Fe/Mn-Al_2O_3整体式催化剂在烟气NH_3-SCR脱除NO_X中的研究
摘要
活性氧化铝粉体的预处理对于增强其在整体式陶瓷载体上的粘结负载和控制料浆的性能有着重要的作用。本文采用气体粉碎机(GSM)预处理高比表面积的活性氧化铝(γ-Al2O3-b),用其制备的料浆有好的流动性和负载率,其最大的特点是在料浆的制备过程中不需要球磨,为下一步制备整体式选择性催化还原(SCR)催化剂提供了有利条件。
本文采用Fe、Mn为主要催化活性组分制备整体式SCR催化剂,用NH3作还原剂。催化剂的制备方法是Fe、Mn和经预处理的γ-Al2O3-b一起调制成涂覆的料浆,一次涂覆到整体式陶瓷载体上,采用此种方法制备催化剂简单,易操作,并且催化活性较高,在空速5200h-1、NH3/NOX比1.0、反应温度180-320℃范围内,NOx达到完全转化。
通过利用H2-TPR、NH3-TPD和situ DRIFTS研究催化剂表面活性组分的氧化物形态,以及在反应过程中气体在活性中心吸附的状态,从而研究催化反应的过程。Fe的部分取代使得Mn的H2-TPR低温峰向低温方向移动,促进了反应的活性提高,同时Fe也有利于NH3在催化剂表面的吸附并参与反应。NOx的吸附能力比NH3强,当二者达到竞争吸附平衡时反应的活性最高,同时,在Fe1/Mn2-Al2O3的表面反应气体的吸附峰最强,验证了其好的反应活性。
Special pretreatment with Gas Smash Machine (GSM) forγ-Al2O3 is very effective way to enhance adherence to the ceramic and control character of the slurry through change of the particle size distribution.γ-Al2O3-b(showed in table 1) has high surface area and appropriate particle size distribution, which makes the slurry to own excellent adherence and fluidness. Fe and Mn are all prospective transfer metal for the selective catalytic reduction (SCR) of NOx with NH3 and more environmental, meanwhile, they can be added into alumina slurry directly during preparation of ceramic catalyst, which can save amount of work time and procedure. Under the preparation of monolithic catalyst, the conversion of NOx is 100% between 180-320℃, under the molar ratios of NOX/NH3=1.0, and GHSV is 5200 h"1.
With the H2-TPR, NH3-TPD and situ DRIFTS, we have researched the oxide of active elements on the surface of catalysts, and absorption of reaction gas on catalysts. As Fe Substituted by Mn, the reduction peak in low temperature of MnOx has been transferred to lower region according to H2-TPR. Meanwhile, FeOx can improve absorption of NH3 to enhance SCR activity. From the situ DRIFTS, absorption of NOX is stronger than NH3 on the Fe1/Mn2-Al2O3, when the two reaction gas arrive at balance points on catalyst, its peak strength absorption of reaction gas is the highest on all catalysts, which also means it has the best conversion of NOX.
本文采用Fe、Mn为主要催化活性组分制备整体式SCR催化剂,用NH3作还原剂。催化剂的制备方法是Fe、Mn和经预处理的γ-Al2O3-b一起调制成涂覆的料浆,一次涂覆到整体式陶瓷载体上,采用此种方法制备催化剂简单,易操作,并且催化活性较高,在空速5200h-1、NH3/NOX比1.0、反应温度180-320℃范围内,NOx达到完全转化。
通过利用H2-TPR、NH3-TPD和situ DRIFTS研究催化剂表面活性组分的氧化物形态,以及在反应过程中气体在活性中心吸附的状态,从而研究催化反应的过程。Fe的部分取代使得Mn的H2-TPR低温峰向低温方向移动,促进了反应的活性提高,同时Fe也有利于NH3在催化剂表面的吸附并参与反应。NOx的吸附能力比NH3强,当二者达到竞争吸附平衡时反应的活性最高,同时,在Fe1/Mn2-Al2O3的表面反应气体的吸附峰最强,验证了其好的反应活性。
Special pretreatment with Gas Smash Machine (GSM) forγ-Al2O3 is very effective way to enhance adherence to the ceramic and control character of the slurry through change of the particle size distribution.γ-Al2O3-b(showed in table 1) has high surface area and appropriate particle size distribution, which makes the slurry to own excellent adherence and fluidness. Fe and Mn are all prospective transfer metal for the selective catalytic reduction (SCR) of NOx with NH3 and more environmental, meanwhile, they can be added into alumina slurry directly during preparation of ceramic catalyst, which can save amount of work time and procedure. Under the preparation of monolithic catalyst, the conversion of NOx is 100% between 180-320℃, under the molar ratios of NOX/NH3=1.0, and GHSV is 5200 h"1.
With the H2-TPR, NH3-TPD and situ DRIFTS, we have researched the oxide of active elements on the surface of catalysts, and absorption of reaction gas on catalysts. As Fe Substituted by Mn, the reduction peak in low temperature of MnOx has been transferred to lower region according to H2-TPR. Meanwhile, FeOx can improve absorption of NH3 to enhance SCR activity. From the situ DRIFTS, absorption of NOX is stronger than NH3 on the Fe1/Mn2-Al2O3, when the two reaction gas arrive at balance points on catalyst, its peak strength absorption of reaction gas is the highest on all catalysts, which also means it has the best conversion of NOX.
引文
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[3]Qichun Lin, Junhua Li. Selective catalytic reduction of NO with NH3 over Mn-Fe/USY under lean burn conditions. Catalysis Today,2010 (151):251-256
[4]N. Jagtap, S.B. Umbarkar, P. Miquel, P. Granger, M.K. Dongare. Appl. Catal. B 90 (2009)416
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[10]Garin F. Mechanism of NOX decomposition. Appl Catal A:Gen 2001,222:183-219
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[14]Snyder S, Bredt D. Les fonctions biologiques du monoxyde d'azote. Pour La Sci 1992, 177:70-7
[15]Sounak Roy a, M.S. Hegde, Catalysis for NOx abatement, Applied Energy,2009 (86) 2283-2297
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[17]Elmer, T.H. Ultra-low Expansion Ceramic Articles. US Patent 3,958,058,1976
[18]Hong Sun, Yun Shu Deng, Experimental and modeling study of selective catalytic reduction of NOx with NH3 over wire mesh honeycomb catalysts,Chemical Engineering Journal,165(2010)769-775
[19]M. Lyubovsky, H. Karim, P. Menacherry, S. Boorse, R. LaPierre, W.C. Pfefferle, S. Roychoudhury, Complete and partial catalytic oxidation of methane over substrates with enhanced transport properties, Catal. Today 83 (2003) 183-197
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[21]T. Alexander Nijhuis, Annemarie E. W. Beers, PREPARATION OF MONOLITHIC CATALYSTS, CATALYSIS REVIEWS,43(4), (2001)345-380
[22]G.S. Qi, R.T. Yang, Appl. Catal. B 44 (2003) 217
[23]Fudong Liu, Hong He, Yun Ding, Changbin Zhang, Effect of manganese substitution on the structure and activity of iron titanate catalyst for the selective catalytic reduction of NO with NH3, Applied Catalysis B:Environmental 93 (2009) 194-204
[24]刘清雅,刘振宇等,涂敷Al2O3的蜂窝状堇青石负载CuO催化剂上NH3选择性催化还原NO,催化学报,2005,26(1)：59-65
[25]刘晓霞,屈睿,国外SCR催化剂研究进展,广东化工,2007,35(187)：65-69
[26]Masahiro Itoha, Makoto Saitoa etc., Influence of supported-metal characteristics on deNOx catalytic activity over Pt/CeO2, Journal of Molecular Catalysis A:Chemical 304 (2009) 159-165
[27]Teresa Grzybek a, Jerzy Kliniketc., Selective catalytic reduction of nitric oxide with ammonia on Mn-promoted carbonized used silica-alumina sorbents, Catalysis Letters 63 (1999)107-111
[28]Xiaolong Tang, Jiming Hao Deng, Low-temperature SCR of NO with NH3 over AC/C supported manganese-based monolithic catalysts, Catalysis Today 126 (2007) 406-411
[29]Motonobu Kobayashi, Katsunori Miyoshi,WO3-TiO2 monolithic catalysts for high temperature SCR of NO by NH3:Influence of preparation method on structural and physico-chemical properties, activity and durability, Applied Catalysis B:Environmental 72 (2007)253-261
[30]Boxiong Shen, Ting Liu, Iron-doped Mn-Ce/TiO2 catalyst for low temperature selective catalytic reduction of NO with NH3, Journal of Environmental Sciences 2010, 22(9):1447-1454
[31]Park T S, Jeong S K, Hong S H, Hong S C, Selective catalytic reduction of nitrogen oxides with NH3 over natural manganese or at low temperature. Industrial & Engineering Chemistry Research,2001,40(21):4491-4495
[32]Xu W Q, Yu Y B, Zhang C B, He H,2008. Selective catalytic reduction of NO with NH3 over a Ce/TiO2 catalyst. Catalysis Communications,9(6):1453-1457
[33]Qi G S, Yang R T,2003. Low-temperature selective catalytic reduction of NO with NH3 over iron and manganese oxides supported on titania. Applied Catalysis B:Environmental, 44(3):217-225
[34]Tang X L, Hao J M, Yi H H, Li J H, Low-temperature SCR of NO with NH3 over AC/C supported manganese-based monolithic catalysts. Catalysis Today,2007,126(3-4):406-411
[35]Long R Q, Yang R T, Selective catalytic reduction of nitrogen oxides by ammonia over Fe3+-exchanged TiO2-pillared clay catalysts. Journal of Catalysis,1999,186(2):254-268
[36]Liu F D, He H, Zhang C B, Novel iron titanate catalyst for the selective catalytic reduction of NO with NH3 in the medium temperature range. Chemical Communications, 2008, (17):2043-2045
[37]Liu F D, He H, Ding Y, Zhang C B, Effect of manganese substitution on the structure and activity of iron titanate catalyst for the selective catalytic reduction of NO with NH3. Applied Catalysis B:Environmental,2009,93(1-2):194-204
[38]Qi G S, Yang R T, Chang R, MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures. Applied Catalysis B: Environmental,2004,51(2):93-106
[39]Qichun Lin a,b, Junhua Li,Selective catalytic reduction of NO with NH3 over Mn-Fe/USY under lean burn Conditions,Catalysis Today 151 (2010) 251-256
[40]林涛,张秋林等,以ZrO2-TiO2为载体的整体式锰基催化剂应用于低温NH3-SCR反应,物化化学学报,2008,24(7)：1127-1132
[41]Sounak Roy, B. Viswanath etc., Low-Temperature Selective Catalytic Reduction of NO with NH3 over Tio.9Mo.i02-δ(M=Cr, Mn, Fe, Co, Cu),J. Phys. Chem. C 2008,112,6002-6012
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[47]Boqiong Jiang, Yue Liu etc., Low-temperature selective catalytic reduction of NO on MnOx/TiO2 prepared by different methods, Journal of Hazardous Materials 162 (2009) 1249-1254
[48]唐幸福,李俊华等,氧化还原沉淀法制备MnOx-SnO2催化剂及其对NO的NH3选择催化还原性能,催化学报,2008年29卷6期：531-536
[49]吴碧君,朱林等,新型低温NH3选择性还原NOx催化剂研究,热力发电,2008年37卷11期：49-54
[50]吴碧君,刘晓勤等,MnOx/TiO2低温NH3选择性催化还原NOx的研究与表征,燃料科学与技术2008年14卷3期：221-226
[51]Jeong Hoi Goo, Muhammad Faisal Irfan etc., Effects of NO2 and SO2 on selective catalytic reduction of nitrogen oxides by ammonia,Chemosphere 67 (2007) 718-723
[52]Robert Buchel, Reto Strobel etc., Influence of Pt location on BaCO3 or A12O3 during NOx storage reduction,Journal of Catalysis 261 (2009) 201-207
[53]M. Takeuchi, S. Matsumoto, Top. Catal.28 (2004) 151-156
[54]K. Katoh, T. Kihara, T. Asanuma, M. Gotoh, N. Shibaki, Toyota Technol. Rev.44 (1995) 27
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