<p>Manganese-cobalt oxide catalyst (Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>-H) with honeycomb structure was prepared from MnCo-BTC (BTC = 1,3,5-benzenetricarboxylic acid). Its honeycomb structure was inherited from MnCo-BTC with nanoneedle structure and Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>-H had a bigger surface area (57.63 m<sup>2</sup>/g) than that (10.06 m<sup>2</sup>/g) of Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>-C prepared by coprecipitation. The Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>-H and Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalysts were tested for low-temperature selective catalytic reduction of NO<sub>x</sub> with NH<sub>3</sub> (NH<sub>3</sub>-SCR) and compared with Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalyst. As a result, Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–H derived from MnCo-BTC exhibited the superior <i>de</i>NO<sub>x</sub> activity, which showed 99% NOx conversion at the existence of 100&#xa0;ppm SO<sub>2</sub> and 200&#xa0;°C. To characterize the Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–H and Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalysts, X-ray diffraction (XRD), scanning electron microscopy (SEM) and temperature-programmed desorption experiments of SO<sub>2</sub> (SO<sub>2</sub>-TPD) were employed. The SO<sub>2</sub>-TPD results showed that Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–H had the weaker SO<sub>2</sub> adsorption than Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalyst, resulting in high SO<sub>2</sub> resistance. Finally, based on the in situ DRIFT experiments, it was demonstrated that SO<sub>2</sub> adsorption on Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–H catalyst was suppressed and the effect of SO<sub>2</sub> on the adsorption of the reactant gases was lower than Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalyst, thus resulting good SO<sub>2</sub> resistance. This work expanded the possible applications of metal organic framework i– the SCR field.</p> Graphical abstract <p>It was demonstrated that SO<sub>2</sub> adsorption on Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–H catalyst (a) was suppressed and the effect of SO<sub>2</sub> on the adsorption of the reactant gases was lower than Mn<sub>x</sub>Co<sub>3-x</sub>O<sub>4</sub>–C catalyst, thus resulting good SO<sub>2</sub> resistance.</p> <p></p>

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Metal organic framework-derived manganese-cobalt oxide with high SO2 resistance for low-temperature NH3-SCR

  • Jin-Hyok Jang,
  • Song-Jin Ko,
  • Jun Yun,
  • Tae-Ui Sim

摘要

Manganese-cobalt oxide catalyst (MnxCo3-xO4-H) with honeycomb structure was prepared from MnCo-BTC (BTC = 1,3,5-benzenetricarboxylic acid). Its honeycomb structure was inherited from MnCo-BTC with nanoneedle structure and MnxCo3-xO4-H had a bigger surface area (57.63 m2/g) than that (10.06 m2/g) of MnxCo3-xO4-C prepared by coprecipitation. The MnxCo3-xO4-H and MnxCo3-xO4–C catalysts were tested for low-temperature selective catalytic reduction of NOx with NH3 (NH3-SCR) and compared with MnxCo3-xO4–C catalyst. As a result, MnxCo3-xO4–H derived from MnCo-BTC exhibited the superior deNOx activity, which showed 99% NOx conversion at the existence of 100 ppm SO2 and 200 °C. To characterize the MnxCo3-xO4–H and MnxCo3-xO4–C catalysts, X-ray diffraction (XRD), scanning electron microscopy (SEM) and temperature-programmed desorption experiments of SO2 (SO2-TPD) were employed. The SO2-TPD results showed that MnxCo3-xO4–H had the weaker SO2 adsorption than MnxCo3-xO4–C catalyst, resulting in high SO2 resistance. Finally, based on the in situ DRIFT experiments, it was demonstrated that SO2 adsorption on MnxCo3-xO4–H catalyst was suppressed and the effect of SO2 on the adsorption of the reactant gases was lower than MnxCo3-xO4–C catalyst, thus resulting good SO2 resistance. This work expanded the possible applications of metal organic framework i– the SCR field.

Graphical abstract

It was demonstrated that SO2 adsorption on MnxCo3-xO4–H catalyst (a) was suppressed and the effect of SO2 on the adsorption of the reactant gases was lower than MnxCo3-xO4–C catalyst, thus resulting good SO2 resistance.