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Effect of Fe3+ or Fe2+ species on the catalytic performance and reaction pathway over CWK modified by iron sources in NH3-SCR reaction

  • Ruihua Guo,
  • Zhongxian Song,
  • Xi Chen,
  • Wei Liu,
  • Mengru Zhang,
  • Yehua Fan,
  • Hongrun Gao,
  • Haiyang Li,
  • Xuejun Zhang

摘要

Developing high-performance catalysts for NOx reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F3C and CWK-F3S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N2 selectivity. The key reasons for the enhanced catalytic activity of CWK-F3C and CWK-F3S catalysts could be attributed to the higher Fe3+ concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce3+. More significantly, the adsorption of NH3 and redox capability were both strengthened by the Fe3+ doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F3C and CWK-F2C catalysts. Furthermore, the introduction of Fe3+ generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH2) (NH3(ads) + O(ads)/O2−(ads) → -NH2(ads) + -OH(ads)). The presence of Fe3+ was conducive to NO3 formation (NO3 + NO(ads) → NO2(ads)), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH2 and NO3 species was responsible for the outstanding catalytic activity of CWK-F3C.