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Preparation of fast pyrolysis carbon for NH.sub.3-SCR at low temperature: a study of experiments and DFT calculations

Journal of materials science, 2022-10, Vol.57 (40), p.18889 [Peer Reviewed Journal]

COPYRIGHT 2022 Springer ;ISSN: 0022-2461 ;EISSN: 1573-4803 ;DOI: 10.1007/s10853-022-07806-4

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  • Title:
    Preparation of fast pyrolysis carbon for NH.sub.3-SCR at low temperature: a study of experiments and DFT calculations
  • Author: Zhang, Juan ; Li, Guobo ; Wu, Peng ; Zhang, Yaping ; Li, Bingyu ; Yang, Hongqiang ; Shen, Kai
  • Subjects: Adsorption ; Chemical properties ; Pyrolysis
  • Is Part Of: Journal of materials science, 2022-10, Vol.57 (40), p.18889
  • Description: A series of residual carbon derived from the rapid pyrolysis of biomass was prepared and applied in the selective catalytic reduction (SCR) of NO with NH.sub.3. Various characterization techniques and Density Function Theory (DFT) calculations were conducted to determine the catalyst structure and reaction mechanism. Mn-loaded residual carbon from corn straw pyrolyzed at 400 °C (MnCorn4PC) exhibited the best NO.sub.x conversion of 87% at 250 °C and maintained conversion of 50% in the temperature range of 100-200 °C. The characterization results revealed that MnCorn4PC catalyst displayed higher specific surface area and more uniform dispersion of active components. It was speculated that better low-temperature redox properties, stronger surface acidity, and richer C = O species contributed to the low-temperature SCR activity of the MnCorn4PC catalyst. DFT calculation results showed that the molecules (NH.sub.3, NO, and O.sub.2) formed a new chemical bond with the Mn site, and the highest adsorption energy of NH.sub.3 was - 236.9 kJ/mol with the bond length of 2.09 Å. The calculation and in situ DRIFTS experiments indicated that the Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms simultaneously occurred on the MnCorn4PC catalyst surface, in which the adsorbed NH.sub.3 on the Brønsted acid and Lewis acid sites reacted with NO and regenerated hydroxide as Brønsted acid for the next cycle promoting the SCR reaction process.
  • Publisher: Springer
  • Language: English
  • Identifier: ISSN: 0022-2461
    EISSN: 1573-4803
    DOI: 10.1007/s10853-022-07806-4
  • Source: AUTh Library subscriptions: ProQuest Central
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