Ag/Al_2O_3催化剂上氢气促进正丁烯选择催化还原氮氧化物
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摘要
本文在反应气组成为1000 ppm NO,1000 ppm正丁烯,5000 ppm H2,10% O2,N2作平衡气,气体流量为200 ml/min的条件下,考察了Ag/Al2O3(0-5%)催化剂选择催化还原氮氧化物(NO_x)的性能和H2对正丁烯-SCR反应的影响。结果表明,H2的加入对低温范围内正丁烯还原NO_x的反应起到了明显的促进作用。当GHSV从48000h-1降低到9600h-1时,在200-250℃反应温度范围内NO_x的转化率明显提高,尤其是在1.5%Ag/Al2O3和2%Ag/Al2O3催化剂上。在GHSV= 9600 h"1的条件下,考察了Ag担载量对催化剂活性的影响。结果表明,在所研究的催化剂中2%Ag/Al2O3活性最高,250℃时该催化剂上NO_x的转化率达到了88%。此外,2%Ag/Al2O3催化剂还具有较高的选择性和稳定性。因此,可以认为,对于低温(250℃)下的正丁烯-H2-SCR反应,2%Ag/Al2O3是最佳的催化剂。
对于2%Ag/Al2O3催化剂,本文还研究了250℃下正丁烯和H2的浓度对NO_x转化率的影响。结果发现,在正丁烯浓度为0～1000 ppm, H2浓度为0～5000 ppm的范围内,NO_x的转化率随二者浓度的增大而增大,但当H2的浓度超过5000 ppm后,NO_x转化率的增加趋势显著变缓。
Selective catalytic reduction (SCR) of nitrogen oxides (NOx) by n-C4H8 in the assistance of H2 (n-C4H8-H2-SCR) was investigated over Ag/Al2O3 catalysts (0-5 wt.% Ag). The n-C4H8-H2-SCR was conducted by feeding a gas mixture of 1000 ppm NO,1000 ppm n-C4H8,5000 ppm H2,10% O2 and N2 balance with a total flow rate of 200 ml/min to a fixed bed reactor loading desired amount of catalyst. The effect of H2 on n-C4H8-SCR was studied. The results showed that the addition of H2 significantly promoted NOx reduction by n-C4H8 in the low temperature range. With the decrease of GHSV from 48000 h"1 to 9600 h-1, NOx conversion remarkably increased at the reaction temperature ranged from 200℃to 250℃, especially over the Ag/Al2O3 catalysts containing 1.5-2 wt.% of Ag. At GHSV = 9600 h-1, the activity of Ag/Al2O3 influenced by the loading amount of Ag was studied. It indicated that the 2%Ag/Al2O3 is most active in the investigated catalysts, over which, as high as 88% of NOx in the feeding gas was reduced at 250℃. Furthermore, the 2%Ag/Al2O3 gave high NOx reduction selectivity and displayed substantial catalytic stability at the reaction conditions. In the catalytic durability test at 250℃, no deactivation of the catalyst could be found with time on stream. Therefore, the 2%Ag/Al2O3 catalyst can be considered to be suitable for the n-C4H8-H2-SCR at low temperature (250℃).
For the 2%Ag/Al2O3 catalyst, the dependence of NOx conversion upon the concentration of n-C4H8 and H2 in the feeding gas was also studied at the reaction temperature of 250℃. The results showed that the NOx conversion markedly increased with the increase of n-C4H8 concentration from 0 to 1000 ppm and the increase of H2 concentration from 0 to 5000 ppm. Nevertheless, when the concentration of H2 further increased from 5000 ppm, less enhanced NOx conversion was observed.
对于2%Ag/Al2O3催化剂,本文还研究了250℃下正丁烯和H2的浓度对NO_x转化率的影响。结果发现,在正丁烯浓度为0～1000 ppm, H2浓度为0～5000 ppm的范围内,NO_x的转化率随二者浓度的增大而增大,但当H2的浓度超过5000 ppm后,NO_x转化率的增加趋势显著变缓。
Selective catalytic reduction (SCR) of nitrogen oxides (NOx) by n-C4H8 in the assistance of H2 (n-C4H8-H2-SCR) was investigated over Ag/Al2O3 catalysts (0-5 wt.% Ag). The n-C4H8-H2-SCR was conducted by feeding a gas mixture of 1000 ppm NO,1000 ppm n-C4H8,5000 ppm H2,10% O2 and N2 balance with a total flow rate of 200 ml/min to a fixed bed reactor loading desired amount of catalyst. The effect of H2 on n-C4H8-SCR was studied. The results showed that the addition of H2 significantly promoted NOx reduction by n-C4H8 in the low temperature range. With the decrease of GHSV from 48000 h"1 to 9600 h-1, NOx conversion remarkably increased at the reaction temperature ranged from 200℃to 250℃, especially over the Ag/Al2O3 catalysts containing 1.5-2 wt.% of Ag. At GHSV = 9600 h-1, the activity of Ag/Al2O3 influenced by the loading amount of Ag was studied. It indicated that the 2%Ag/Al2O3 is most active in the investigated catalysts, over which, as high as 88% of NOx in the feeding gas was reduced at 250℃. Furthermore, the 2%Ag/Al2O3 gave high NOx reduction selectivity and displayed substantial catalytic stability at the reaction conditions. In the catalytic durability test at 250℃, no deactivation of the catalyst could be found with time on stream. Therefore, the 2%Ag/Al2O3 catalyst can be considered to be suitable for the n-C4H8-H2-SCR at low temperature (250℃).
For the 2%Ag/Al2O3 catalyst, the dependence of NOx conversion upon the concentration of n-C4H8 and H2 in the feeding gas was also studied at the reaction temperature of 250℃. The results showed that the NOx conversion markedly increased with the increase of n-C4H8 concentration from 0 to 1000 ppm and the increase of H2 concentration from 0 to 5000 ppm. Nevertheless, when the concentration of H2 further increased from 5000 ppm, less enhanced NOx conversion was observed.
引文
[1]张改莲,戚慧心.汽车排气污染物的形成及危害[J].生物学通报,2000,35(6)：17-18
[2]李英实,陈宏德：负载型汽车尾气催化剂简介[J].环境科学进展,1999,7(3)：52-61
[3]于秀敏,杨士春,高莹.降低汽车发动机排放的技术[J].汽车工程,2002,24(1)：445-450.
[4]AUSTU G P. Mechanism of the lean NOx reaction over Cu/ZSM-5 [J].Appl Catal B,1993, 2:81-100
[5]叶青,金钧,陈永宝等.汽车尾气三效催化剂的现状[J].发展和动向,2000,26(1)：112-117.
[6]SATOKAWA S. Enhancing the NO/C3H8/O2 reaction by using H2 over Ag/Al2O3 catalysts under lean-exhaust conditions [J]. Chem Lett,2000,29(3):294-295.
[7]孙锦余.利用氮氧化物控制技术治理大气污染[J].节能,2004,5：41-44.
[8]李智森.燃烧中氮氧化物的形成和防治[J].环境保护,1994,11：6-7.
[9]任剑锋,王增长,牛志卿.大气中氮氧化物的污染与防治[J].科技情报开发与经济,2003,13：92-93.
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[26]WEN B. NO reduction with H2 in the presence of excess O2 over Pd/MFI catalyst [J]. Fuel, 2002,81:1841-1846
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[36]SHIBATA J, TAKADA Y, SHICHI A, ea al. Influence of zeolite support on activity enhancement by addition of hydrogen for SCR of NO by propane over Ag-zeolites [J]. Appl Catal B,2004,54:137-144
[37]SHIMIZU K, HASHIMOTO M, SHIBATA J, et al. Effect of modified-alumina supports on propane-hydrogen-SCR over Ag/alumina [J]. Catal Today,2007,126:266-271
[38]ARVE K, BACKMAN H, KLINGSTEDT F, et al. Hydrogen as a remedy for the detrimental effect of aromatic and cyclic compounds on the HC-SCR over Ag/alumina [J]. Appl Catal B, 2007,70:65-72
[39]HOUEL V, MILLINGTON P, RAJARAM R, et al. Promoting functions of H2 in diesel-SCR over silver catalysts [J]. Appl Catal B,2007,77:29-34
[40]SHIBATA J, TAKADA Y, SHICHI A, et al. Ag cluster as active species for SCR of NO by propane in the presence of hydrogen over Ag-MFI [J]. J Catal,2004,222:368-376
[41]SHIBATA J, SHIMIZU K, TAKADA Y, et al. Structure of active Ag clusters in Ag zeolites for SCR of NO by propane in the presence of hydrogen [J]. J Catal,2004,227:367-374
[42]KONDRATENKO E V, KONDRATENKO V A, RICHTER M, et al. Influence of O2 and H2 on NO reduction by NH3 over Ag/Al2O3:A transient isotopic approach [J]. J Catal,2006,239:23-33
[43]KONDRATENKO V A, BENTRUP U, RICHTER M, et al. Mechanistic aspects of N20 and N2 formation in NO reduction by NH3 over Ag/Al2O3:The effect of O2 and H2 [J]. Appl Catal B, 2008,84:497-504
[44]SHIMIZU K, SATSUMA A. Reaction mechanism of H2-promoted selective catalytic reduction of NO with NH3 over Ag/Al2O3. J Phys Chem C,2007,111:2259-2264
[45]BREEN J P, BURCH R, HARDACRE C, et al. Structural investigation of the promotional effect of hydrogen during the selective catalytic reduction of NOx with hydrocarbons over Ag/Al2O3 catalysts [J]. J Phys Chem B,2005,109:4805-4807
[46]SHIMIZU K, TSUZUKI M, KATO K, et al. Reductive activation of O2 with H2-reduced silver clusters as a key step in the H2-promoted selective catalytic reduction of NO with C3H8 over Ag/Al203 [J]. J Phys Chem C,2007,111:950-959
[47]SHIBATA J, SHIMIZU K, SATOKAWA S, et al. Promotion effect of hydrogen on surface steps in SCR of NO by propane over alumina-based silver catalyst as examined by transient FT-IR [J]. Phus Chem Chem Phys,2003,5:2154-2160
[48]SHIMIZU K, SUGINO K, KATO K, et al. Reaction mechanism of H-promoted selective catalytic reduction of NO with CH over Ag-MFI zeolite [J]. J Phys Chem C,2007,111(17):6481-6487
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[2]李英实,陈宏德：负载型汽车尾气催化剂简介[J].环境科学进展,1999,7(3)：52-61
[3]于秀敏,杨士春,高莹.降低汽车发动机排放的技术[J].汽车工程,2002,24(1)：445-450.
[4]AUSTU G P. Mechanism of the lean NOx reaction over Cu/ZSM-5 [J].Appl Catal B,1993, 2:81-100
[5]叶青,金钧,陈永宝等.汽车尾气三效催化剂的现状[J].发展和动向,2000,26(1)：112-117.
[6]SATOKAWA S. Enhancing the NO/C3H8/O2 reaction by using H2 over Ag/Al2O3 catalysts under lean-exhaust conditions [J]. Chem Lett,2000,29(3):294-295.
[7]孙锦余.利用氮氧化物控制技术治理大气污染[J].节能,2004,5：41-44.
[8]李智森.燃烧中氮氧化物的形成和防治[J].环境保护,1994,11：6-7.
[9]任剑锋,王增长,牛志卿.大气中氮氧化物的污染与防治[J].科技情报开发与经济,2003,13：92-93.
[10]Nakajima F. Air pollution control with catalysis [J]. Catal Today,1991,1:1-20.
[11]IWAMOTO M. Proceedings of the meeting of catalytic technology for removal of nitrogen monoxide [C]. Tokyo:Catalysis Society of Japan,1990,17
[12]HELD W, KONING A, RIHTER T, et al. Catalytic nitrogen oxide (NOx) reduction in net oxidizing exhaust gas [J]. Appl Catal B,1993,2(2):257
[13]LI Y, ARMOR J N. Catalytic reduction of NOx using methane in the presence of oxygen: US, invention. US:5149512[P].1992
[14]JEON J Y, KIMA H Y, WOO S I. Mechanistic study on the SCR of NO by C3H6 over Pt/V/MCM-41 [J]. Appl Catal B,2003,44:301-310
[15]YOKOTA K, FUKUI M, TANAKA K. Catalytic removal of nitric oxide with hydrogen and carbon monoxide in the presence of excess oxygen [J]. Appl Surf Sci,1997,121/122:273-277
[16]UEDA A, NAKAOB T, AZUMAB M, et al. Two conversion maxima at 373 and 573K in the reduction of nitrogen monoxide with hydrogen over Pd/TiO2 catalyst [J]. Catal Today, 1998,45:135-138
[17]BURCH R, COLEMAN M D. An investigation of the NO/H2/O2 reaction on noble-metal catalysts at low temperatures under lean-burn conditions [J]. Appl Catal B,1999,23:115-121
[18]SCHOTT F J P, BALLE P, ADLER J, ea al. Reduction of NO, by H2 on Pt/WO3/ZrO2 catalysts in oxygen-rich exhaust [J]. Appl Catal B,2009,87:18-29
[19]COSTA C N, STATHOPOULOS V N, BELESSI V C, ea al. An investigation of the NO/H2/02(lean-deNOx) reaction on a highly active and selective Pt/La0.5Ce0.5Mn03 catalyst [J]. J Catal,2001,197:350-364
[20]COSTA C N, EFSTATHIOU A M. Low-temperature H2-SCR of NO on a novel Pt/MgO-CeO2 catalyst [J]. Appl Catal B,2007,72:240-252
[21]COSTA C N, SAVVA P G, FIERRO J L G, ea al. Industrial H2-SCR of NO on a novel Pt/MgO-CeO2 catalyst [J]. Appl Catal B,2007,75:147-156
[22]COSTA C N, EFSTATHIOU A M. Mechanistic aspects of the H2-SCR of NO on a novel Pt/MgO-CeO2 catalyst [J]. J Phys Chem,2007,111:3010-3020
[23]MACHIDA M, IKEDA S, KUROGI D, ea al. Low temperature catalytic NOX-H2 reactions over Pt/Ti02-ZrO2 in an excess oxygen [J]. Appl Catal B,2001,35:107-116
[24]QI G S, YANG R T, RINALDI F C. Selective catalytic reduction of nitric oxide with hydrogen over Pd-based catalysts [J]. J Catal,2006,237:381-392
[25]LI L D, ZHANG F X, GUAN N J, ea al. NO selective reduction by hydrogen on potassium titanate supported palladium catalyst [J]. Catal Commu,2008,9:1827-1832
[26]WEN B. NO reduction with H2 in the presence of excess O2 over Pd/MFI catalyst [J]. Fuel, 2002,81:1841-1846
[27]MACHIDA M, WATANABE T. Effect of Na-addition on catalytic activity of Pt-ZSM-5 for low-temperature NO-H2-O2 reactions [J]. Appl Catal B,2004,52:281-286
[28]WU P, LIU Y X, ZHANG F X, ea al. Influences of mesoporous structure on the NO+ H2+ 02 low temperature reaction over Pt/Si-MCM-41 catalyst [J]. Acta Phys-Chem Sin, 2008,24:369-374
[29]武鹏,刘运霞,章福祥等.Pt/SAPO-34在低温H2选择催化还原NO反应中的催化活性[J].催化学报,2008,29：191-196
[30]QI G S, YANG R T, THOMPSON L T. Catalytic reduction of nitric oxide with hydrogen and carbon monoxide in the presence of excess oxygen by Pd supported on pillared clays [J]. Appl Catal A,2004,259:261-267
[31]LAW H Y, KUNG M C, KUNG H H. Low temperature NOx removal from diesel exhaust by coupling ethylene glycol reforming with SCR [J]. Catal Today,2008,136:40-45
[32]SHIMIZU K, SATSUMA A. Hydrogen assisted urea-SCR and NH3-SCR with silver-alumina as highly active and SO2 tolerant de-NO, catalysis [J]. Appl Catal B,2007,77:202-205
[33]张秀丽,贺泓,余运波.氢气对Ag/Al2O3和Cu/Al2O3催化剂选择性催化C3H6还原NOx反应的影响[J].催化学报,2007,28(2)：117-123
[34]SATOKAWA S, SHIBATA J, SHIMIZU K, et al. Promotion effect of H2 on the low temperature activity of the selective reduction of NO by light hydrocarbons over Ag/Al2O3 [J]. Appl Catal B,2003,42:179-186
[35]RICHTER M, FRICKE R, ECKELT R. Unusual activity enhancement of NO conversion over Ag/Al2O3 by using a mixed NH3/H2 reductant under lean conditions [J]. Catal Lett, 2004,94:115-118
[36]SHIBATA J, TAKADA Y, SHICHI A, ea al. Influence of zeolite support on activity enhancement by addition of hydrogen for SCR of NO by propane over Ag-zeolites [J]. Appl Catal B,2004,54:137-144
[37]SHIMIZU K, HASHIMOTO M, SHIBATA J, et al. Effect of modified-alumina supports on propane-hydrogen-SCR over Ag/alumina [J]. Catal Today,2007,126:266-271
[38]ARVE K, BACKMAN H, KLINGSTEDT F, et al. Hydrogen as a remedy for the detrimental effect of aromatic and cyclic compounds on the HC-SCR over Ag/alumina [J]. Appl Catal B, 2007,70:65-72
[39]HOUEL V, MILLINGTON P, RAJARAM R, et al. Promoting functions of H2 in diesel-SCR over silver catalysts [J]. Appl Catal B,2007,77:29-34
[40]SHIBATA J, TAKADA Y, SHICHI A, et al. Ag cluster as active species for SCR of NO by propane in the presence of hydrogen over Ag-MFI [J]. J Catal,2004,222:368-376
[41]SHIBATA J, SHIMIZU K, TAKADA Y, et al. Structure of active Ag clusters in Ag zeolites for SCR of NO by propane in the presence of hydrogen [J]. J Catal,2004,227:367-374
[42]KONDRATENKO E V, KONDRATENKO V A, RICHTER M, et al. Influence of O2 and H2 on NO reduction by NH3 over Ag/Al2O3:A transient isotopic approach [J]. J Catal,2006,239:23-33
[43]KONDRATENKO V A, BENTRUP U, RICHTER M, et al. Mechanistic aspects of N20 and N2 formation in NO reduction by NH3 over Ag/Al2O3:The effect of O2 and H2 [J]. Appl Catal B, 2008,84:497-504
[44]SHIMIZU K, SATSUMA A. Reaction mechanism of H2-promoted selective catalytic reduction of NO with NH3 over Ag/Al2O3. J Phys Chem C,2007,111:2259-2264
[45]BREEN J P, BURCH R, HARDACRE C, et al. Structural investigation of the promotional effect of hydrogen during the selective catalytic reduction of NOx with hydrocarbons over Ag/Al2O3 catalysts [J]. J Phys Chem B,2005,109:4805-4807
[46]SHIMIZU K, TSUZUKI M, KATO K, et al. Reductive activation of O2 with H2-reduced silver clusters as a key step in the H2-promoted selective catalytic reduction of NO with C3H8 over Ag/Al203 [J]. J Phys Chem C,2007,111:950-959
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