Acta Phys. -Chim. Sin. ›› 2017, Vol. 33 ›› Issue (9): 1855-1864.doi: 10.3866/PKU.WHXB201704282

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Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

Zhi-Dan FU,Jia-Xin ZANG,Qing YE*(),Shui-Yuan CHENG,Tian-Fang KANG   

  • Received:2017-03-17 Published:2017-07-05
  • Contact: Qing YE E-mail:yeqing@bjut.edu.cn
  • Supported by:
    The project was supported by the National Natural Science Foundation of China(21277008);The project was supported by the National Natural Science Foundation of China(20777005);Natural Science Foundation of Beijing, China(8082008);Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(IDHT20140504)

Abstract:

Octahedral layered birnessite (denoted as OL) was synthesized by the oxidation-reduction method and a series of Cux/OL catalysts were prepared by the ion exchange method with various Cu loadings. The materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N2 adsorption-desorption, hydrogen temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric (TG) and.oxygen temperature-programmed desorption (O2-TPD) techniques, and their catalytic activities for CO and ethyl acetate oxidation were evaluated. The results show that OL is a typical octahedral layered structure, and the doping of Cu hardly affects the structure of OL. Moreover, Cux/OL samples had different reducibility, oxygen mobility, and atomic ratio of Cu2+/CuO, (Mn2++Mn3+)/Mn4+, and Oads/Olatt after the addition of Cu to OL. Among the Cux/OL samples, the Cu5/OL sample showed the best activity for the catalytic oxidation of CO and ethyl acetate (T50=70 and T90=100℃ for CO oxidation; T50=160℃ and T90=200℃ for ethyl acetate oxidation). Cu5/OL showed the best reducibility, most isolated Cu2+ species, highest surface (Mn2++Mn3+)/Mn4+ atomic ratio, highest chemisorbed oxygen species, and lowest O2 desorption temperature. Hence, factors such as the strong interaction between copper and manganese, good reducibility, and oxygen mobility were responsible for the excellent catalytic activity of Cu5/OL.

Key words: Octahedral layered birnessite, Cux/OL, Carbon monoxide, Ethyl acetate, Catalytic oxidation