Han Zhicheng, Yu Qingbo, Xue Zhijia, Liu Kaijie, Qin Qin
School of Metallurgy, Northeastern University P. O. Box345, No. 11, Lane 3, WenHua Road, HePing District Shenyang 110819 Liaoning PR China
College of Energy and Power Engineering, Shenyang Institute of Engineering No. 18, PuChang Road, ShenBei District Shenyang 110136 Liaoning PR China.
RSC Adv. 2018 Dec 18;8(73):42017-42024. doi: 10.1039/c8ra09434a. eCollection 2018 Dec 12.
In this work, Sm-doped manganese supported Zr-Fe polymeric pillared interlayered montmorillonites (Mn/ZrFe-PILMs) were prepared for the low-temperature selective catalytic reduction (SCR) of NO with NH in metallurgical sintering flue gas. These pillared interlayered montmorillonite catalysts were characterized by X-ray diffraction, scanning electron microscopy and energy dispersive spectroscopy, nitrogen adsorption-desorption isotherm, ammonia temperature-programmed desorption, and hydrogen temperature-programmed reduction to study the influence of Sm doping on the SCR performance. The ZrFe-PILMs with a Mn/Sm molar ratio of 18 : 2 showed the excellent SCR activity among these catalysts, where a 95.5% NO conversion ratio at 200 °C at a space velocity of 20 000 h was obtained. Samarium oxide and manganese oxides were highly dispersed on the ZrFe-PILMs with different Mn/Sm molar ratios by the XRD results and SEM-EDS results. Meanwhile, the Mn-Sm/ZrFe-PILM (18 : 2) had the lowest temperature hydrogen reduction peak by H-TPR results, which indicated that it had the lowest active bond energy on its surface. And the NH-TPD results expressed that the Mn-Sm/ZrFe-PILM (18 : 2) had the most acidic sites, especially the weakly acidic sites. Therefore, it was found that the introduction of a small amount of Sm (Mn : Sm = 18 : 2) to Mn/ZrFe-PILM can significantly improve catalytic activity by the increased active oxygen component and the surface acidity.
在本工作中,制备了钐掺杂的锰负载锆铁聚合柱撑蒙脱石(Mn/ZrFe-PILMs),用于冶金烧结烟气中NH对NO的低温选择性催化还原(SCR)。通过X射线衍射、扫描电子显微镜和能谱、氮气吸附-脱附等温线、氨程序升温脱附以及氢程序升温还原对这些柱撑蒙脱石催化剂进行表征,以研究钐掺杂对SCR性能的影响。在这些催化剂中,Mn/Sm摩尔比为18:2的ZrFe-PILMs表现出优异的SCR活性,在200℃、空速为20000 h时获得了95.5%的NO转化率。XRD结果和SEM-EDS结果表明,氧化钐和氧化锰在不同Mn/Sm摩尔比的ZrFe-PILMs上高度分散。同时,H-TPR结果表明,Mn-Sm/ZrFe-PILM(18:2)具有最低温度的氢还原峰,这表明其表面具有最低的活性键能。NH-TPD结果表明,Mn-Sm/ZrFe-PILM(18:2)具有最多的酸性位点,尤其是弱酸性位点。因此,发现向Mn/ZrFe-PILM中引入少量Sm(Mn:Sm = 18:2)可以通过增加活性氧成分和表面酸度显著提高催化活性。