Citation: JIN Rui-Rui, YOU Ji-Guang, ZHANG Qian, LIU Dan, HU Shao-Zheng, GUI Jian-Zhou. Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity[J]. Acta Physico-Chimica Sinica, 2014, 30(9): 1706-1712. doi: 10.3866/PKU.WHXB201406272
Fe掺杂g-C3N4的制备及其可见光催化性能
以硝酸铁和三聚氰胺为原料制备不同含铁量的Fe 掺杂石墨氮化碳(g-C3N4). 采用X 射线衍射光谱(XRD)、紫外-可见(UV-Vis)光谱、傅里叶变换红外(FT-IR)光谱、电感耦合等离子体-原子发射光谱(ICP-AES)、荧光(PL)光谱、X光电子能谱(XPS)等分析手段对制备的催化剂进行了表征. 结果表明,铁以离子形式镶嵌在g-C3N4的结构单元中,影响了g-C3N4的能带结构,增加了g-C3N4对可见光的吸收,降低了光生电子-空穴对的复合几率. 以染料罗丹明B的降解为探针反应系统研究了不同含铁量对g-C3N4在可见光下催化性能的影响. 结果表明,m(Fe)/m(g-C3N4)=0.14%时,制备的Fe 掺杂g-C3N4表现出最佳的光催化性能,120 min 内罗丹明B的降解率高达99.7%,速率常数达到0.026 min-1,是纯g-C3N4的3.2 倍. 以叔丁醇、对苯醌、乙二胺四乙酸二钠为自由基(·OH)、自由基(O2-·)和空穴(hVB+)的捕获剂,研究了光催化反应机理.
English
Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity
A series of Fe-doped graphitic carbon nitride (g-C3N4) photocatalysts were prepared using ferric nitrate and melamine as precursors. X-ray diffraction (XRD), ultraviolet-visible (UV-Vis) spectroscopy, Fouriertransform infrared (FT-IR) spectroscopy, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), photoluminescence (PL) spectrum, and X-ray photoelectron spectroscopy (XPS) were used to identify changes in the characteristics caused by coordination of N atoms in the structural units of g-C3N4. The results indicate that embedded Fe3+ changed the optical properties, affected the energy band structure, and increased the electron/hole separation rate. The activities of the Fe3+-doped g-C3N4 catalysts were tested in the photocatalytic degradation of rhodamine B (RhB) under visible light. The degradation rate of RhB over Fe3+-doped g-C3N4 was 99.7% in 120 min. The rate constant for Fe3+-doped g-C3N4 was 3.2 times as high as that of pure g-C3N4. Disodium ethylenediamine tetraacetate, tert-butyl alcohol, and 1,4-benzoquinone were used as hole (hVB+), hydroxyl radical (·OH), and superoxide radical (O2-·) scavengers, respectively, to investigate the possible mechanism.
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Key words:
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Graphitic carbon nitride
- / Photocatalysis
- / Visible light
- / RhB degrdatiaon
- / Fe doping
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