The Adsorption Behavior and Reaction Mechanism of MnOx/TiO2 Catalytic Materials to NO and NH3 by DRIFTS
HELIAN Yizhe, MA Xiaoyu, CUI Suping, WAN Yeqiang
The Key Laboratory of New Functional Materials of Ministry of Education, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124
Abstract: MnOx/TiO2 catalysts has been shown excellent selective catalyst reduction (SCR) activity at low temperature.In order to understand its mechanism thoroughly and improve its catalytic activity further, in situ diffuse reflectance infrared spectroscopy (DRIFTS) was adopted to systematically analyze the single adsorption and coadsorption of NO and NH3 on MnOx/TiO2 catalytic materials. It is considered that the selective catalytic reduction process of the catalytic material conforms to the Eley-Ridal mechanism,and the reaction occurs between the adsorbed NH3 and the gaseous NO,while the adsorbed NO and the produced azotate and nitrite will occupy the active site of the catalytic material,which affects the adsorption of NH3 and leads to the decrease of the denitrification activity.
赫连一哲, 马晓宇, 崔素萍, 万业强. 原位漫反射红外光谱研究NO和NH3在MnOx/TiO2催化材料上的吸附行为及反应机理[J]. 材料导报, 2018, 32(22): 3973-3978.
HELIAN Yizhe, MA Xiaoyu, CUI Suping, WAN Yeqiang. The Adsorption Behavior and Reaction Mechanism of MnOx/TiO2 Catalytic Materials to NO and NH3 by DRIFTS. Materials Reports, 2018, 32(22): 3973-3978.
1 Xia F,Song Z,Liu X,et al.Improved catalytic activity and N2,selectivity of Fe-MnOx, catalyst for selective catalytic reduction of NO by NH3,at low temperature[J].Research on Chemical Intermediates,2018,44(4):2703. 2 Liu F,Shan W,Lian Z,et al.Novel MnWO catalyst with remarkable performance for low temperature NH3-SCR of NO[J].Catalysis Scie-nce & Technology,2013,3(10):2699. 3 Liu H Y,Zhang Y.Dynamic model of catalytic denitrification of nitrate over Pd-Cu catalysts from groundwater[J]. Advanced Mate-rials Research,2011,322:195. 4 Chen L,Li J,Ge M.DRIFT study on cerium-tungsten/titania catalyst for selective catalytic reduction of NOx with NH3[J].Environmental Science&Technology,2010,44(24):9590. 5 Sun L S, Zhao Q S, Xiang J, et al. Adsorption of NO and NH3 over CuO/γ-Al2O3 catalyst[J]. CIESC Journal,2009,60(2):444(in Chinese). 孙路石,赵清森,向军,等.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[J].化工学报,2009,60(2):444. 6 Li J, Zhang Y P, Wang W X, et al.Surface properties, NH3 adsorption characteristic and NOx removal mechanism of TiO2-SnO2 supported WO3 catalysts[J]. Journal of Southeast University (Natural Science Edition),2016,46(1):92(in Chinese). 李娟,张亚平,王文选,等.TiO2-SnO2基钨催化剂的表面性质和NH3吸附特性及脱硝机理[J].东南大学学报(自然科学版),2016,46(1):92. 7 Wei L,Cui S,Guo H,et al.The effect of alkali metal over Mn/TiO2,for low-temperature SCR of NO with NH3,through DRIFT and DFT[J].Computational Materials Science,2018,144:216. 8 Shen B,Wang Y,Wang F,et al.The effect of Ce-Zr on NH3-SCR activity over MnOx(0.6)/Ce0.5Zr0.5O2, at low temperature[J].Chemical Engineering Journal,2014,236(2):171. 9 Zhao H H,Xie G Y,Liu Z Y,et al.A combined in-situ diffuse reflectance FTIR and on-line mass spectroscopy study of surface acidity and reactivity over a CuO/Al2O3 catalyst[J].Acta Chimica Sinica,2008,66(9):1021(in Chinese). 赵海红,谢国勇,刘振宇,等.应用原位漫反射红外-质谱技术研究CuO/Al2O3催化剂表面酸性及其反应性能[J].化学学报,2008,66(9):1021. 10 Guo W Q,Zhang Y P,Wang W X,et al.Study on the surface properties of TiO2-SnO2 supported catalysts for low temperature selective catalytic reduction of NOx[J].Journal of Fuel Chemistry and Technology,2015,43(11):1393(in Chinese). 郭婉秋,张亚平,王文选,等.基于钛锡载体的SCR低温脱硝催化剂的表面性质研究[J].燃料化学学报,2015,43(11):1393. 11 Fan J,Ning P,Song Z,et al.Mechanistic aspects of NH3-SCR reaction over CeO2/TiO2-ZrO2-(SO4)2-catalyst:In situ DRIFTS investigation[J].Chemical Engineering Journal,2018,334:855. 12 Kantcheva M,Vakkasoglu A S.Cobalt supported on zirconia and sulfated zirconia:Ⅱ.Reactivity of adsorbed NOx,compounds toward methane[J].Journal of Catalysis,2004,223(2):364. 13 Wu J C S,Cheng Y T.In situ FTIR study of photo-catalytic NO reaction on photo-catalysts under UV irradiation[J].Journal of Catalysis,2006,237(2):393. 14 Liu J,Li X,Zhao Q,et al.Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide:In situ,FTIR analysis for structure-activity correlation[J].Applied Catalysis B Environmental,2017,200:297. 15 Liu C,Shi J W,Gao C,et al.Manganese oxide-based catalysts for low-temperature selective catalytic reduction of NOx with NH3:A review[J].Applied Catalysis A General,2016,522:54.