Acta Phys. -Chim. Sin. ›› 2015, Vol. 31 ›› Issue (12): 2366-2374.doi: 10.3866/PKU.WHXB201510141

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Electrochemical Synthesis of Cu3(BTC)2-MOF for Selective Catalytic Reduction of NO with NH3

Zhen-Zhen. LIU,Yong. SHI*(),Chun-Yan. LI,Qi-Dong. ZHAO,Xin-Yong. LI   

  • Received:2015-07-14 Published:2015-12-04
  • Contact: Yong. SHI E-mail:sys-99@163.com
  • Supported by:
    the National Key Basic Research Program of China (973)(2011CB936002);National Natural Science Foundation ofChina(51178076);Fundamental Research Funds for the Central Universities, China(DUT14LK17)

Abstract:

A Cu3(BTC)2 (copper(Ⅱ) benzene 1, 3, 5-tricarboxylate) metal organic framework (MOF) catalyst was successfully prepared through an electrochemical route and used for selective catalytic reduction of nitrogen oxide (NOx) with NH3 for the first time. After systematically optimizing the reaction conditions such as solvents, voltage, electrolyte concentration, and reaction time, pure Cu3(BTC)2 with high crystallinity was obtained in 97.2% yield. The physicochemical properties of the catalyst were determined using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), Raman spectroscopy, in situ Fourier transform infrared (FTIR) spectroscopy, temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS). TGA results indicated that the framework was stable up to 310℃. The catalytic activity of Cu3(BTC)2 was evaluated using NO conversion as a model reaction. The Cu3(BTC)2 activation temperature significantly affected the catalytic activity. The Cu3(BTC)2 sample activated at 240℃ had the best catalytic activity and gave NO conversion of 90% at 220-280℃. A reaction mechanism was proposed based on the in situ FTIR spectroscopy results.

Key words: Electrochemical synthesis, Cu3(BTC)2, Metal-organic framework, NO, NH3-selective catalytic reduction