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Fe2O3/AC催化剂的低温选择性催化还原脱硝性能

  • 尹寿来 朱宝忠 孙运兰 操政 陈光 江汝清 徐天宇 刘锋
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  • 安徽工业大学能源与环境学院,安徽 马鞍山 243002

收稿日期: 2017-06-05

  修回日期: 2017-08-09

  网络出版日期: 2018-04-10

基金资助

焦化能量系统耦合优化、节能设备及排放物协同治理技术

Low-temperature Selective Catalytic Reduction of NOx with Ammonia over Fe2O3/AC Catalysts

  • Shoulai YIN Baozhong ZHU Yunlan SUN Zheng CAO Guang CHEN Ruqing JIANG Tianyu XU Feng LIU
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  • School of Energy and Environment, Anhui University of Technology, Ma?anshan, Anhui 243002, China

Received date: 2017-06-05

  Revised date: 2017-08-09

  Online published: 2018-04-10

摘要

以活性焦(AC)为载体、Fe2O3为活性组分,采用等体积浸渍法制备Fe2O3/AC催化剂,研究了Fe含量对Fe2O3/AC催化剂低温脱硝性能的影响. 结果表明,当Fe负载量为6wt%时能获得比其它负载量更佳的NOx转化率,尤其在240℃时NOx转化率达93.9%,当分别有120?10?6(vol) SO2和3.5vol H2O存在时,脱硝率分别稳定在约86%和74%;催化剂孔径≤4 nm,随Fe负载量增加,孔径呈增大趋势;催化剂较稳定;Fe主要以γ-Fe2O3分散在催化剂表面,负载适量Fe2O3使表面吸附氧Oβ和Fe3+增多,为催化剂提供更多活性位,提高了Fe2O3/AC催化剂的低温选择性催化还原脱硝活性.

关键词: γ-Fe2O3; 活性焦; 低温; SCR

本文引用格式

尹寿来 朱宝忠 孙运兰 操政 陈光 江汝清 徐天宇 刘锋 . Fe2O3/AC催化剂的低温选择性催化还原脱硝性能[J]. 过程工程学报, 2018 , 18(2) : 330 -336 . DOI: 10.12034/j.issn.1009-606X.217251

Abstract

Activated coke (AC) loaded with various amounts Fe was prepared via impregnation method to investigate the effect of iron content on the denitrification performance at low temperature. The results showed that the Fe2O3/AC catalyst with 6wt% Fe addition exhibits the best NOx conversion rate, which reached 93.9% at 240℃, the NOx conversion rate of the catalyst are about 86% and 7% when there are 120?10?6 (vol) SO2 and 3.5vol% H2O, respectively. The pore sizes of these catalysts are less than 4 nm, and increase with the increasing of Fe loading. These catalysts are stable. Fe is mainly existed as γ-Fe2O3 which disperses on the catalyst surface. A certain amount of Fe2O3 on the AC surface increase the contents of Oβ and Fe3+, and provide more active sites, so the selective catalytic reduction (SCR) denitrification performance of the catalyst is improved.

参考文献

[1] 李良华, 刘杰, 曹银平. 焦炉烟气脱硝工艺技术探讨[J]. 燃料与化工, 2015, 46(3): 42-44.
[2] 孙刚森,尹华,吕文彬等. 焦炉烟气脱硫脱硝一体化工艺. 中国会议, 2014年(第八届)焦化节能环保及干熄焦技术研讨会论文集, 2015, 06.
[3] 李金虎, 张先龙, 陈天虎, 等. 凹凸棒石负载锰氧化物低温选择性催化还原催化剂的表征及对氨的吸脱附[J]. 催化学报, 2010, 31(4): 454-460
[4] Khodayari R, Odenbrand C U I. Regeneration of commercial TiO2-V2O5-WO3 SCR catalysts used in bio fuel plants [J]. Appl. Catal. B-Environ., 2001, 30(1-2): 87-99.
[5] Gao X, Du X S, Fu Y C, et al. Theoretical and experimental study on the deactivation of V2O5 based catalyst by lead for selective catalytic reduction of nitric oxides [J]. Catal. Today, 2011, 175(1): 625-630.
[6] Zhao W, Zhong Q, Pan Y, et al. Systematic effects of S-doping on the activity of V2O5/TiO2 catalyst for low-temperature NH3-SCR [J]. Chem. Eng. J., 2013, 228(6): 815-823.
[7] Wang C, Yang S, Chang H, et al. Dispersion of tungsten oxide on SCR performance of V2O5-WO3/TiO2: Acidity, surface species and catalytic activity [J]. Chem. Eng. J., 2013, 225(6): 520-527.
[8] Pasel J,Kβner P,Montanari B,et al. Transition metaloxides supported on active carbons as low temperature catalysts for the selective catalytic reduction (SCR) of NO with NH3 [J]. Appl. Catal. B-Environ.,1998, 18(3-4): 199-213.
[9] Mangun C L, DeBarr J A, Economy J. Adsorption of sulfur dioxide on ammonia-treated activated carbon fibers [J]. Carbon, 2001, 39(11): 1689-1696.
[10] Yu Y M, Guo R L, Li C H. Flue gas desulfurization and denitrification performance of the semi-coke adsorbents [J]. J. Fuel Chem. Technol., 2011, 39(5): 385-389.
[11] Tsuji K, Shiraishi I. Combined desuifurization, denitrification and reduction of air toxics using activated coke: l. Activity of activated coke [J]. Fuel, 1997, 76(6): 549-553.
[12] 王晓波, 归柯庭. 铁基催化剂低温脱硝性能研究[J]. 工程热物理学报, 2013, 34(9): 1671-1674
[13] Liu Z, Wang A, Wang X, et al. Ir-C xerogels synthesized by sol-gel method for NO reduction [J]. Catal. Today, 2008, 137(2):162-166..
[14] Myatt J F. Catalytic Graphitization of Carbon Aerogels by Transition Metals [J]. Langmuir, 2000, 16(9): 4367-4373.
[15] Xiang G, Liu S, Yang Z, et al. Physicochemical properties of metal-doped activated carbons and relationship with their performance in the removal of SO2 and NO [J]. J. Hazard. Mater., 2011, 188(1-3): 58-66.
[16] Wan Y, Zhao W, Yu T, et al. Ni-Mn bi-metal oxide catalysts for the low temperature SCR removal of NO with NH3 [J]. Appl. Catal. B- Environ., 2014, 148-149(6): 114-122.
[17] Sing K S W, Everett D H, Haul R A W, Moscou L, Pierotti R A, Rouquerol J and Siemieniewska T. Reporting PhysisorptionData for Gas/Solid Systems [J]. Pure and Appl. Chem., 1985, 57(4): 603-619.
[18] 王栋, 张信莉, 彭建升,等. 煅烧温度对γ-Fe2O3催化剂结构及其脱硝活性的影响[J]. 环境科学研究, 2015, 28(5): 808-815.
[19] Roosendaal S J, Asselen B V, Elsenaar J W, et al. The oxidation state of Fe(100) after initial oxidation in O2 [J]. Surf. Sci., 1999, 442(3): 329-337.
[20] Zhang R, Li Y, Zhen T. Ammonia selective catalytic reduction of NO over Fe/Cu-SSZ-13 [J]. RSC. Adv. 2014,4(94): 52130-52139
[21] Allen G C, Curtis M T, Hooper A J, Tucker, P. M. X-ray photoelectron spectroscopy of iron-oxygen systems [J]. J. Chem. Soc. Dalton Trans. 1974, 1974(14): 1525-1530.
[22] Devadas M, Kr?cher O, Elsener M, et al. Characterization and catalytic investigation of Fe-ZSM5 for urea-SCR [J]. Catal. Today, 2007, 119(1-4): 137-144.
[23] Delahay G, Valade D, Guzmán-Vargas A, et al. Selective catalytic reduction of nitric oxide with ammonia on Fe-ZSM-5 catalysts prepared by different methods [J]. Appl. Catal. B- Environ., 2005, 55(2): 149-155.
[24] Zhu L, Zhang L, Qu H, et al. A study on chemisorbed oxygen and reaction process of Fe-CuOx/ZSM-5 via ultrasonic impregnation method for low-temperature NH3-SCR [J]. J. Mol. Catal. A-Chem., 2015, 409: 207-215.
[25] Schindler M, Hawthorne F C, Freund M S, Burns P C. XPS spectra of uranyl minerals and synthetic uranyl compounds. II: The O1s spectrum [J]. Geochim. Cosmochim. Ac. 2009, 73(9): 2471-2487.
[26] Wu Z, Jin R, Liu Y, Wang H. Ceria modified MnOx/TiO2 as a superior catalyst for NO reduction with NH3 at low-temperature [J]. Catal. Commun. 2008, 9(13): 2217-2220.
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