运行中的Cu-CHA除氧催化剂:由Operando XAS和XES监控的温度依赖的NH3辅助选择性催化减排
Kirill A Lomachenko1,2, Elisa Borfecchia1, Chiara Negri1
1Department of Chemistry, NIS Centre and INSTM Reference Center, University of Turin , via P. Giuria 7, 10125 Turin, Italy.
Journal of the American Chemical Society
|August 18, 2016
概括
这项研究揭示了Cu-CHA焦中铜活性位点在氨选择性催化还原 (NH3-SCR) 过程中的两种不同的行为. 移动铜种主导低温,而框架协调铜位则驱动高温NH3-SCR.
科学领域:
- 催化剂
- 材料科学
- 环境化学
背景情况:
- 小孔Cu-CHA焦化物在NH3选择性催化还原 (SCR) 中表现出高性能,用于去除氧化.
- 了解SCR机制和铜活性位点对于优化催化剂设计至关重要.
研究的目的:
- 在NH3-SCR过程中研究Cu-CHA中的Cu活性位点的原子尺度行为.
- 在温度范围内将铜的物种化和流动性与催化活性相关联.
主要方法:
- 使用了X射线吸收光谱 (XANES,EXAFS) 和X射线发射光谱 (XES).
- 在150-400°C的NH3-SCR过程中对Cu-CHA催化剂进行现场监测.
主要成果:
- 根据温度确定了两种不同的Cu活性部位行为.
- 在低温下 (<200°C),移动的NH3化Cu (I) /Cu (II) 物种占主导地位.
- 在高温 (>250°C) 时,框架协调的Cu(II) 位点变得主导,与催化活性增加相关.
结论:
- 该研究阐明了NH3-SCR期间Cu-CHA中的铜活性位点的温度依赖性演变.
- 移动铜种在较低的温度下活跃,而框架协调的Cu (II) 位点对于高温SCR性能至关重要.
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