钾盐沉积对Mn-Ce/TiO2低温SCR催化剂脱硝性能的影响The poisoning effect of K depositing over Mn-Ce/TiO2 catalyst for low-temperature selective catalytic reduction of NO by NH3
陈新利,周爱奕,盛重义,杨柳,谭月
摘要(Abstract):
采用浸渍法分别制备K_2CO_3、K_2SO_4、KNO_3和KCl四种钾盐前驱体沉积的Mn-Ce/Ti O_2催化剂,通过分析催化剂活性与催化剂理化特性之间的关系,考察碱金属钾沉积对Mn-Ce/Ti O_2低温SCR催化剂脱硝性能的影响。结果显示,钾的加入会导致催化剂中毒,且不同钾前驱体掺杂对催化剂中毒效应不同。KNO_3的沉积对Mn-Ce/Ti O_2催化剂脱硝效率的影响最小,而KCl沉积对催化剂活性抑制作用最为强烈。通过X射线晶体衍射(XRD)和程序升温脱附(TPD)的方法对不同催化剂进行表征发现,催化剂的晶型变化、表面活性元素及酸性点位的减少是催化剂中毒的主要原因。
关键词(KeyWords): 低温选择性催化还原;锰铈钛复合氧化物;碱金属;钾盐沉积;催化剂中毒
基金项目(Foundation): 国家自然科学基金(51508281);; 江苏省自然科学基金(BK20130907)
作者(Author): 陈新利,周爱奕,盛重义,杨柳,谭月
参考文献(References):
- [1]郝吉明,马广大,王书肖.大气污染控制工程[M].北京:高等教育出版社,2010.
- [2]江博琼.Mn/Ti O2系列低温SCR脱硝催化剂制备及其反应机理研究[D].杭州:浙江大学,2008.
- [3]周爱奕,毛华峰,盛重义,等.碱土金属钙沉积对Mn-Ce/Ti O2低温SCR催化剂脱硝性能的影响[J].环境科学,2014(12):4745-4751.
- [4]Kijlstra W S,Biervliet M,Poels E K,et al.Deactivation by SO2of MNOx/Al2O3catalysts used for the selective catalytic reduction of NO with NH3at low temperatures[J].Applied Catalysis B:Environmental,1998,16(4):327-337.
- [5]Pe n~a D A,Uphade B S,Reddy E P,et al.Identification of Surface Species on Titania-Supported Manganese,Chromium,and Copper Oxide Low-Temperature SCR Catalysts[J].Journal of Physical Chemistry B,2004,108(28):9927-9936.
- [6]Moreno-Tost R,Castellón E R,Jiménez-López A.Cobalt-iridium impregnated zirconium-doped mesoporous silica as catalysts for the selective catalytic reduction of NO with ammonia[J].Journal of Molecular Catalysis A:Chemical,2006,248(1-2):126-134.
- [7]Chen J P,Yang R T,Buzanowski M A,et al.Cold selective catalytic reduction of nitric oxide for flue gas applications[J].Industrial&Engineering Chemistry Research,2002,29(7):1431-1435.
- [8]Li J,Chen J,Ke R,et al.Effects of precursors on the surface Mn species and the activities for NO reduction over MNOx/Ti O2catalysts[J].Catalysis Communications,2007,8(12):1896-1900.
- [9]Kim S S,Kang Y S,Lee H D,et al.Release of potassium and sodium species during combustion of various rank coals,biomass,sludge and peats[J].Journal of Industrial&Engineering Chemistry,2012,18(6):2199-2203.
- [10]Chen J P,Buzanowski M A,Yang R T.et al.Deactivation of the Vanadia Catalyst in the Selective Catalytic Reduction Process[J].Journal of the Air&Waste Management Association,1990,40(10):1403-1409.
- [11]Shen Y,Zhu S.Deactivation mechanism of potassium additives on Ti0.8Zr0.2Ce0.2O2.4 for NH3-SCR of NO[J].Catalysis Science&Technology,2012,2(9):1806-1810.
- [12]朱崇兵,金保升,仲兆平,等.碱金属氧化物对V2O5-WO3/Ti O2催化剂脱硝性能的影响[J].环境化学,2007(26):783-786.
- [13]Wu Z B,Jin R B,Liu Y,et al.Ceria modified MNOx/Ti O2as a superior catalyst for NO reduction with NH3at low-temperature[J].Catalysis Communications,2008,9(13):2217-2220.
- [14]Wu Z B,Jing B Q,Liu Y,et al.Experimental study on a lowtemperature SCR catalyst based on Mn O(x)/Ti O2prepared by sol-gel method[J].Journal of Hazardous Materials,2007,145(3):488-494.
- [15]Lonyi F,Valyon J,Engelhardt J,et al.Characterization and catalytic properties of sulfated Zr O2-Ti O2mixed oxides[J].Journal of Catalysis,1996,160(2):179-189.
- [16]Lietti L,Nova I,Ramis G,et al.Characterization and reactivity of V2O5-Mo O3/Ti O2De-NOxSCR catalysts[J].Journal of Catalysis,1999,187(2):419-435.
- [17]邹鹏,熊志波,韩奎华,等.钒钛SCR脱硝低温研究进展[J].电力科技与环保,2011,27(5):5-9.
- [18]肖雨亭,赵建新,汪德志,等.废旧脱硝催化剂再生清洗研究[J].电力科技与环保,201329(4):44-46.