γ-Al2O3酸性修饰稀土尾矿NH3-SCR脱硝性能

摘要
图/表
参考文献
相关文章 (1)

全文: PDF (1485 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要为增加脱硝催化剂的酸性位点和比表面积，以稀土尾矿为活性主体，通过物理球磨方式添加γ-Al₂O₃，制得NH₃-SCR催化剂，脱硝温度为100~400℃.结果表明：原尾矿脱硝活性为7.6%，γ-Al₂O₃的脱硝活性为9.4%，稀土尾矿添加50%γ-Al₂O₃脱硝活性达到了64.8%，即添50%γ-Al₂O₃后加极大程度地提高了尾矿的脱硝活性.XRD实验结果表明：Al₂O₃不会与尾矿成分发生反应生成新的物质.SEM实验结果表明：当添加γ-Al₂O₃低于50%时，γ-Al₂O₃均匀分散在尾矿表面，当添加65%γ-Al₂O₃和80%γ-Al₂O₃时，γ-Al₂O₃发生团聚，分散性较差.NH₃-TPD实验结果表明：添加γ-Al₂O₃为脱硝催化剂增加酸性位点，但是当添加γ-Al₂O₃过低时（15%、35%），吸附NH₃量不足，催化反应进行不完全.BET实验结果表面：添加γ-Al₂O₃可以增加尾矿的比表面积.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	付金艳
	王振峰
	白心蕊
	崔梦壳
	武文斐

关键词 ：稀土尾矿, 拟薄水铝石, 酸性位点, 催化脱硝

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

收稿日期: 2020-01-06

PACS:

X511

基金资助:国家自然科学基金资助项目（51866013），内蒙古自治区自然科学基金资助项目（2019ZD13，2017MS（LH））；内蒙古自治区重大基础研究开放课题资助（0406091701）

通讯作者: 武文斐,教授,wwf@imust.cn E-mail: wwf@imust.cn

作者简介: 付金艳(1996-),女,内蒙古赤峰人,内蒙古科技大学硕士研究生,主要从事稀土尾矿基催化剂制备研究.

引用本文:

付金艳, 王振峰, 白心蕊, 崔梦壳, 武文斐. γ-Al₂O₃酸性修饰稀土尾矿NH₃-SCR脱硝性能[J]. 中国环境科学, 2020, 40(9): 3741-3747. FU Jin-yan, WANG Zhen-feng, BAI Xin-rui, CUI Meng-ke, WU Wen-fei. Denitration performance of NH₃-SCR from γ-Al₂O₃ acid modified rare earth tailings. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(9): 3741-3747.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/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.