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Mechanistic study of selective catalytic reduction of NO with NH3 over highly dispersed Fe2O3 loaded on Fe-ZSM-5

机译:在Fe-ZSM-5上加入高度分散的Fe2O3的NH3选择性催化还原NO选择性催化还原的机械研究

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ZSM-5 supported highly dispersed Fe _( x ) O _( y ) clusters were prepared by a sol–gel method for selective catalytic reduction (SCR) of NO with NH _(3) . XRD, SEM, UV-vis, H _(2) -temperature-programmed reduction (H _(2) -TPR), NH _(3) -temperature-programmed desorption (NH _(3) -TPD), and BET analyses all indicated that Fe species mainly existed as highly dispersed surface Fe _( x ) O _( y ) clusters with a Fe ~(3+) concentration of 22 wt%. NO-temperature-programmed oxidation (NO-TPO) revealed that the Fe _( x ) O _( y ) clusters promoted the oxidation of NO to NO _(2) , which promoted the low temperature NO _( X ) removal. NH _(3) was activated above 250 °C and over-oxidation of NH _(3) to NO _( X ) was not observed, as a result, a NO _( X ) removal efficiency of 91% was achieved at 400 °C. Moreover, the SCR reaction route was found to be temperature dependent, below 200 °C, the NO _( X ) reduction followed the reaction between NO _(2) and non-activated NH _(3) . Fast SCR reaction dominated the NO _( X ) removal in the temperature window of 200–325 °C. At temperatures above 250 °C, the normal reaction between activated NH _(3) and NO compensated the thermodynamic limitation induced suppression of fast SCR.
机译:ZSM-5支持高度分散的Fe _(X)O _(Y)簇通过溶胶 - 凝胶法制备用于选择性催化还原(SCR)的NH _(3)。 XRD,SEM,UV-VI,H _(2) - 编程减小(H _(2)-TPR),NH _(3) - 编程 - 编程解吸(NH _(3)-TPD)和下注分析表明Fe种主要存在于具有22wt%的Fe〜(3+)浓度的Fe〜(3+)浓度的高度分散的表面Fe _(x)o_(y)簇。无温度编程的氧化(NO-TPO)显示Fe _(x)O _(Y)簇促进NO至NO _(2)的氧化,该氧化物促进低温NO _(X)去除。 NH _(3)以高于250℃,并未观察到NH _(3)至No _(X)的过氧化,结果,在400时实现了91%的NO _(x)去除效率°C。此外,发现SCR反应途径为温度依赖性,低于200℃,否_(x)还原遵循NO _(2)和非活化NH _(3)之间的反应。快速SCR反应在200-325°C的温度窗口中占据了NO _(x)的去除。在高于250℃的温度下,活性NH _(3)之间的正常反应,没有补偿热力学限制诱导的快速舒缓抑制。

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