钒基催化剂同步去除燃煤烟气中甲苯与NO<sub><i>x</i></sub>研究

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摘要采用不同工艺制备V₂O₅-WO₃-MoO_x/TiO₂堇青石整体式催化剂，以甲苯和NO为探针分子，考察了Mo的负载量、涂覆方法、粘结剂的种类等制备工艺对整体式催化剂性能的影响，用XRD、SEM-EDS、FT-IR、BET等技术对催化剂进行了表征分析.结果表明，采用涂敷法，以添加量为1%的甲基纤维素为粘结剂所制备的V1W6Mo3/TiO₂堇青石蜂窝陶瓷整体式催化剂具有最优活性和稳定性（T₉₀为307℃，负载率为28.26%，脱落率为6.81%），在燃煤烟气中具有优异的同步去除VOCs与NO性能，甲苯去除率可达99%，NO去除率为100%，N₂选择性为99%.XRD、SEM-EDS表明V、W、Mo活性组分分布均匀且高度分散.FT-IR证明添加甲基纤维素的整体式催化剂具有优异的抗硫性能.

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	张益兰
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	付名利
	胡芸

关键词 ：燃煤烟气, 催化氧化, 整体式催化剂, VOCs与NO_x同步去除

Abstract：V₂O₅-WO₃-MoO_x/TiO₂ cordierite monolithic catalyst was prepared by different synthetic methods. Using toluene and NO as probe molecules, the effects of Mo loading, coating method and binder type on the performance of monolithic catalyst were investigated. XRD, SEM-EDS, FT-IR and BET techniques were used to characterize the catalysts. The results showed that V1W6MO3/TiO₂ cordierite honeycomb ceramic monolithic catalyst prepared by coating method with 1% methyl cellulose as binder had the highest activity and stability (T₉₀=307℃, load rate=28.26%, shedding rate=6.81%), and had excellent performance of simultaneous removal of VOCs and NO in the flue gas of coal burning (toluene removal rate=99%, NO removal rate=100%, N₂ selectivity=99%). XRD and SEM-EDS showed that the active components of V, W and Mo were evenly distributed and highly dispersed. FT-IR showed that the monolithic catalyst with methyl cellulose added had excellent SO₂ resistance performance.

Key words： coal-fired flue gas catalytic oxidation monolithic catalyst synergistic removal of VOCs and NO_x

收稿日期: 2021-01-13

PACS:

X511

基金资助:国家重点研发计划项目（2018YFB0605200）；广州市科技计划项目（201804020026）

通讯作者: 胡芸,教授,huyun@scut.edu.cn E-mail: huyun@scut.edu.cn

作者简介: 张益兰(1996-),女,河南信阳人,华南理工大学硕士研究生,主要从事催化氧化挥发性有机化合物(VOCs)技术研究.发表论文1篇.

引用本文:

张益兰, 肖高飞, 李剑晗, 杜玥莹, 付名利, 胡芸. 钒基催化剂同步去除燃煤烟气中甲苯与NO_x研究[J]. 中国环境科学, 2021, 41(8): 3546-3554. ZHANG Yi-lan, XIAO Gao-fei, LI Jiang-han, DU Yue-ying, FU Ming-li, HU Yun. Synergistic removal of toluene and NO_x on vanadium-based catalyst. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(8): 3546-3554.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I8/3546

[1]	Boltic Z, Ruzic N, Jovanovic M, et al. Cleaner production aspects of tablet coating process in pharmaceutical industry:problem of VOCs emission[J]. Journal of Cleaner Production, 2013,44:123-132.
[2]	Yan Y, Yang C, Peng L, et al. Emission characteristics of volatile organic compounds from coal-, coal gangue-, and biomass-fired power plants in China[J]. Atmospheric Environment, 2016,143(11):261-269.
[3]	Ding Y, Lu J, Liu Z, et al. Volatile organic compounds in Shihezi, China, during the heating season:pollution characteristics, source apportionment, and health risk assessment[J]. Environmental Science and Pollution Research, 2020,27(14):16439-16450.
[4]	Yang H H, Gupta S K, Dhital N B, et al. Comparative investigation of coal-and oil-fired boilers based on emission factors, ozone and secondary organic aerosol formation potentials of VOCs[J]. Journal of Environmental Sciences, 2020,92:245-255.
[5]	Guttikunda S K, Jawahar P. Atmospheric emissions and pollution from the coal-fired thermal power plants in India[J]. Atmospheric Environment, 2014,92:449-460.
[6]	Deepak P, Jeong H K, Sang H Lee, et al. Hazardous air pollutants emission from coal and oil-fired power plants[J]. Asia-Pacific Journal of Chemical Engineering, 2010,5(2):299-303.
[7]	Fernández-Martínez G, López-Mahía P, Muniategui-Lorenzo S, et al. Distribution of volatile organic compounds during the combustion process in coal-fired power stations[J]. Atmospheric Environment, 2001,35(33):5823-5831.
[8]	SHI J, DENG H, BAI Z, et al. Emission and profile characteristic of volatile organic compounds emitted from coke production, iron smelt, heating station and power plant in Liaoning Province, China[J]. Science of the Total Environment, 2015,515:101-108.
[9]	徐静颖,卓建坤,姚强.燃煤有机污染物生成排放特性与采样方法研究进展[J]. 化工学报, 2019,70(8):2823-2834. Xu J Y, Zhuo J K, Yao Q. Research progress on formation, emission characteristics and sampling methods of organic compounds from coal combustion[J]. Journal of Chemical Industry and Engineering (China), 2019,70(8):2823-2834.
[10]	李津津,陈扉然,马修卫,等.燃煤有机污染物排放及其控制技术研究展望[J]. 化工进展, 2019,38(12):5539-5547. Li J J, Chen F R, Ma X W, et al. Emission of coal-fired VOCs and prospect of control technology[J]. Chemical Industry and Engineering Progress, 2019,38(12):5539-5547.
[11]	耿新泽,段钰锋,胡鹏,等.SCR气氛下Ce-W/TiO2催化剂的脱硝协同脱汞特性[J]. 中国环境科学, 2019,39(4):77-84. Geng X Z, Duan Y F, Hu P, et al. Characteristics of denitrification and mercury removal of Ce-W/TiO2 catalysts in SCR atmosphere[J]. China Environmental Science, 2019,39(4):77-84.
[12]	Kamal M S, Razzak S A, Hossain M M. Catalytic oxidation of volatile organic compounds (VOCs)-A review[J]. Atmospheric Environment, 2016,140(9):117-134.
[13]	Yang G T, Miao G,Pi Y, et al. Abatement of various types of VOCs by adsorption/catalytic oxidation:A review[J]. Chemical Engineering Journal, 2019,370:1128-1153.
[14]	Sungkono I E, Kameyama H, Koya T. Development of catalytic combustion technology of VOC materials by anodic oxidation catalyst[J]. Applied Surface Science, 1997,121:425-428.
[15]	Zhang X, Wu D. Ceramic monolith supported Mn-Ce-M ternary mixed-oxide (M=Cu, Ni or Co) catalyst for VOCs catalytic oxidation[J]. Ceramics International, 2016,42(15):16563-16570.
[16]	周瑛,卢晗锋,张宏华,等.LaBO3钙钛矿催化剂的VOCs催化燃烧特性[J]. 中国环境科学, 2012,32(10):1772-1777. Zhou Y, Lu H F, Zhang H H, et al. Catalytic properties of LaBO3 perovskite catalysts in VOCs combustion[J]. China Environmental Science, 2012,32(10):1772-1777.
[17]	刘双,卜龙利,宁珂,等.整体式分子筛基催化剂制备及其微波催化燃烧VOCs[J]. 中国环境科学, 2020,40(11):4688-4696. Liu S, Bo L L, Ning K, et al. Preparation and application of monolithic molecular sieve-based catalysts in microwave catalytic combustion of VOCs[J]. China Environmental Science, 2020,40(11):4688-4696.
[18]	Busca G, Baldi M, Pistarino C, et al. Evaluation of V2O5-WO3-TiO2 and alternative SCR catalysts in the abatement of VOCs[J]. Catalysis Today, 1999,53(4):525-533.
[19]	Lazr L, Kser H, Balasanian I, et al. Catalytic destruction of aromatic VOCs on SCR-DeNOx commercial catalyst[J]. Environmental Engineering and Management Journal, 2007,6(1):13-20.
[20]	Wei Y, Jiang, Y L, Feng B, et al. Synergistic elimination of NOx and chloroaromatics on a commercial V2O5-WO3-TiO2 catalyst:Byproduct analyses and the SO2 effect[J]. Environmental Science & Technology, 2019,53(21):12657-12667.
[21]	Li C, Brewe D, Lee J Y. Effects of impregnation sequence for Mo-modified V-based SCR catalyst on simultaneous Hg(0) oxidation and NO reduction[J]. Applied Catalysis B:Environmental, 2020,270:118854.
[22]	Zhang P, Pan W G, Guo R T, et al. The Mo modified Ce/TiO2 catalyst for simultaneous Hg0 oxidation and NO reduction[J]. Journal of the Energy Institute, 2018, 92(5):1313-1328.
[23]	Sun X, Guo R T, Liu J, et al. The enhanced SCR performance of Mn/TiO2 catalyst by Mo modification:Identification of the promotion mechanism[J]. International Journal of Hydrogen Energy, 2018,43(33):16038-16048.
[24]	司涵,黄琼,陶涛,等.La-M-Co-O/堇青石催化剂的制备及催化氧化氯苯[J]. 中国环境科学, 2020,40(10):4314-4322. Si H, Huang Q, Tao T, et al. Study on the preparation and catalytic oxidation of chlorobenzene over La-M-Co-O/cordierite catalysts.[J]. China Environmental Science, 2020,40(10):4314-4322.
[25]	Zhao Q, Zheng Y F, Song C F, et al. Novel monolithic catalysts derived from in-situ decoration of Co3O4 and hierarchical Co3O4@MNOx on Ni foam for VOC oxidation[J]. Applied Catalysis B:Environmental, 2020,265:118-132.
[26]	Shang X, Hu G, 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.
[27]	Lin C, Liao Y F, Xin S R, et al. Simultaneous removal of NO and volatile organic compounds (VOCs) by Ce/Mo doping-modified selective catalytic reduction (SCR) catalysts in denitrification zone of coal-fired flue gas[J]. Fuel, 2020,262:116485.
[28]	Liu X, Yan J, Mao J, et al. Inhibitor, co-catalyst, or intermetallic promoter? Probing the sulfur-tolerance of MoOx surface decoration on Ni/SiO2 during methane dry reforming[J]. Applied Surface Science, 2021,548:149231.
[29]	Hou Z,Jie F, Tao L, et al. The performance of manganese-based catalysts with Ce0.65Zr0.35O2 as support for catalytic oxidation of toluene[J]. Applied Surface Science, 2018,434:82-90.
[30]	Polina, A Z, Andrey V S, Sergey N, et al. Synthesis, characterization, and sulfur tolerance of Pt−x catalysts prepared from Pt−Mo alloy precursors[J]. Journal of Physical Chemistry C, 2007,111(40):14790-14798.
[31]	Klimczak M, Kern P, Heinzelmann T, et al. High-throughput study of the effects of inorganic additives and poisons on NH3-SCR catalysts-Part I:V2O5-WO3/TiO2 catalysts[J]. Applied Catalysis B Environmental, 2010,95(1/2):39-47.
[32]	Lietti L, Nova I, Ramis G, et al. Characterization and reactivity of V2O5-MoO3/TiO2 de-NOx SCR catalysts[J]. Journal of catalysis, 1999,187(2):419-435.
[33]	Lee M, Ye B, Jeong B, et al. Reduced graphene oxide supported V2O5-WO3-TiO2 catalysts for selective catalytic reduction of NOx[J]. Korean Journal of Chemical Engineering, 2018,35(10):1988-1993.
[34]	Shang X, Hu G, 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.
[35]	Kong M, Liu Q, Wang X, et al. Performance impact and poisoning mechanism of arsenic over commercial V2O5-WO3/TiO2 SCR catalyst[J]. Catalysis Communications, 2015,72:121-126.
[36]	于艳科,何炽,陈进生,等.电厂烟气脱硝催化剂V2O5-WO3/TiO2失活机理研究[J]. 燃料化学学报, 2012,40(11):1359-1365. Yu Y K, He C, Chen J S, et al. Deactivation mechanism of de-NOx catalyst (V2O5-WO3/TiO2) used in coal fired power plant[J]. Journal of Fuel Chemistry and Technology, 2012,40(11):1359-1365.