MnCeOx@MgO催化剂上同步脱除NOx和氯苯的研究
Study on Simultaneous Removal of NOx and Chlorobenzene over MnCeOx@MgO Catalyst
DOI: 10.12677/HJCET.2022.124039, PDF,    国家科技经费支持
作者: 郑余凡, 陈郑辉, 凌 鑫, 潘 华*：浙江树人学院生物与环境工程学院，浙江 杭州
关键词: MnCeOx@MgO；氮氧化物还原；氯苯氧化；同步脱除；MnCeOx@MgO； NOx Reduction； Chlorobenzene Oxidation； Simultaneous Removal
摘要: 采用水热法和共沉淀法分别制备了MnCeOx@MgO核壳催化剂和MnCeMgOx复合金属氧化物催化剂，通过催化活性评价和催化表征考察了MnCeOx@MgO催化剂和MnCeMgOx复合金属催化剂上同步脱除氮氧化物(NOx)和氯苯(CB)的构效关系。活性测试结果表明，MnCeOx@MgO核壳催化剂的催化活性强于MnCeMgOx复合金属氧化物催化剂，且MnCeOx@MgO核壳催化剂具有更宽的活性温度窗口。其中NOx和CB在MnCeOx@MgO核壳催化剂上的转化率分别在250℃和350℃达到77%和84%，NOx和CB在MnCeMgOx复合金属催化剂的转化效率分别为62.6% (200℃)和89% (350℃)。MnCeOx@MgO催化剂的活性与其物化结构、表面活性氧物种比值和过渡金属活性组分的形态有关。MnCeOx@MgO核壳催化剂的平均孔径和Olatt/Oads比值均大于MnCeMgOx复合金属催化剂，与催化活性成正相关。催化剂中活性组分分别为Mn2+、Mn3+、Mn4+、Ce3+。
Abstract: MnCeOx@MgO core-shell catalyst and MnCeMgOx composite catalyst were prepared by hydrothermal method and coprecipitation method, respectively. Structure-activity relationship in simultaneous removal of NOx and chlorobenzene (CB) on MnCeOx@MgO and MnCeMgOx catalysts was investigated by catalytic activity test and characterization. The results show that the activity of MnCe-Ox@MgO catalyst is higher than that of MnCeMgOx catalyst. For MnCeOx@MgO core-shell catalyst, the conversion of NOx and CB was 77% and 84% at 250˚C and 350˚C, respectively. For MnCeMgOx composite catalyst, the conversion of NOx and CB was 62.6% and 89% at 200˚C and 350˚C, respectively. The activity of MnCeOx@MgO catalyst is related to its physicochemical structure, surface active oxygen species ratio and the morphology of transition metal active components. Both average pore size and Olatt/Oads ratio of MnCeOx@MgO catalysts are higher than those of MnCeMgOx catalysts, which were positively correlated with the catalytic activity. The active components in MnCeOx@MgO catalyst are Mn2+, Mn3+, Mn4+, Ce3+ respectively.
文章引用：郑余凡, 陈郑辉, 凌鑫, 潘华. MnCeOx@MgO催化剂上同步脱除NOx和氯苯的研究[J]. 化学工程与技术, 2022, 12(4): 292-301. https://doi.org/10.12677/HJCET.2022.124039

参考文献

[1] Huang, X., Wang, D., Yang, Q., Peng, Y. and Li, J. (2021) Multi-Pollutant Control (MPC) of NO and Chlorobenzene from Industrial Furnaces Using a Vanadia-Based SCR Catalyst. Applied Catalysis B: Environmental, 285, Article ID: 119835. [Google Scholar] [CrossRef] 
[2] Li, J., He, H., Hu, C. and Zhao, J. (2013) The Abatement of Major Pollutants in Air and Water by Environmental Catalysis. Frontiers of Environmental Science & Engineering, 7, 302-325. [Google Scholar] [CrossRef] [PubMed]
[3] Everaert, K. and Baeyens, J. (2004) Removal of PCDD/F from Flue Gases in Fixed or Moving Bed Adsorbers. Waste Management, 24, 37-42. [Google Scholar] [CrossRef] 
[4] Stuart, H., Taylor, S.H., Heneghan, C.S., Hutchings, G.J. and Hudson, I.D. (2000) The Activity and Mechanism of Uranium Oxide Catalysts for the Oxidative Destruction of Volatile Organic Compounds. Catalysis Today, 59, 249-259. [Google Scholar] [CrossRef] 
[5] Forzatti, P. and Lietti, L. (1999) Catalyst Deactivation. Catalysis Today, 52, 165-181. [Google Scholar] [CrossRef] 
[6] Weng, X., Sun, P., Long, Y., Meng, Q. and Wu, Z. (2017) Catalytic Oxidation of Chlorobenzene over MnxCe1-xO2/HZSM-5 Catalysts: A Study with Practical Implications. Environmental Science & Technology, 51, 8057-8066. [Google Scholar] [CrossRef] [PubMed]
[7] Gallastegi-Villa, M., Aranzabal, A., Gonzalez-Marcos, J.A. and Gonzalez-Velasco, J.R. (2016) Metal-Loaded ZSM5 Zeolites for Catalytic Purification of Dioxin/Furans and NOx Containing Exhaust Gases from MWI Plants: Effect of Different Metal Cations. Applied Catalysis B: Environmental, 184, 238-245. [Google Scholar] [CrossRef] 
[8] Zhang, P., Lu, H., Zhou, Y., Zhang, L., Wu, Z., Yang, S., Shi, H., Zhu, Q., Chen, Y. and Dai, S. (2015) Mesoporous MnCeOx Solid Solutions for Low Temperature And Selective Oxidation of Hydrocarbons. Nature Communications, 6, Article No. 8446. [Google Scholar] [CrossRef] [PubMed]
[9] Delimaris, D. and Ioannides, T. (2008) VOC Oxidation over MnOx-CeO2 Catalysts Prepared by a Combustion Method. Applied Catalysis B: Environmental, 84, 303-312. [Google Scholar] [CrossRef] 
[10] Gan, L., Wang, Y., Chen, J., Yan, T., Li, J., Crittenden, J. and Peng, Y. (2019) The Synergistic Mechanism of NOx and Chlorobenzene Degradation in Municipal Solid Waste Incinerators. Catalysis Science & Technology, 9, 4286-4292. [Google Scholar] [CrossRef] 
[11] Jampaiah, D., Ippolito, S.J., Sabri, Y.M., Reddy, B.M. and Bhargava, S.K. (2015) Highly Efficient Nanosized Mn and Fe Codoped Ceria-Based Solid Solutions for Elemental Mercury Removal at Low Flue Gas Temperatures. Catalysis Science & Technology, 5, 2913-2924. [Google Scholar] [CrossRef] 
[12] Venkataswamy, P., Rao, K.N., Jampaiah, D. and Reddy, B.M. (2015) Nanostructured Manganese Doped Ceria Solid Solutions for CO Oxidation at Lower Temperatures. Applied Catalysis B: Environmental, 162, 122-132. [Google Scholar] [CrossRef] 
[13] Han, J., Meeprasert, J., Maitarad, P., Nammuangruk, S., Shi, L. and Zhang, D. (2016) Investigation of the Facet-Dependent Catalytic Performance of Fe2O3/CeO2 for the Selective Catalytic Reduction of NO with NH3. The Journal of Physical Chemistry C, 120, 1523-1533. [Google Scholar] [CrossRef] 
[14] Pan, H., Jian, Y. and Chen C. (2017) Sphere-Shaped Mn3O4 Catalyst with Remarkable Low-Temperature Activity for Methyl-Ethyl-Ketone Combustion. Environmental Science & Technology, 51, 6288-6297. [Google Scholar] [CrossRef] [PubMed]
[15] 仲蕾. 铬基催化剂的制备及其催化氧化NO的性能研究[D]: [博士学位论文]. 南京: 南京理工大学, 2016.
[16] 任丽丽. 担载型分子筛催化剂上CH4选择还原NO反应的研究[D]: [博士学位论文]. 大连: 中国科学院大连化学物理研究所, 2003.