化工学报 ›› 2009, Vol. 60 ›› Issue (2): 444-449.

• 能源和环境工程 • 上一篇    下一篇

原位漫反射红外光谱研究NO和NH3在CuO/γ-Al2O3催化剂上的吸附行为

孙路石;赵清森;向军;石金明;王乐乐;胡松;苏胜   

  1. 华中科技大学煤燃烧国家重点实验室
  • 出版日期:2009-02-05 发布日期:2009-02-05


Adsorption of NO and NH3 over CuO/γ-Al2O3 catalyst by DRIFTS

SUN Lushi;ZHAO Qingsen;XIANG Jun;SHI Jinming;WANG Lele;HU Song;SU Sheng   

  • Online:2009-02-05 Published:2009-02-05

摘要:

利用原位漫反射红外光谱法在线研究NH3和NO在CuO/γ-Al2O3催化剂表面吸附和氧化的反应过程。NH3不仅能被吸附在L酸位,也能被吸附在B酸位。NH3氧化脱氢形成NH2物种是反应的中间步骤。NO和NO2以多种形态吸附在催化剂表面。O2存在条件下有利于吸附的NO物种被氧化成高价的NO2。暂态实验中,吸附NH3饱和的催化剂载体通入NO和O2后,共价吸附的NH3首先消失,而NH+4没有参加反应。吸附NO饱和的催化剂载体通入NH3和O2后,吸附态NO特征峰基本没有变化。选择性催化还原反应发生在吸附态NH3和气态NO之间,吸附态的NO及其氧化生成的亚硝基和硝基物种不参与SCR反应。

关键词:

原位漫反射红外光谱, 选择性催化还原, CuO/γ-Al2O3, NH3, NO, 吸附

Abstract:

Granular CuO/γ-Al2O3 catalysts were synthesized by the sol-gel method.The performance of CuO/γ-Al2O3 catalysts for selective catalytic reduction(SCR)was analyzed in a fixed bed adsorption system.The optimum temperature range for SCR reaction on CuO/γ-Al2O3 catalyst was 250—450℃.Based on the previous study,CuO/γ-Al2O3 catalysts were investigated with in-situ diffuse reflectance infrared fourier transform spectroscopy(DRIFTS)for revealing the reaction mechanism.The DRIFTS indicated both coordinated NH3 and NH+4 were present on the catalysts.NO and NO2 could be adsorbed on the catalyst surface and produce a number of different transformation species.Formation of NO-3 after O2 addition suggested the oxidation of adsorbed NO species to nitrates.When NO was introduced into the samples with pre-adsorbed NH3+O2,the coordinated NH3 on the catalyst surface was consumed rapidly.But NH+4 was not consumed under the SCR reaction.It indicated that these coordinated NH3 species could react with NO effectively.When NH3 was introduced into the samples with pre-adsorbed NO+O2,the intensity of adsorbed NO species did not change; it inferred that SCR reaction would not proceed.It was found that the SCR reaction could take place between the adsorbed NH3 and gaseous NO.The adsorbed NO and formed NO-2 and NO-3 species did not participate in the SCR reaction.

Key words:

原位漫反射红外光谱, 选择性催化还原, CuO/γ-Al2O3, NH3, NO, 吸附