PREPARATION AND PROPERTIES OF V-Mo/TiO2 CORDIERITE SUPPORTED DENITRATION CATALYST
-
摘要: 随着环境问题日益突出,锅炉烟气中氮氧化物(NOx)的脱除成为亟待解决的问题。采用同步浸渍法制备了堇青石蜂窝负载型脱硝催化剂,研究了钒含量、温度、气时空速以及酸处理等对堇青石负载型脱硝催化剂脱硝效率的影响,同时采用BET、XRD等对催化剂进行物理化学表征。结果表明:负载型脱硝催化剂脱硝效率随着V2O5含量的增加逐渐变大,脱硝效率随着温度提高先增加后降低;在340℃时,负载型催化剂达到较好的脱硝效果,脱硝效率达到98%以上(气时空速为18000 h-1);硫酸处理后的催化剂脱硝效率提高1~3百分点,而HCl处理后的催化剂脱硝效率降低4~8百分点;堇青石负载型催化剂负载率维持在25%左右,经过超声处理后的脱落率<10%。Abstract: With the increasing environmental problems, the removal of nitrogen oxides (NOx) in flue gas has become an urgent problem. In this paper, the cordierite honeycomb-supported denitration catalyst was prepared by simultaneous impregnation method. The effects of vanadium content, temperature, gas hourly space velocity and acid treatment on the denitration efficiency of cordierite-supported denitration catalyst were studied. At the same time, the catalyst was subjected to physical and chemical characterization by means including BET and XRD. The results showed that the supported denitration catalyst could achieve good denitration effect, the denitration efficiency gradually increased with the increase of V2O5 content, as the temperature rose, the efficiency increased first and then decreased; at 340℃, the supported catalyst achieved the best denitration effect, the denitration efficiency was above 98% (the gas hourly space velocity was 18000 h-1); the de-NOx efficiency of sulfuric acid treated catalyst increased by 1~3 percents, while that of hydrochloric acid treated catalyst decreased by 4~8 percents; the loading rate of the supported catalyst was maintained at about 25%, and the shedding rate after ultrasonic treatment was less than 10%.
-
Key words:
- catalyst /
- cordierite /
- support /
- SCR /
- de-NOx
-
FORZATTI P. Present status and perspectives in de-NOx SCR catalysis[J]. Applied Catalysis A:General, 2001, 222(1/2):221-236. 中华人民共和国环保部. 火电厂大气污染物排放标准:GB 13223-2011[S]. 北京:中国标准出版社, 2011. SHANG X S, HU G R, HE C, et al. Regeneration of full-scale commercial honeycomb monolith catalyst (V2O5-WO3/TiO2) used in coal-fired power plant[J]. Journal of Industrial and Engineering Chemistry, 2012, 18(1):513-519. KHODAYARI R, ODENBRAND C U I. Regeneration of commercial TiO2-V2O5-WO3 SCR catalysts used in bio fuel plants[J]. Applied Catalysis B:Environmental, 2001, 30(1):87-99. QIU Y, LIU B, DU J, et al. The monolithic cordierite supported V2O5-MoO3/TiO2 catalyst for NH3-SCR[J]. Chemical Engineering Journal, 2016, 294:264-272. HOU Y Q, LI Y L, LI Q Y, et al. Insight into the role of TiO2 modified activated carbon fibers for the enhanced performance in low-temperature NH3-SCR[J]. Fuel, 2019, 245:554-562. ZHU B Z, LI G B, SUN Y L, et al. De-NOx performance and mechanism of mn-based low-temperature scr catalysts supported on foamed metal nickel[J]. Journal of the Brazilian Chemical Society, 2018, 29(8):1680-1689. 张华, 胡娟, 周万城,等. 堇青石质蜂窝陶瓷的制备[J]. 硅酸盐学报, 2004, 32(1):24-28. GONZÁLEZ-VELASCO J, GUTIERREZ ORTIZ M, FERRET R, et al. Synthesis of cordierite monolithic honeycomb by solid state reaction of precursor oxides[J]. Journal of Materials Science, 1999, 34:1999-2002. 田柳青, 叶代启. 以堇青石蜂窝陶瓷为载体的新型钒氧化物脱氮催化剂研究[J]. 环境科学, 2004, 25(1):7-13. LIU B, DU J, LV X W, et al. Washcoating of cordierite honeycomb with vanadia-tungsta-titania mixed oxides for selective catalytic reduction of NO with NH3[J]. Catalysis Science & Technology, 2015, 5(2):1241-1250. TIAN X, XIAO Y, ZHOU P, et al. Investigation on performance of V2O5-WO3-TiO2-cordierite catalyst modified with Cu, Mn and Ce for urea-SCR of NO[J]. Materials Research Innovations, 2014, 18(sup2):S2-202-S2-206. 蔺卓玮, 陆强, 唐昊,等. 平板式V2O5-MoO3/TiO2型SCR催化剂的中低温脱硝和抗中毒性能研究[J]. 燃料化学学报, 2017, 45(1):113-122. 孔明. NaCl与Hg0对V2O5-WO3/TiO2-SCR脱硝催化剂的协同作用研究[J]. 燃烧化学学报, 2015, 43(12):1504-1509. CIMINO S, TOTARELLA G, TORTORELLI M, et al. Combined poisoning effect of K+ and its counter-ion (Cl- or NO3-) on MnOx/TiO2 catalyst during the low temperature NH3-SCR of NO[J]. Chemical Engineering Journal, 2017, 330:92-101. 陈玲霞, 金保升, 李锋, 等. 添加硫酸根对燃煤电厂V2O5基脱硝催化剂性能的影响[J]. 环境科学学报, 2008, 28(2):294-298. 张秋林, 张金辉, 宁平, 等. SO42-改性对Ce、Ti基催化剂NH3-SCR脱硝性能的影响[J]. 昆明理工大学学报, 2014, 39(6):110-115. ABE H, TSUZUKI H, FUKUNAGA A, et al. Preparation of microporous material from cordierite by acid treatment[J]. Key Engineering Materials-KEY ENG MAT, 1996, 115:159-166. SOYER S, UZUN A, SENKAN S, et al. A quantum chemical study of nitric oxide reduction by ammonia (SCR reaction) on V2O5 catalyst surface[J]. Catalysis Today, 2006, 118(3/4):268-278. BLIZNAKOV G, PESHEVA Y, KLISSURSKI D, et al. Methanol oxidation on V2O5-MoO3-TeO3 catalysts[J]. Applied Catalysis, 1987, 29(2):211-218. COLTON R J, GUZMAN A M, RABALAIS J W. Electrochromism in some thin-film transition-metal oxides characterized by x-ray electron spectroscopy[J]. Journal of Applied Physics, 1978, 49(1):409-416. CHOI S H, CHO S P, LEE J Y, et al. The influence of non-stoichiometric species of V/TiO2 catalysts on selective catalytic reduction at low temperature[J]. Journal of Molecular Catalysis A:Chemical, 2009, 304(1/2):166-173. WIATOWSKA-MROWIECKA J, DE DIESBACH S, MAURICE V, et al. Li-ion intercalation in thermal oxide thin films of MoO3 as Studied by XPS, RBS, and NRA[J]. The Journal of Physical Chemistry C, 2008, 112(29):11050-11058. ANWAR M, HOGARTH C A, BULPETT R. An XPS study of amorphous MoO3/SiO films deposited by co-evaporation[J]. Journal of Materials Science, 1990, 25(3):1784-1788. ANWAR M, HOGARTH C A, BULPETT R. Effect of substrate temperature and film thickness on the surface structure of some thin amorphous films of MoO3 studied by X-ray photoelectron spectroscopy (ESCA)[J]. Journal of Materials Science, 1989, 24(9):3087-3090. BONDARENKA V, SEREIKA R. XPS study of sol-gel synthesized vanadium-titanium-hydroquinone oxide bronze films[J]. International Letters of Chemistry, Physics and Astronomy, 2015, 54:201-207. SUTTHIUMPORN K, KAWI S. Promotional effect of alkaline earth over Ni-La2O3 catalyst for CO2 reforming of CH4:role of surface oxygen species on H2 production and carbon suppression[J]. International Journal of Hydrogen Energy, 2011, 36(22):14435-14446. FANG J, BI X Z, SI D J, et al. Spectroscopic studies of interfacial structures of CeO2-TiO2 mixed oxides[J]. Applied Surface Science, 2007, 253(22):8952-8961. 郭凤, 余剑, 初茉. 溶胶-凝胶原位合成宽活性温度V2O5/TiO2脱硝催化剂[J]. 化工学报,2014, 65(6):2098-2105. LIU F D, HE H. Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NOx with NH3[J]. The Journal of Physical Chemistry C, 2010, 114(40):16929-16936. REICHE M, MACIEJEWSKI M, BAIKER A. Characterization by temperature programmed reduction[J]. Catalysis Today, 2000, 56:347-355.
点击查看大图
计量
- 文章访问数: 243
- HTML全文浏览量: 22
- PDF下载量: 5
- 被引次数: 0