SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2023, Vol. 63 ›› Issue (11): 185-196.DOI: 10.1016/j.cjche.2023.04.019

• Full Length Article • 上一篇    下一篇

Fabrication of highly dispersed carbon doped Cu-based oxides as superior selective catalytic oxidation of ammonia catalysts via employing citric acid-modified carbon nanotubes doping CuAl-LDHs

Fengrong Li1, Xuezhen Liu2, ZhengYi Zhao1, Xia An1, Yali Du3, Xu Wu1   

  1. 1. College of Chemistry, Taiyuan University of Technology, Taiyuan 030024, China;
    2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
    3. College of Chemistry and Chemical Engineering, Jinzhong University, Jinzhong 030619, China
  • 收稿日期:2022-12-25 修回日期:2023-04-19 出版日期:2023-11-28 发布日期:2024-01-08
  • 通讯作者: Xu Wu,E-mail:wuxu@tyut.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (51978436, 52000092, 22272116), Fundamental Research Program of Shanxi Province (202103021224043).

Fabrication of highly dispersed carbon doped Cu-based oxides as superior selective catalytic oxidation of ammonia catalysts via employing citric acid-modified carbon nanotubes doping CuAl-LDHs

Fengrong Li1, Xuezhen Liu2, ZhengYi Zhao1, Xia An1, Yali Du3, Xu Wu1   

  1. 1. College of Chemistry, Taiyuan University of Technology, Taiyuan 030024, China;
    2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
    3. College of Chemistry and Chemical Engineering, Jinzhong University, Jinzhong 030619, China
  • Received:2022-12-25 Revised:2023-04-19 Online:2023-11-28 Published:2024-01-08
  • Contact: Xu Wu,E-mail:wuxu@tyut.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (51978436, 52000092, 22272116), Fundamental Research Program of Shanxi Province (202103021224043).

摘要: In this work, the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides (LDHs) and citric acid-modified carbon nanotubes (c-CNTs) followed by annealing treatment, and evaluated in the selective catalytic oxidation (SCO) of NH3 to N2. The CuAl-LDO/c-CNTs catalyst presented better catalytic performance (98% NH3 conversion with nearly 90% N2 selectivity at 513 K) than other catalysts, such as CuAlO/CNTs, CuAlO/c-CNTs and CuAl-LDO/CNTs. Multiple characterizations were utilized to analyze the difference of physicochemical properties among four catalysts. XRD, TEM and XPS analyses manifested that CuO and Cu2O nanoparticles dispersed well on the surface of the CuAl-LDO/c-CNTs catalyst. Compared with other catalysts, larger specific surface area and better dispersion of CuAl-LDO/c-CNTs catalyst were conducive to the exposure of more active sites, thus improving the redox capacity of the active site and NH3 adsorption capacity. In-situ DRIFTS results revealed that the internal selective catalytic reduction (iSCR) mechanism was found over CuAl-LDO/c-CNTs catalyst.

关键词: Selective catalytic oxidation of ammonia, Layered-double hydroxides, Cu-based oxides, CNTs, Citric acid-modified

Abstract: In this work, the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides (LDHs) and citric acid-modified carbon nanotubes (c-CNTs) followed by annealing treatment, and evaluated in the selective catalytic oxidation (SCO) of NH3 to N2. The CuAl-LDO/c-CNTs catalyst presented better catalytic performance (98% NH3 conversion with nearly 90% N2 selectivity at 513 K) than other catalysts, such as CuAlO/CNTs, CuAlO/c-CNTs and CuAl-LDO/CNTs. Multiple characterizations were utilized to analyze the difference of physicochemical properties among four catalysts. XRD, TEM and XPS analyses manifested that CuO and Cu2O nanoparticles dispersed well on the surface of the CuAl-LDO/c-CNTs catalyst. Compared with other catalysts, larger specific surface area and better dispersion of CuAl-LDO/c-CNTs catalyst were conducive to the exposure of more active sites, thus improving the redox capacity of the active site and NH3 adsorption capacity. In-situ DRIFTS results revealed that the internal selective catalytic reduction (iSCR) mechanism was found over CuAl-LDO/c-CNTs catalyst.

Key words: Selective catalytic oxidation of ammonia, Layered-double hydroxides, Cu-based oxides, CNTs, Citric acid-modified