Effects of alkali metals on catalyst of MnOx-CeO2/ZrO2-PILC in the low-temperature selective catalytic reduction
-
摘要: 采用浸渍法模拟低温选择性催化还原(SCR)催化剂MnOx-CeO2/ZrO2-PILC的碱土金属中毒特性,研究了碱土金属及其负载量对中毒程度的影响。实验表明,钙/镁的添加会引起催化剂中毒,催化剂中毒失活程度与碱土金属的负载量有关。运用 X射线衍射(XRD)、H2程序升温还原( H2-TPR)、氮气吸脱附及 NH3程序升温脱附(NH3-TPD)对新鲜催化剂以及碱土金属中毒后的催化剂进行了表征。结果表明,钙/镁中毒后催化剂的比表面积降低、催化剂氧化还原性和表面酸性减少,进而造成催化剂失活。Abstract: The poisoning effects of alkali metals on low-temperature selective catalytic reduction (SCR) catalyst MnOx-CeO2/ZrO2-PILC were invested by the method of impregnation in the laboratory. It was indicated that the addition of Ca/Mg would decrease the activities of the catalyst, and the poisoning effects were contacted with the amount and acidity of the doped-alkali metal. X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR), N2 adsorption-desorption and temperature-programmed desorption of NH3 (NH3-TPD) were used to characterize the properties of the fresh and alkali earth doped catalysts. According to the results, the doped-alkali metals would inhibit the reduction properties, induce the loss in surface area and surface acidity.
-
张先龙, 吴雪平, 黄张根, 刘振宇. 燃煤烟气中碱金属化合物对V2O5/AC催化剂低温脱硝的影响[J]. 燃料化学学报,2009, 37(4): 496-500. (ZHANG Xian-long, WU Xue-ping,HUANG Zhang-gen, LIU Zhen-yu. Effect of potassium compounds on the catalytic activity of V2O5 /AC for SCR of NO by NH3 at low temperatures:NH3 adsorption and oxidation[J]. Journal of Fuel Chemistry and Technology, 2009, 37(4): 496-500.) CHEN L, LI J, GE M. The poisoning effect of alkali metals doping over nano V2O5–WO3/TiO2 catalysts on selective catalytic reduction of NOx by NH3[J]. Chem Eng J, 2011, 170(2/3): 531-537. 郭凤, 余剑, 朱剑虹, 刘云义, 许光文. Mn-Fe-Ce/TiO2低温NH3选择性催化还原NO[J]. 过程工程学报, 2009, 9(6): 1192-1197. (GUO Feng, YU Jian, ZHU Jian-hong, LIU Yun-yi, XU Guang-wen. Low-temperature selective catalytic reduction of NO with NH3 over Mn-Fe-Ce/TiO2[J]. The Chinese Journal of Process Engineering, 2009, 9(6): 1192-1197.) SHEN B, LIU T, ZHAO N, YANG X, DENG L. Iron-doped Mn-Ce/TiO2 catalyst for low temperature selective catalytic reduction of NO with NH3[J]. J Environ Sci, 2010, 22(9): 1447-1454. 熊丽仙, 沈伯雄, 杨晓燕, 邓黎丹, 赵宁. 纳米负载型V2O5-WO3/TiO2催化剂碱及碱土金属中毒[J]. 环境化学, 2010, 29(4): 690-695. (XIONG Li-xian, SHEN Bo-xiong, YANG Xiao-yan, DENG Li-dan, ZHAO Ning. Deactivation of V2O5-WO3/TiO2 nona catalysts by alkali and alkaline earth metals[J]. Environmental Chemistry,2010,29(4):690-695.) TANG F, XU B, SHI H,QIU J, FAN Y. The poisoning effect of Na+ and Ca2+ ions doped on the V2O5/TiO2 catalysts for selective catalytic reduction of NO by NH3[J]. Appl Catal B, 2010, 94(1/2): 71–76. 沈伯雄, 邓黎丹, 马娟, 左琛, 郝晓翠. Mn-CeOx/钛基层柱黏土( Ti-PILCs)低温选择性催化还原催化剂的钙中毒研究[J]. 环境污染与防治, 2011, 33(3): 1-5,10. (SHEN Bo-xiong, DENG Li-dan, MA Juan,ZUO Chen, HAO Xiao-cui. Calcium deact ivation of Mn-CeOx/Ti-PILCs low-temperature SCR catalyst[J]. Environmental Pollution & Control, 2011, 33(3): 1-5.) SHEN B, LIU T, YANG X, ZHAO N. The catalysts of MNOx/CeO2-ZrO2 for low-temperature selective catalytic reduction of NOx with NH3[J]. Environ Eng Sci, 2011, 28(4): 291-298. KUSTOVSTOV A L, KUSTOVA M Y, FEHRMANNA R, SIMONSEN P. Vanadia on sulphated-ZrO2, a promising catalyst for NO abatement with ammonia in alkali containing ue gases[J]. Appl Catal B, 2005, 58(1/2): 97-104. KLIMCZAK M, KERN P, HEINZELMANN T, LUCAS M, CLAUS P. High-throughput study of the effects of inorganic additives and poisons on NH3-SCR catalysts: Part II Fe-zeolite catalysts[J]. Appl Catal B, 2010, 95(1/2): 48-56. LONG R Q, YANG R T. The promoting role of rare earth oxides on Fe-exchanged TiO2-pillared clay for selective catalytic reduction of nitric oxide by ammonia[J]. Appl Catal B,2000, 27(2):87-95. CHMIELARZ L, KUSTROWSKI P, ZBROJA M, ASOCHA W, DZIEMBAJ R. Selective reduction of NO with NH3 over pillared clays modified with transition metals[J]. Catal Today, 2004, 90(1/2): 43-49. EINVALL J,ALBERTAZZI S,HULTEBERG C,MALIK A, BASILE F, LARSSON A, BRANDIN J, SANATI M.Investigation of reforming catalyst deactivation by exposure to fly ash from biomass gasification in laboratory scale[J]. Energy Fuels 2007, 21(5), 2481-2488. 沈伯雄, 熊丽仙, 刘亭, 王静, 田晓娟. 纳米负载型 V2O5-WO3/TiO2催化剂碱中毒及再生研究[J]. 燃料化学学报,2010, 38(4): 85-90. (SHEN Bo-xiong, XIONG Li-xian, LIU Ting, WANG Jing, TIAN Xiao-juan.Alkali deactivation and regeneration of nano V2O5-WO3/TiO2 catalysts[J]. Journal of Fuel Chemistry and Technology, 2010, 38(4): 85-90.) TANG X, LI Y, HUANG X, XU Y, ZHU H, WANG J, SHEN W.MNOx-CeO2 mixed oxide catalysts for complete oxidation of formaldehyde: Effect of preparation method and calcination temperature[J]. Appl Catal B, 2006, 62(3/4): 265-273. CHOI E-Y, NAM I-S, KIM Y G. TPD study of mordenite-type zeolites for selective catalytic reduction of NO by NH3[J]. J Catal, 1996, 161(2): 597-604. LISI L, LASORELLA G, MALLOGGI S, RUSSO G. Single and combined deactivating effect of alkali metals and HCl on commercial SCR catalysts[J]. Appl Catal B, 2004, 50(4): 251-25.
点击查看大图
计量
- 文章访问数: 1812
- HTML全文浏览量: 18
- PDF下载量: 863
- 被引次数: 0