γ-Al2O3酸性修饰稀土尾矿NH3-SCR脱硝性能

Abstract
Figure/Table
References
Related Citation (1)

Download: PDF (1485 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract In order to increase the acidic sites and specific surface area of the denitration catalyst, with rare earth tailings as the active main body, γ-Al₂O₃ was added by physical ball milling to prepare NH₃-SCR catalyst. The denitration temperature was 100~400℃. The experimental results showed that the denitration activity of the original tailings was 7.6%, the denitration activity of γ-Al₂O₃ was 9.4%, and the denitration activity of rare earth tailings with 50% γ-Al₂O₃ reached 64.8%, That was to say, adding 50wt% γ-Al₂O₃ could denitrification activity of tailings greatly. The XRD results showed that γ-Al₂O₃ cann't react with tailings to form new materials. The SEM results showed that γ-Al₂O₃ was uniformly dispersed on the tailings when adding weight of γ-Al₂O₃ was less than 50%. If adding weight of γ-Al₂O₃ was more than 50%, γ-Al₂O₃ agglomerated on the tailings and showed poor dispersion. The results of NH₃-TPD showed that adding γ-Al₂O₃ can enhance the amount of acid sites. And the NH₃ adsorption first increased and then decresed with the increase of addition weight of γ-Al₂O₃. However, if addition weight of γ-Al₂O₃ was too low (15wt%, 35wt%), the amount of NH₃ adsorption was inadequate, resulting in incomplete catalytic reaction. The BET results showed that the specific surface area of tailings could be increased by adding γ-Al₂O₃.

Key words： rare earth tailings pseudo boehmite acid sites catalytic denitratio

Received: 06 January 2020

PACS:

X511

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	FU Jin-yan
	WANG Zhen-feng
	BAI Xin-rui
	CUI Meng-ke
	WU Wen-fei

Cite this article:

FU Jin-yan,WANG Zhen-feng,BAI Xin-rui等. Denitration performance of NH₃-SCR from γ-Al₂O₃ acid modified rare earth tailings[J]. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(9): 3741-3747.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2020/V40/I9/3741

[1]	皮冬勤,陈焕盛,魏巍,等.京津冀一次重污染过程的成因和来源[J]. 中国环境科学, 2019,39(5):109-118. Pi D Q, Chen H S, Wei W, et al. The causes and sources of a heavy-polluted event in Beijing-Tianjin-Hebei region[J]. China Environmental Science, 2019,39(5):109-118.
[2]	Yang G, Zhao H, Luo X, et al. Promotion effect and mechanism of the addition of Mo on the enhanced low temperature SCR of NOx by NH3 over MnOx/γ-Al2O3 catalysts.[J]. Applied Catalysis B:Environmental, 2019,245(245).
[3]	杨旭,张小玲,康延臻,等.京津冀地区冬半年空气污染天气分型研究[J]. 中国环境科学, 2017,37(9):3201-3209. Yang X, Zhang X L, Kang Y Z, et al. Circulation weather type cl-assification for air pollution over the Beijing-Tianjin-Hebei region during winte[J]. China Environmental Science, 2017,37(9):3201-3209.
[4]	Jeon M J, Park S H, Kim J M, et al. Removal of NOx at low temperature over mesoporous α-Mn2O3 catalyst[J]. Journal of Nanoscience and Nanotechnology, 2014,14(3):2527-2531.
[5]	Phil H H, Reddy M P, Kumar P A, et al. SO2 resistant antimony promoted V2O5/TiO2 catalyst for NH3-SCR of NOx at low temperatures[J]. Applied Catalysis B Environmental, 2008,78(3/4):301-308.
[6]	杜英,姚远.V2O5/TiO2催化剂脱除NO的研究[J]. 能源环境保护, 2014,28(1):22-24. Du Y, Yao Y. Study of selecyive catalytic reduction of NO over titanium supported vanadium catalysts[J]. Energy environmental protection, 2014,28(1):22-24.
[7]	刘亭,王廷春,吴瑞青,等.低温NH3-SCR脱硝催化剂研究进展[J]. 安全与环境学报, 2012,19(6):42-44. Liu T, Wang T C, Wu R Q, et al. Research advance review for low-temperature NH3-SCR catalysts[J]. Journal of Safety and Environment, 2012,19(6):42-44.
[8]	陈东.低温NH3-SCR脱硝催化剂研究进展[J]. 四川化工, 2016, 19(2):42-44. Chen D. Research progress in low temperature NH3-SCR of De-NOx catalysts.[J]. Sichuan Chemical Industry, 2016,19(2):42-44.
[9]	Ryu J C, Lee D H, Kang K S, et al. Effect of additives on redox behavior of iron oxide for chemical hydrogen storage[J]. Journal of Industrial & Engineering Chemistry, 2008,14(2):252-260.
[10]	He J, Li B, Mao J, et al. Erratum to:Four-electron oxygen reduction from mesoporous carbon modified with Fe2O3 nanocrystals[J]. Journal of Materials Science, 2017,52(18):10948-10949.
[11]	Shu Y, Sun H, Quan X, et al. Enhancement of catalytic activity over the iron-modified Ce/TiO2 catalyst for selective catalytic reduction of NOx with ammonia[J]. Journal of Physical Chemistry C, 2012, 116(48):25319-25327.
[12]	Sorescu M, Xu T, Burnett J D, et al. Investigation of LaFeO3 perovskite growth mechanism through mechanical ball milling of lanthanum and iron oxides[J]. Journal of Materials Science, 2011, 46(20):6709-6717.
[13]	Chang M J, Wang H, Li H L, et al. Facile preparation of novel Fe2O3/BiOI hybrid nanostructures for efficient visible light photocatalysis[J]. Journal of Materials Science, 2017.doi:10.1007/s10853-017-1813-z.
[14]	张光学,周安琪,范海燕,等.铁铈氧化物SCR脱硝催化剂的制备及性能[J]. 燃料化学学报, 2015,(10):118-123. Zhang G X, Zhou A Q, Fan H Y, et al.Preparation of Fe-Ce oxide SCR denitration catalyst and its performance study[J]. Journal of Fuel Chemistry and Technology, 2015,(10):118-123.
[15]	熊志波,路春美,等.铁铈复合氧化物催化剂SCR脱硝的改性研究[J]. 燃料化学学报, 2013,41(3):361-367. Xiong Z B, Lu CH Y, et al. Study on the modification of iron-cerium mixed oxide catalyst for selective catalytic reduction of NO[J]. Journal of Fuel Chemistry and Technology, 2013,41(3):361-367.
[16]	张志伟,徐斌,张毅敏,等.Go/(CeO2-TiO2)改性复合膜紫外光催化去除氨氮、DOC[J]. 中国环境科学, 2020,40(3):1116-1122. Zhang Z W, Xu B, Zhang Y M, et al. Ultraviolet photocatalytic removal of ammonia nitrogen and DOC by GO/(CeO2-TiO2) modified composite membrane[J]. China Environmental Science, 2020,40(3):1116-1122.
[17]	张悦,林海,董颖博,等.白云鄂博地区尾矿中铁、铌、稀土、萤石综合回收研究[J]. 稀有金属, 2017,41(7):799-809. Zhang Y, Lin H, Dong Y B, et al. Comprehensive recovery of iron, niobium, rare earth and fluorite in Bayan Obo tailings[J]Chinese Journal of Rare Metals, 2017,41(7):799-809.
[18]	余永富.白云鄂博矿稀土、铌资源综合利用研究意义重大[J]. 稀土信息, 2007,(8):8-9. Yu Y F. Research on comprehensive utilization of rare earth and niobium resources in Bayan Obo Mine is of great significance[J]. Rare Earth Information, 2007,(8):8-9.
[19]	赵海燕.包钢发展与白云鄂博矿产资源保护的思考[J]. 矿产保护与利用, 2007,(4):9-12. Zhao H Y. Thoughts of development and ore resources' saving of Baotou Iron & Steel (group) Co.ltd[J]. Conservation and Utilization of Mineral Resources, 2007,(4):9-12
[20]	王鑫,林海,董颖博,等.不同磁浮工艺对综合回收某稀土尾矿中稀土、铁、铌和萤石的影响[J]. 稀有金属, 2014,38(5):846-854. Wang X, Lin H, Dong Y B, et al. Recovery of rare-earth, iron, niobium and fluorite in rera-earth tailings with different magnetic separation and flotation technologies[J]. Chinese Journal of Rare Metals, 2014,38(5):846-854.
[21]	Liu J, Liu J, Zhao Z, et al. Fe〣eta@CeO2 core-shell catalyst with tunable shell thickness for selective catalytic reduction of NOx with NH3[J]. AIChE Journal, 2017,63(10):4430-4441.
[22]	Wang T, Zhu C, Liu H, et al. Performance of selective catalytic reduction of NO with NH3 over natural manganese ore catalysts at low temperature[J]. Environmental Technology, 2017,39(3):317-326.
[23]	乔南利,杨忆新,刘清龙,等.载体物化性质对锰铈催化剂NH3-SCR脱硝性能的影响[J]. 燃料化学学报, 2018,46(6):733-742. Qiao N L, Yang Y X, Liu L Q, et al. Influence of different supports on the physicochemical properties and denitration performance of the supported MnCe-based catalysts for NH3-SCR[J]. Journal of Fuel Chemistry and Technology, 2018,46(6):733-742.
[24]	Cao F, Su S, Xiang J, et al. Performances of Mn-Ce-Zr/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO[J]. Zhongguo Dianji Gongcheng Xuebao/Proceedings of the Chinese Society of Electrical Engineering, 2015,35(9):2238-2245.
[25]	方祺隆,朱宝忠,孙运兰,等.Mn-Fe/Al2O3催化剂的低温脱硝性能研究[J]. 分子催化, 2018,32(4):18-27. Fang Q L, Zhu B Z, Sun Y L, et al. Study on the performance of low temperature de-NOx based on Mn-Fe/Al2O3 catalysts[J]. Journal of Molecular Catalysis(China), 2018,32(4):18-27.
[26]	钱怡君,归柯庭,梁辉.负载型Fe-Ce催化剂低温SCR脱硝性能的研究[J]. 工程热物理学报, 2015,36(1):101-105. Qian Y J, Gui K T, Liang H, et al. Study on the performance of supported Fe-Ce catalyst for low temperature SCR denitration[J]. Journal of Engineering Thermophysics, 2015,36(1):101-105.
[27]	陈焕章,李宏,李花.负载型Mn-Fe/γ-Al2O3低温脱硝催化剂的性能[J]. 化工进展, 2016,35(4):1107-1112. Chen H ZH, Li H, Li H, et al. Denitration performance of supported Mn-Fe/γ-Al2O3 catalyst at low temperature[J]. Chemical Industry and Engineering Progress, 2016,35(4):1107-1112.
[28]	王晓波,归柯庭.负载型铁基催化剂低温SCR脱硝实验研究[A]//江苏省工程热物理学会第六届学术会议论文集[C]. 江苏省工程热物理学会, 2012:711-716. Wang X B, Gui K T. Experimental study on low temperature SCR denitration with supported iron-based catalyst[A]//Proceedings of the Sixth Academic Conference of Jiangsu Engineering Thermophysics Society[C]. Jiangsu Engineering Thermophysics Society, 2012:711-716.
[29]	王宽岭,王学海,刘忠生.Mn-Fe-Ce/Al2O3/堇青石催化剂低温NH3-SCR脱硝性能研究[J]. 当代化工, 2015,44(9):2057-2060. Wang K L, Wang X H, Liu ZH SH. Low-temperature NH3-SCR denitrification performance of Mn-Fe-Ce/Al2O3/cordierite monolithic catalyst[J]. Contemporary Chemical Industry, 2015,44(9):2057-2060.
[30]	Cao F, Su S, Xiang J, et al. The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO with NH3[J]. Fuel., 2015,13(9)232-239.
[31]	黄秀兵,王鹏.CeO2修饰Mn-Fe-O复合材料及其NH3-SCR脱硝催化性能[J]. 无机材料学报, 2020,(4):1-8. Huang X B, Wang P. CeO2 modified Mn-Fe-O composites and their catalytic performance for NH3-SCR of NO[J]. Journal of Inorganic Materials, 2020,(4):1-8.
[32]	Han J, Meeprasert J, Maitarad P, et al. Investigation of the facet-dependent catalytic performance of Fe2O3/CeO2 for the selective catalytic reduction of NO with NH3[J]. The Journal of Physical Chemistry C, 2016,120(3):1523-1533.
[33]	Neri G, Visco A M, et al. Au/iron oxide catalysts:Temperature programmed reduction and X-ray diffraction characterization[J]. Thermochimica Acta, 1999,329(1):39-46.
[34]	Fang N, Guo J, Shu S, et al. Enhancement of low-temperature activity and sulfur resistance of Fe0.3Mn0.5Zr0.2, catalyst for NO removal by NH3-SCR[J]. Chemical Engineering Journal, 2017,325:114-123.
[35]	黄雅楠,王振峰,武文斐.稀土尾矿催化剂脱硝性能研究[J]. 稀有金属, 2019,(4)1-7. Huang Y N, Wang Z F, Wu W F, et al. Study on Denitration performance of rare earth tailings catalyst[J]. Chinese Journal of Rare Metals, 2019,(4):1-7.
[36]	Mu K D, Oliver R K, Martin Er, et al. Characterization and catalytic investigation of Fe-ZSM-5for urea-SCR[J]. Catalysis Today, 119(1-4):137-144.
[37]	Liu F, 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.
[38]	Gérard D, Valade D, Ariel G V, et al. Selective catalytic reduction of nitric oxide with ammonia on Fe-ZSM-5catalysts prepared by different methods[J]. Applied Catalysis B Environmental, 2005,55(2):149-155.
[39]	Zhang D, Yang R T.NH3 -SCR of NO over one-pot Cu-SAPO-34catalyst:Performance enhancement by doping Fe and MnCe and insight into N2O formation[J]. Applied Catalysis A:General, 2017,543(5):247-256.