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

doi:10.1016/j.cjche.2023.04.019

Abstract

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

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

Fengrong Li, Xuezhen Liu, ZhengYi Zhao, Xia An, Yali Du, Xu Wu. 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[J]. Chinese Journal of Chemical Engineering, 2023, 63(11): 185-196.

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