Experimental study on NO reduction by propane over iron
-
摘要: 在程序控温电加热水平陶瓷管反应器、N2气氛和模拟烟气气氛以及300~1 100 ℃时,对丙烷在金属铁表面还原NO的特性进行了实验研究,并且与相同条件下甲烷在金属铁表面脱硝的效率进行了对比。结果表明,丙烷在金属铁表面能够高效地还原NO。N2气氛中在500~900 ℃,丙烷在金属铁表面的脱硝效率高于相同含量的甲烷脱硝效率,900 ℃以上丙烷在金属铁表面的脱硝效率超过95%,并且与甲烷的脱硝效率差别很小。模拟烟气条件下,当过量空气系数SR1小于1.0时,温度超过900 ℃后丙烷在金属铁表面还原NO的效率能够达到90%以上,且有、无燃尽的情况下,NO的还原率相差不大。在相同的条件下,丙烷在金属铁表面的脱硝效率高于相同条件下甲烷的脱硝效率。SO2对丙烷在金属铁表面还原NO的效率影响很小,可以忽略。Abstract: NO reduction by propane over iron was experimentally investigated in a one-dimensional temperature-programmed ceramic tubular reactor at 300~1 100 ℃ in N2 and simulated flue gas atmospheres. The NO reduction efficiencies by C3H8 over iron were compared to that by methane. The results show that propane can effectively reduce NO to N2 over metallic iron. In N2 atmosphere, the NO reduction efficiency by propane over metallic iron is higher than that by methane at 500~900 ℃. More than 95% of NO is reduced by propane over metallic iron when the temperature is above 900 ℃, which is very close to that by methane. In simulated flue gas atmosphere, when the excessive air ratio is lower than 1.0, NO reduction by propane over iron exceeds 90% when the temperature is above 900 ℃. There is little difference in NO reduction whether there is a burnout for propane. At same conditions, NO reduction by propane over iron is higher than that by methane. The effect of SO2 on NO reduction by propane over iron is rather small and can be ignored.
-
Key words:
- NO reduction /
- propane /
- iron /
- methane
-
国家环境保护总局. 火电厂大气污染物排放标准(GB13223—2011)[S]. 2011. (Ministry of Environment Protection of China. Emission standard of air pollutants for thermal power plants(GB13223—2011)[S]. 2011.) FORZATTI P, NOVA I, TRONCONI E, KUSTOV A, THOGERSEN J R. Effect of operating variables on the enhanced SCR reaction over a commercial V2O5-WO3/TiO2 catalyst for stationary applications[J]. Catal Today, 2012, 184(1): 153-159. HELD W, KOING A, RICHTER T, PUPPE L. Catalytic NOx reduction in net oxidizing exhaust gas[J]. SAE Trans, 1990, 99(4): 209-216. IWAMOTO M, YAHIRO H, YU U Y. Selective reduction of NO by lower hydrocarbons in the presence of O2 and SO2 over copper ion-exchanged zeolites[J]. Shokubai, 1990, 32(6): 430-433. ERKFELDT S, PALMQVIST A, PETERSSON M. Influence of the reducing agent for lean NOx reduction over Cu-ZSM-5[J]. Appl Catal B: Environ , 2011, 102(3/4): 547-554. LI J H, ZHU R H, CHENG Y S, LAMBERT C K, YANG R T. Mechanism of propene poisoning on Fe-ZSM-5 for selective catalytic reduction of NOx with ammonia[J]. Environ Sci Technol, 2010, 44(5): 1799-1805. YANG T T, BI H T, CHENG X X. Novel fluidized bed reactor for integrated nox adsorption-reduction with hydrocarbons[J]. Environ Sci Technol, 2009, 43(13): 5049-5053. YANG T T, BI H T, CHENG X X. Effects of O2, CO2 and H2O on NOx adsorption and selective catalytic reduction over Fe/ZSM-5[J]. Appl Catal B: Environ, 2011, 102(1/2): 163-171. CAPEK L, DEDECEK J, WICHTERLOVA B. Co-beta zeolite highly active in propane-SCR-NOx in the presence of water vapor: Effect of zeolite preparation and Al distribution in the framework[J]. J Catal, 2004, 227: 352-366. FERREIRA A P, HENRIQUES C, RIBEIRO M F, RIBEIRO F R. SCR of NO with methane over Co-HBEA and PdCo-HBEA catalysts: The promoting effect of steaming over bimetallic catalyst[J]. Catal Today, 2005, 107-108: 181-191. CHEN X M, ZHU A, AU C T, SHI C. Enhanced low-temperature activity of Ag-promoted Co-ZSM-5 for the CH4-SCR of NO[J]. Catal Lett, 2011, 141(1): 207-212. CHEN S, YAN X, WANG Y, CHEN J, PAN D ,MA J, LI R. Effect of SO2 on Co sites for NO-SCR by CH4 over Co-Beta[J]. Catal Today, 2011, 175(1): 12-17. LÓNYI F, SOLT H E, VALYON J, BOIX A, GUTIERREZ L B. The SCR of NO with methane over In, H- and Co, In, H-ZSM-5 catalysts: The promotional effect of cobalt[J]. Appl Catal B: Environ, 2012, 117-118: 212-223. LÓNYI F, SOLT H E, PÁSZTI Z, VALYON J. Mechanism of NO-SCR by methane over Co,H-ZSM-5 and Co, H-mordenite catalysts[J]. Appl Catal B: Environ, 2014, 150-151: 218-229. 荆国华, 李俊华, 杨栋, 郝吉明. 分子筛类催化剂上甲烷选择性催化还原NOx研究进展[J]. 化工进展, 2009, 28(3): 504-510. (JING Guo-hua, LI Jun-hua, YANG Dong, HAO Ji-ming. Progress of selective catalytic reduction of NOx with methane over zeolite-based catalysts[J]. Chemical Industry and Engineering Progress, 2009, 28(3): 504-510.) KIM P S, KIM M K, CHO B K, NAM I-S, OH S H. Effect of H2 on deNOx performance of HC-SCR over Ag/Al2O3: Morphological, chemical, and kinetic changes[J]. J Catal, 2013, 301: 65-76. CHANG F Y, WEY M Y, CHEN J C. Effects of sodium modification, different reductants and SO2 on NO reduction by Rh/Al2O3 catalysts at excess O2 conditions[J]. J Hazard Mater, 2008, 156(1/3): 348-355. NGUYEN L Q, SALIM C, HINODE H. Performance of nano-sized Au/TiO2 for selective catalytic reduction of NOx by propene[J]. Appl Catal A: Gen, 2008, 347(1): 94-99. PÉREZ-RAMÍREZ J, KAPTEIJN F. Effect of NO on the SCR of N2O with propane over Fe-zeolites[J]. Appl Catal B: Environ, 2004, 47: 177-187. JIANG J, PAN H, SUN G, YE Q, SHAO Z, SHI Y. Promotion of Ni/H-BEA by Fe for NOx reduction with propane in a lean-burn condition[J]. Energy Fuels, 2011, 25(10): 4377-4383. 苏亚欣, 苏阿龙, 成豪. 金属铁直接催化还原NO的实验研究[J]. 煤炭学报, 2013, 38(S1): 206-210. (SU Ya-xin, SU A-long, CHENG Hao. Experimental study on direct catalytic reduction of NO by metallic iron[J]. J China Coal Soc, 2013, 38(s1): 206-210.) GRADON B, LASEK J. Investigation of reduction of NO to N2 by reaction with Fe[J]. Fuel, 2010, 89(11): 3505-3509. 苏亚欣, 邓文义, 苏阿龙. 甲烷在氧化铁表面还原NO的特性与反应机理研究[J]. 燃料化学学报, 2013, 41(9): 1129-1135. (SU Ya-xin, DENG Wen-yi, SU A-long. NO reduction by methane over iron oxides and the mechanism[J]. Journal of Fuel Chemistry and Technology, 2013, 41(9): 1129-1135.) 苏亚欣, 任立铭, 苏阿龙, 邓文义. 甲烷在金属铁及氧化铁表面还原NO的实验研究[J]. 燃料化学学报, 2013, 41(11): 1393-1400. (SU Ya-xin, REN Li-ming, SU A-long, DENG Wen-yi. Experimental study on NO reduction by methane over iron and its oxides[J]. Journal of Fuel Chemistry and Technology, 2013, 41(11): 1393-1400.) 苏亚欣, 苏阿龙, 任立铭, 邓文义. SO2对甲烷在金属铁表面还原NO的影响[J]. 燃料化学学报, 2014, 42(3): 377-384. (SU Ya-xin, SU A-long, REN Li-ming, DENG Wen-yi. Effect of SO2 on NO reduction by methane over iron[J]. Journal of Fuel Chemistry and Technology, 2014, 42(3): 377-384.) MUHLER M, SCHÜTZEA J, WESEMANNA M, RAYMENT T, DENT A, SCHLÖGL R, ERTL G.. The nature of the iron oxide-based catalyst for dehydrogenation of ethylbenzene to styrene: I. Solid-state chemistry and bulk characterization[J]. J Catal, 1990, 126: 339-360. SHIMADA H, AKAZAWA T, IKENAGA N, SUZUKI T. Dehydrogenation of isobutane to isobutene with iron-loaded activated carbon catalyst[J]. Appl Catal A: Gen, 1998, 168(2): 243-250. MICHORCZYK P, KUSTROWSKI P, CHMIELARZ L, OGONOWSKI J. Influence of redox properties on the activity of iron oxide catalysts in dehydrogenation of propane with CO2[J]. React Kinet Catal Lett, 2004, 82(1): 121-130. 董文生, 王心葵, 彭少逸. 丙烷脱氢制丙烯研究进展[J]. 合成化学, 1997, 5(3): 246-250. (DONG Wen-sheng, WANG Xin-kui, PENG Shao-yi. New progress in propane dehydrogenation to propene[J]. Chinese Journal of Synthetic Chemistry, 1997, 5(3): 246-250.) BALDI M, ESCRIBANO V S, AMORES J M G, MILELLA F, BUSCA G. Characterization of manganese and iron oxides as combustion catalysts for propane and propene[J]. Appl Catal B: Environ, 1998, 17(3): 175-182. KRYLOV O V, MAMEDOV A K, MIRZABEKOVA S R. The regularities in the interaction of alkanes with CO2 on oxide catalysts[J]. Catal Today, 1995, 24(3): 371-375. JANG H Y, LOBO R F. Catalytic dehydrogenation of propane over iron-silicate zeolites[J]. J Catal, 2014, 312: 263-270. 陈庚. 气基还原氧化铁动力学机理研究[D]. 大连: 大连理工大学, 2011. (CHENG Geng. The kinetics of the gas-based reduction of iron oxide[D]. Dalian: Dalian University of Technology, 2011.) JANAS J, ROJEK W, SHISHIDO T, DZWIGAJ S. Selective catalytic reduction of NO on single site FeSiBEA zeolite catalyst: Influence of the C1 and C2 reducing agents on the catalytic properties[J]. Appl Catal B: Environ, 2012, 123/124: 134-140. DAGAUT P, LUCHE J, CATHONNET M. Reduction of NO by propane in a JSR at 1 atm: Experimental and kinetic modeling[J]. Fuel, 2001, 80(7): 979-986. 苏亚欣, GATHITU B B, CHEN W Y. Fe2O3 控制再燃脱硝中间产物HCN的实验研究[J]. 环境科学学报, 2011, 31(6): 1181-1186. (SU Ya-xin, GATHITU B B, CHEN Wei-yin. Experimental examination of HCN compound control by Fe2O3 during reburning processes[J]. Acta Scientiae Circumstantiae, 2011, 31(6): 1181-1186.)
点击查看大图
计量
- 文章访问数: 485
- HTML全文浏览量: 23
- PDF下载量: 415
- 被引次数: 0