Cu改性Fe/Al-PILC催化剂的SCR-C3H6脱硝特性实验研究

Experimental study on the selective catalytic reduction of NO by C3H6 over Cu modified Fe/Al-PILC catalysts

  • 摘要: 为提高Fe/Al-PILC催化剂的SCR脱硝的低温活性,采用Cu对Fe/Al-PILC催化剂进行改性。采用超声浸渍法合成系列xCu-Fe/Al-PILC催化剂,通过XRD、N2吸附-脱附、H2-TPR、UV-vis、XPS、Py-FTIR等系列技术手段进行表征。在固定床微反应器上进行C3H6的选择性催化还原NO的实验。结果表明,经过铜改性后的xCu-Fe/Al-PILC催化剂有效解决了Fe/Al-PILC催化剂低温SCR活性不足的问题,同时提高了中高温活性。催化剂在200-500℃能够实现80%以上脱硝效率,其中,0.13Cu-Fe/Al-PILC在250-500℃实现了90%以上NO转化率,并在250℃达到最高脱硝效率93%。XRD、N2吸附-脱附结果表明,经过铜改性的催化剂可以提供更多反应活性位,提高反应速率。H2-TPR结果表明,掺杂铜使催化剂获得低温还原能力,同时增强了中高温还原能力。UV-vis、XPS结果表明,铜掺杂不仅使铁获得更高氧化态,同时产生了更多低温活性物质孤立Fe3+。Py-FTIR结果表明,催化剂表面同时存在Lewis酸和Brønsted酸,Lewis酸是SCR反应活性中心。

     

    Abstract: In order to improve the low temperature activity of Fe/Al-PILC catalysts for SCR of NO, copper doping was used for the modification. xCu-Fe/Al-PILC catalysts were prepared by ultrasonic impregnation technique and characterized by XRD, N2 adsorption-desorption, H2-TPR, UV-vis, XPS and Py-FTIR. The SCR of NO with C3H6 tests were carried out in a fixed bed reactor. The experimental results showed that the xCu-Fe/Al-PILC catalysts can effectively solve the problem of insufficient SCR activity of Fe/Al-PILC catalysts at low temperature and as well as improve the activity at medium and high temperature. High NO reduction efficiency, 80% and beyond could be achieved at a wide temperature range of 200-500℃ by the catalysts, among which 0.13Cu-Fe/Al-PILC exhibited 90% of the NO conversion at 250-500℃ and maximum NO reduction efficiency of 93% at 250℃. XRD and N2 adsorption-desorption results proved that the catalysts modified by copper provided more active sites and increased the reaction rate. The results of H2-TPR indicated that the doping of copper improved the catalyst's redox ability at lower temperature, while enhanced the catalyst's redox ability at medium and high temperature. UV-vis and XPS study showed that the doping of copper not only increased the higher oxidation state of iron but also produced more isolated Fe3+ which is the low-temperature active species. Py-FTIR test illustrated that Lewis acid and Brönsted acid existed simultaneously on the catalyst surface, and Lewis acid sites were the activity center of the SCR reaction.

     

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