Effect of chelating agents on selective catalytic reduction activity and mechanism for MnCr₂O₄ spinel catalyst

Abstract

Four different chelating agents, ethylenediamine tetraacetic acid, citric acid, glucose, and sucrose, were selected to synthesize MnCr₂O₄ catalysts (spinel structure) with sol-gel method. Among the prepared catalysts, MnCr₂O₄-S-700, which had the largest specific surface area, showed the best catalytic performance, with a T80 temperature window of 200–260 °C and a denitrification rate of up to 91.6% at 220 °C. Hydrogen temperature programmed reduction, ammonia temperature programmed desorption, and X-ray photoelectron spectroscopy results showed that MnCr₂O₄-S-700 possessed more chemisorbed oxygen O_α as well as active sites (Mn³⁺ + Mn⁴⁺) and (Cr³⁺ + Cr⁵⁺), which improved acidity and redox capacity. There was abundant electron transfer between Mn and Cr elements (Cr⁵⁺ + Mn³⁺ → Cr³⁺ + Mn⁴⁺), enhancing the redox capacity of catalysts. According to the in situ diffuse reflectance infrared transform spectroscopy spectra, it could be concluded that the MnCr₂O₄-S-700 catalyst followed not only the Langmuir-Hinshelwood mechanism but also the Eley-Rideal mechanism. This work displays the effect of the complexation mechanism of chelating agents on the SCR reaction with NH₃ over spinel catalysts.

Graphical abstract

Keywords

chelating agent / NH₃-SCR / MnCr₂O₄ spinel / complexation mechanism

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