-65. doi: 10.1039/c3cp44687e. Epub 2013 Apr 17.
Graphitic carbon nitride (g-C3N4) was prepared by pyrolysis of urea at different temperatures (450-650 °C), and characterized by thermogravimetric and differential thermal analysis (TG-DTA), elemental analysis (C/H/N), X-ray diffraction (XRD), UV-vis diffuse reflectance spectra (DRS), Brunauer-Emmett-Teller (BET) analysis, Fourier transform-infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and photoluminescence (PL) spectra. The samples prepared at low temperatures (450 and 500 °C) are a mixture of g-C3N4 and impurities, whereas the samples prepared at high temperatures (550, 600 and 650 °C) should be g-C3N4 (polymeric carbon nitride). The polymerization degree of g-C3N4 for the prepared samples increases to a maximum at 600 °C with increasing pyrolysis temperature and then decreases, whereas the defect concentration changes conversely, that is, g-C3N4 prepared at 600 °C has the lowest defect concentration. Using Eosin Y (EY) and the prepared sample as the sensitizer and the matrix, respectively, the photocatalytic activity for hydrogen evolution from aqueous triethanolamine solution was investigated. The g-C3N4 prepared at 600 °C exhibits the highest sensitization activity. Under optimum conditions (1.25 × 10(-5) mol L(-1) EY and 7.0 wt% Pt), the maximal apparent quantum yield of EY-sensitized g-C3N4 prepared at 600 °C for hydrogen evolution is 18.8%. The highest activity can be attributed to the pure composition, the higher dye adsorption amount and the lowest defect concentration.
石墨相氮化碳(g-C3N4)是通过在不同温度(450-650°C)下热解尿素制备的,并通过热重和差热分析(TG-DTA)、元素分析(C/H/N)、X 射线衍射(XRD)、紫外-可见漫反射光谱(DRS)、BET 分析、傅里叶变换-红外(FT-IR)光谱、X 射线光电子能谱(XPS)和光致发光(PL)光谱进行了表征。在低温(450 和 500°C)下制备的样品是 g-C3N4 和杂质的混合物,而在高温(550、600 和 650°C)下制备的样品应该是 g-C3N4(聚合碳氮化物)。随着热解温度的升高,制备样品的 g-C3N4 的聚合度先增加到最大值,然后降低,而缺陷浓度则相反变化,即 600°C 下制备的 g-C3N4 具有最低的缺陷浓度。使用曙红 Y(EY)和制备的样品分别作为敏化剂和基质,研究了从水三乙醇胺溶液中光催化析氢的活性。在 600°C 下制备的 g-C3N4 表现出最高的敏化活性。在最佳条件下(1.25×10(-5)mol L(-1)EY 和 7.0wt%Pt),600°C 下制备的 EY 敏化 g-C3N4 的最大表观量子产率为 18.8%。最高的活性可以归因于纯组成、更高的染料吸附量和更低的缺陷浓度。