化学学报 ›› 2011, Vol. 69 ›› Issue (20): 2379-2384. 上一篇    下一篇

研究论文

4-二苯胺基苯甲醇功能化石墨烯的制备、电子传递及光催化性能

董玉培,牟志刚,杜玉扣,杨平*   

  1. (苏州大学材料与化学化工学部 苏州 215123)
  • 投稿日期:2011-03-19 修回日期:2011-05-28 发布日期:2011-06-23
  • 通讯作者: 杨平 E-mail:pyang@suda.edu.cn
  • 基金资助:

    共轭树枝分子与纳米金属簇之间能量迁移效应和催化作用

Preparation, Electron Transfer and Photocatalysis of 4-(N,N-Diphenylamine) Benzyl Alcohol Functionalized Graphene

DONG Yu-Pei, MOU Zhi-Gang, DU Yu-Kou, YANG Ping   

  1. (College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123)
  • Received:2011-03-19 Revised:2011-05-28 Published:2011-06-23
  • Contact: Ping Yang E-mail:pyang@suda.edu.cn

在碱性条件下由氧化石墨(GO)还原获得还原石墨烯(RGO). RGO与4-二苯胺基苯甲醇(TPACH2OH)混合后发生相互作用, 得到功能化石墨烯复合物(TPACH2OH-RGO). 采用密度泛函理论(DFT)对TPACH2OH-RGO模拟计算结果表明, TPACH2OH和RGO之间主要通过氢键作用形成复合物. 利用紫外-可见光谱(UV-vis)、拉曼光谱(Raman)、荧光光谱(Fluorescence)、原子力显微镜(AFM)、透射电子显微镜(TEM)和电化学等方法研究了TPACH2OH-RGO结构和光电性质, 并研究了以TPACH2OH-RGO为催化剂在光照射下光催化分解水制氢性能. 实验结果表明: 光照下复合物中激发态TPACH2OH向RGO转移电子. 在TPACH2OH和RGO的质量比为4/3, 体系pH=6条件下, 光照6 h, TPACH2OH-RGO的产氢总量达到35.0 μmol, 比RGO的产氢总量(20.4 mmol)有明显的提高.

关键词: 石墨烯, 4-二苯胺基苯甲醇, 电子转移, 光催化, 氢气

The reduced graphene oxide (RGO) was prepared by the reduction of graphite oxide (GO) under alkaline conditions. 4-(N,N-Diphenylamine) benzyl alcohol functionalized graphene (TPACH2OH-RGO) were formed by stirring the mixture of TPACH2OH and RGO at room temperature. Density functional method (DFT) studies show that hydrogen bond is present between TPACH2OH and RGO in TPACH2OH-RGO. The structure and photoelectric properties of TPACH2OH-RGO conjugate were investigated by using ultraviolet-visible spectra (UV-vis), Raman spectra (Raman), fluorescence spectra (Fl), atomic force microscopy (AFM), transmission electron microscopy (TEM) and electrochemical method. The TPACH2OH-RGO conjugate was employed as a photocatalyst for H2 generation from water under ultraviolet-visible light illumination. The experiment results indicated that electron transfer occurred from the excited-state of TPACH2OH to RGO. When the mass ratio of TPACH2OH to RGO is 4/3, the total amount of H2 evolved from the TPACH2OH-RGO system at pH 6 after 6 h irradiation was 35.0 mmol, which is higher than that produced from the RGO (20.4 mmol).

Key words: graphene, 4-(N,N-diphenylamine) benzyl alcohol, electron transfer, photocatalysis, hydrogen