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<p>Selective catalytic reduction of NO<sub>x</sub> to N<sub>2</sub> by methanol as a reducing agent presents a prospective solution for the removal of NO<sub>x</sub> from the exhaust of methanol engines and the coal-fired power plant, but it confronts the problem of insufficient deNO<sub>x</sub> activity at low temperatures (&lt;350 °C). Here, we discover a strategy for boosting the activity of low-temperature Methanol-SCR by the collaboration of zeolitic acid sites with single iron redox sites. The further pilot-scale bench test using the coated monolithic catalyst also exhibits a remarkable NO<sub>x</sub> conversion and a high stability at low temperature. The location of different Fe sites in FER zeolite is identified by X-ray absorption spectroscopy, Mössbauer spectroscopy, as well as 2D <sup>1</sup>H-<sup>1</sup>H DQ MAS NMR technology. While the dynamic evolution of [FeO]<sup>+</sup> as the critical redox site for NO oxidation is successfully captured by in situ Mössbauer spectroscopy, which unravels the mechanism for the generation of key intermediate HONO on [FeO]<sup>+</sup> sites contributing the low-temperature Methanol-SCR activity. These results indicate the great potential application of Fe-FER zeolite catalyst in industrial Methanol-SCR and provide an atomic-level comprehension of how the dual-active-sites contribute to low-temperature Methanol-SCR activity.</p>

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Single iron redox sites boost Methanol-SCR at low temperature

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月20日

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  • Han Sun,
  • Dekai Liu,
  • Chenyang Li,
  • Chang Wang,
  • Haijun Chen,
  • Zhili Wang,
  • Guangjin Hou,
  • Yun Hu,
  • Masaaki Kitano,
  • Xiaobo Li,
  • Ke Li,
  • Haoran Yang,
  • Mian Wei,
  • Zhaoyu Xiao,
  • Weili Dai

摘要

Selective catalytic reduction of NOx to N2 by methanol as a reducing agent presents a prospective solution for the removal of NOx from the exhaust of methanol engines and the coal-fired power plant, but it confronts the problem of insufficient deNOx activity at low temperatures (<350 °C). Here, we discover a strategy for boosting the activity of low-temperature Methanol-SCR by the collaboration of zeolitic acid sites with single iron redox sites. The further pilot-scale bench test using the coated monolithic catalyst also exhibits a remarkable NOx conversion and a high stability at low temperature. The location of different Fe sites in FER zeolite is identified by X-ray absorption spectroscopy, Mössbauer spectroscopy, as well as 2D 1H-1H DQ MAS NMR technology. While the dynamic evolution of [FeO]+ as the critical redox site for NO oxidation is successfully captured by in situ Mössbauer spectroscopy, which unravels the mechanism for the generation of key intermediate HONO on [FeO]+ sites contributing the low-temperature Methanol-SCR activity. These results indicate the great potential application of Fe-FER zeolite catalyst in industrial Methanol-SCR and provide an atomic-level comprehension of how the dual-active-sites contribute to low-temperature Methanol-SCR activity.