物理化学学报 >> 2014, Vol. 30 >> Issue (9): 1706-1712.doi: 10.3866/PKU.WHXB201406272

催化和表面科学 上一篇    下一篇

Fe掺杂g-C3N4的制备及其可见光催化性能

金瑞瑞, 游继光, 张倩, 刘丹, 胡绍争, 桂建舟   

  1. 辽宁石油化工大学化学化工与环境学部, 辽宁抚顺 113001
  • 收稿日期:2014-05-08 修回日期:2014-06-26 发布日期:2014-08-29
  • 通讯作者: 胡绍争, 桂建舟 E-mail:hushaozheng001@163.com;jzgui@hotmail.com
  • 基金资助:

    新世纪优秀人才支持计划(NCET-11-1011),国家自然科学基金(21103077)和辽宁省自然科学基金(201202123)资助项目

Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity

JIN Rui-Rui, YOU Ji-Guang, ZHANG Qian, LIU Dan, HU Shao-Zheng, GUI Jian-Zhou   

  1. Division of Chemistry, Chemical Engineering and Environment, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China
  • Received:2014-05-08 Revised:2014-06-26 Published:2014-08-29
  • Contact: HU Shao-Zheng, GUI Jian-Zhou E-mail:hushaozheng001@163.com;jzgui@hotmail.com
  • Supported by:

    The project was supported by the Program for New Century Excellent Talents in University, China (NCET-11-1011), National Natural Science Foundation of China (21103077), and Natural Science Foundation of Liaoning Province, China (201202123).

摘要:

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.

关键词: 石墨氮化碳, 光催化, 可见光, RhB降解, 铁掺杂

Abstract:

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.

Key words: Graphitic carbon nitride, Photocatalysis, Visible light, RhB degrdatiaon, Fe doping

MSC2000: 

  • O641