新型Mn-Fe/ZSM-5催化剂的NH_3-SCR脱硝性能
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摘要
采用氨水沉淀-化学蒸气沉积法制备Mn-Fe/ZSM-5催化剂,并考察其NH_3-SCR脱硝性能。结果表明:Mn-Fe/ZSM-5催化剂具有很好的低温活性和较宽的活性温度范围,在180~450℃的温度范围,NO的脱除率达到98%以上。在该催化剂上活性组分具有很好的分散度、较高的还原能力、较适中的酸性和较好的低温抗硫性,且活性组分Mn和Fe之间存在着协同作用。在SO_2存在的条件下,Mn-Fe/ZSM-5催化剂的活性在240~450℃的温度范围内具有很好的抗硫性,NO的脱除率均高于98%.
Mn-Fe/ZSM-5 catalyst was prepared by ammonia precipitation-chemical vapor deposition method and its performance of the selective catalytic reduction of NO by NH_3(NH_3-SCR)was investigated.Mn-Fe/ZSM-5 catalyst had better low temperature SCR activity and wider activity temperature range.NO conversion on it was up to 98% at 180~450 ℃.Meanwhile,this catalyst had better dispersity,higher ability of redox,more appropriate acidity and better resistance to SO_2.The active components Mn and Fe over Mn-Fe/ZSM-5 catalyst had a synergetic interaction.In presence of SO_2,Mn-Fe/ZSM-5 catalyst exhibited an excellent resisitance to SO_2 with a NO conversion of above 98% at 240~450 ℃.
Mn-Fe/ZSM-5 catalyst was prepared by ammonia precipitation-chemical vapor deposition method and its performance of the selective catalytic reduction of NO by NH_3(NH_3-SCR)was investigated.Mn-Fe/ZSM-5 catalyst had better low temperature SCR activity and wider activity temperature range.NO conversion on it was up to 98% at 180~450 ℃.Meanwhile,this catalyst had better dispersity,higher ability of redox,more appropriate acidity and better resistance to SO_2.The active components Mn and Fe over Mn-Fe/ZSM-5 catalyst had a synergetic interaction.In presence of SO_2,Mn-Fe/ZSM-5 catalyst exhibited an excellent resisitance to SO_2 with a NO conversion of above 98% at 240~450 ℃.
引文
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[19]贺丽芳,刘建东,黄伟,等.制备方法对Mn-Ce-ZSM-5催化剂低温选择性催化还原NO性能的影响[J].高等学校化学学报,2012,33(11):2532-2536.HE L F,LIU J D,HUANG W,et al.Effect of preparation methods on performance of Mn-Ce/ZSM-5catalyst for low-temperature selective catalytic reduction of NO[J].Chemical Journal of Chinese Universities,2012,33(11):2532-2536.
[2]杨超,程华,黄碧纯.抗SO2和H2O中毒的低温NH3-SCR脱硝催化剂研究进展[J].化工进展,2014,33(4):907-913.YANG C,CHENG H,HUANG B C.Review of de-NOxcatalysts with SO2and H2O poisoning resistance for low-temperature NH3-SCR[J].Chemical Engineering Progress,2014,33(4):907-913.
[3]MA A Z,GRUNERT W.Selective catalytic reduction of NO by ammonia over Fe-ZSM-5catalysts[J].Chemical Communications,1999,(1):71-72.
[4]LONG R Q,YANG R T.Catalytic performance of Fe-ZSM-5catalysts for selective catalytic reduction of nitric oxide by ammonia[J].Journal of Catalysis,1999,188(2):332-339.
[5]LONG R Q,YANG R T.Characterization of Fe-ZSM-5catalyst for selective catalytic reduction of nitric oxide by ammonia[J].Journal of Catalysis,2000,194(1):80-90.
[6]WANG X,GUI K.Fe2O3particles as superior catalysts for low temperature selective catalytic reduction of NO with NH3[J].Journal of Environmental Sciences,2013,25(12):2469-2475.
[7]LIU F,HE H,ZHANG C.Novel iron titanate catalyst for the selective catalytic reduction of NO with NH3in the medium temperature range[J].Chemical Communications,2008,164(17):2043-2045.
[8]LIU F,ASAKURA K,HE H,et al.Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NOx with NH3[J].Applied Catalysis B:Environmental,2011,103(3):369-377.
[9]LOU X,LIU P,LI J,et al.Effects of calcination temperature on Mn species and catalytic activities of Mn/ZSM-5catalyst for selective catalytic reduction of NO with ammonia[J].Applied Surface Science,2014,307:382-387.
[10]高蕊蕊,娄晓荣,白文君,等.制备工艺对Mn-Fe/ZSM-5催化剂在NH3选择催化还原NO反应中催化性能的影响[J].分子催化,2015,29(6):563-574.GAO R R,LOU X R,BAI W J,et al.Influence of preparation technology on the activities of Mn-Fe/ZSM-5catalysts for selective catalytic reduction of NO with NH3[J].Journal of Molecular Catalysis,2015,29(6):563-574.
[11]SHI X,HE H,XIE L.The effect of Fe species distribution and acidity of Fe-ZSM-5on the hydrothermal stability and SO2and hydrocarbons durability in NH3-SCR reaction[J].Chinese Journal of Catalysis,2015,36(4):649-656.
[12]LI J,YANG C,ZHANG Q,et al.Effects of Fe addition on the structure and catalytic performance of mesoporous Mn/AlSBA-15catalysts for the reduction of NO with ammonia[J].Catalysis Communications,2015,62:24-28.
[13]KIJLSTRA W S,BRANDS D S,POELS E K,et al.Mechanism of the selective catalytic reduction of NO by NH3 over MNOx/Al2O3[J].Journal of Catalysis,1997,171(1):208-218.
[14]SJOERD K,BRANDS D S,SMIT H I,et al.Mechanism of the selective catalytic reduction of NO with NH3over MNOx/Al2O3:II.Reactivity of adsorbed NH3and NO complexes[J].Journal of Catalysis,1997,171(1):219-230.
[15]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,2017,200:297-308.
[16]刘越,江博琼,吴忠标.以MNOx/TiO2作为催化剂的低温SCR反应过程中还原剂NH3的作用[J].环境科学学报,2008,28(4):671-675.LIU Y,JIANG B Q,WU Z B.The role of NH3in the low-temperaure selective catalytic reduction of NO over MNOx/TiO2[J].Acta Scientiae Circumstantiae,2008,28(4):671-675.
[17]王晓波,伍士国,邹伟欣,等.Fe-Mn/Al2O3催化剂低温NH3选择性催化还原NO的性能[J].催化学报,2016,37(8):1314-1323.WANG X B,WU S G,ZOU W X,et al.Fe-Mn/Al2O3catalysts for low temperature selective catalytic reduction of NO with NH3[J].Chinese Journal of Catalysis,2016,37(8):1314-1323.
[18]黄增斌,李翠清,王振,等.不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能[J].Journal of Fuel Chemistry and Technology,2016,44(11):1388-1393.HUANG Z B,LI C Q,WANG Z,et al.Performance of Mn-Ce catalysts supported on different zeolitesin the NH3-SCR of NOx[J].Journal of Fuel Chemistry and Technology,2016,44(11):1388-1393.
[19]贺丽芳,刘建东,黄伟,等.制备方法对Mn-Ce-ZSM-5催化剂低温选择性催化还原NO性能的影响[J].高等学校化学学报,2012,33(11):2532-2536.HE L F,LIU J D,HUANG W,et al.Effect of preparation methods on performance of Mn-Ce/ZSM-5catalyst for low-temperature selective catalytic reduction of NO[J].Chemical Journal of Chinese Universities,2012,33(11):2532-2536.