Performance enhancement mechanism of Mn-based catalysts prepared under N2 for NOx removal: Evidence of the poor crystallization and oxidation of MnOx

doi:10.1016/S1872-2067(17)62814-6

Abstract

Abstract:

Among multitudinous metal-oxide catalysts for the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR), Mn-based catalysts have become very popular and developed rapidly in recent years because of its superior low-temperature denitrification activity, mainly originating from multi-valence of Mn. Most studies suggest that the catalytic activity of multi-component oxides is superior to that of single-component catalysts owing to the synergistic effect among the metallic elements in such materials, of which more attentions have been given to Ce as an additive owing to its powerful oxygen storage capacity, redox ability and its ready availability. As the core of SCR technology, the research points in catalyst development at the present stage of all researchers in countries mainly centralize on the optimization of active components, carriers, calcination temperature, calcination time and temperature-raising procedure, giving little thought to the effects of the calcination atmosphere. In the present work, Ce-modified Mn-based catalysts were prepared by a simple impregnation method. The effects of the calcination atmosphere (N₂, air or O₂) on the performance of the resulting materials during NH₃-SCR and its causes of the differences were subsequently investigated and characterized using various analytical methods. Data obtained from X-ray diffraction, thermogravimetry and temperature-programmed reduction with hydrogen show that calcination under N₂ reduces both the degree of oxidation and crystallization of the MnO_x. Scanning electron microscopy also demonstrates that the use of N₂ inhibits the growth of grains and increases the dispersion of the catalysts. In addition, the results of temperature-programmed desorption with ammonia indicate that catalysts calcined under N₂ exhibit a greater quantity of acid sites. Finally, X-ray photoelectron spectrometry and activity results demonstrate that MnO_x in the lower valence states is more favorable for NH₃-SCR reactions. In conclusion, catalysts calcined under N₂ show superior performance during NH₃-SCR for NO_x removal, allowing NO conversions up to 94% at 473 K.

Key words: Mn-based catalyst, Selective catalytic reduction, Calcination atmosphere, Mn species, Oxidation degree, Crystallization degree

Kai Qi, Junlin Xie, De Fang, Fengxiang Li, Feng He. Performance enhancement mechanism of Mn-based catalysts prepared under N₂ for NO_x removal: Evidence of the poor crystallization and oxidation of MnO_x[J]. Chinese Journal of Catalysis, 2017, 38(5): 845-852.

×
share this article

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(17)62814-6

https://www.cjcatal.com/EN/Y2017/V38/I5/845

References

[1] P. Forzatti, Appl. Catal. A, 2001, 222, 221–236.
[2] B. J. Wu, X. Q. Liu, S. G. Wang, L. Zhu, L. Y. Cao, J. Combust. Sci. Technol., 2008, 14, 221–226.
[3] J. F. Zhang, H. J. Li, Z. Q. Tong, Y. Huang, S. A. Li, Natur. Sci. J. Xiangtan Univ., 2011, 33(2), 65–72, 77.
[4] Z. B. Wu, B. Q. Jiang, Y. Liu, H. Q. Wang, R. B. Jin, Environ. Sci. Technol., 2007, 41, 5812–5817.
[5] Z. B. Wu, B. Q. Jiang, Y. Liu, Appl. Catal. B, 2008, 79, 347–355.
[6] M. Kantcheva, J. Catal., 2001, 204, 479–494.
[7] B. J. Wu, W. B. Zhu, J. Ma, C. Xu, C. W. Jiang, L. Lü, Thermal Power Generation, 2010, 39(12), 23–28, 34.
[8] D. Fang, J. L. Xie, D. Mei, Y. M. Zhang, F. He, X. Q. Liu, Y. M. Li, RSC Adv., 2014, 4, 25540–25551.
[9] P. G. Smirniotis, D. A. Peña, B. S. Uphade, Angew. Chem. Int. Ed., 2001, 40, 2479–2482.
[10] W. G. Pan, J. N. Hong, R. T. Guo, W. L. Zhen, H. L. Ding, Q. Jin, C. G. Ding, S. Y. Guo, J. Ind. Eng. Chem., 2014, 20, 2224–2227.
[11] B. Thirupathi, P. G. Smirniotis, Appl. Catal. B, 2011, 110, 195–206.
[12] H. Hu, J. L. Xie, D. Fang, H. F. Cui, Z. Zhang, D. Mei, F. He, J. Wuhan Univ. Technol., 2015, 37(2), 5–10.
[13] Y. Xu, D. J. Yan, X. M. Huang, Y. Yu, S. J. Liu, Chin. J. Environ. Eng., 2015, 9, 862–866.
[14] D. J. Yan, Y. Xu, X. M. Huang, Y. Yu, S. J. Liu, Acta Sci. Circum., 2015, 35, 1697–1702.
[15] Y. X. Wu, H. T. Kao, J. R. Fang, B. X. Lei, L. Wang, Mater. Rev., 2014, 28(4), 75–79.
[16] K. Shen, Y. P. Zhang, X. L. Wang, H. T. Xu, K. Q. Sun, C. C. Zhou, J. Energy Chem., 2013, 22, 617–623.
[17] Z. B. Wu, R. B. Jin, Y. Liu, H. Q. Wang, Catal. Commun., 2008, 9, 2217–2220.
[18] Z. Y. Sheng, Y. F. Hu, J. M. Xue, X. M. Wang, W. P. Liao, J. Rare Earths, 2012, 30, 676–682.
[19] Y. Xiong, C. J. Tang, X. J. Yao, L. Zhang, L. L. Li, X. B. Wang, Y. Deng, F. Gao, L. Dong, Appl. Catal. A, 2015, 495, 206–216.
[20] L. Li, Y. F. Diao, X. Liu, J. Rare Earths, 2014, 32, 409–415.
[21] Z. M. Liu, Y. Yi, S. X. Zhang, T. L. Zhu, J. Z. Zhu, J. G. Wang, Catal. Today, 2013, 216, 76–81.
[22] S. Andreoli, F. A. Deorsola, R. Pirone, Catal. Today, 2015, 253, 199–206.
[23] Z. M. Liu, J. Z. Zhu, J. H. Li, L. L. Ma, S. I. Woo, ACS Appl. Mater. Interfaces, 2014, 6, 14500–14508.
[24] G. Qi, R. T. Yang, R. Chang, Catal. Lett., 2003, 87, 67–71.
[25] L. Xu, X. S. Li, M. Crocker, Z. S. Zhang, A. M. Zhu, C. Shi, J. Mol. Catal. A, 2013, 378, 82–90.
[26] X. Q. Wang, A. J. Shi, Y. F. Duan, J. Wang, M. Q. Shen, Catal. Sci. Technol., 2012, 2, 1386–1395.
[27] G. J. Wang, Chem. React. Eng. Technol., 2013, 29, 157–163.
[28] L. Y. Bai, Y. M. Zhou, Y. W. Zhang, H. Liu, X. L. Sheng, Y. Z. Duan, Catal. Commun., 2009, 10, 2013–2017.
[29] H. Slimen, H. Lachheb, S. Qourzal, A. Assabbane, A. Houas, J. Environ. Chem. Eng., 2015, 3, 922–929.
[30] X. Yan, X. D. Lü, X. Wang, C. H. Luan, J. C. Fan, W. Huang, Nat. Gas Chem. Ind., 2015, 40, 33–38.
[31] R. Klaysri, S. Wichaidit, T. Tubchareon, S. Nokjan, S. Piticharoenphun, O. Mekasuwandumrong, P. Praserthdam, Ceram. Int., 2015, 41, 11409–11417.
[32] E. W. Wang, L. Hu, S. M. Lei, S. J. Zhang, S. C. Zhang,W. Q. Gong, Appl. Clay Sci., 2015, 118, 138–150.
[33] J. L. Xie, D. Fang, F. He, J. F. Chen, Z. B. Fu, X. L. Chen, Catal. Commun., 2012, 28, 77–81.
[34] D. Fang, F. He, J. L. Xie, Z. B. Fu, J. F. Chen, J. Wuhan Univ. Technol. Mater. Sci. Ed., 2013, 28, 888–892.
[35] D. Fang, [Ph D Dissertation], Wuhan University of Technology, Wuhan, 2015.
[36] E. R. Stobbe, B. A. de Boer, J. W. Geus, Catal. Today, 1999, 47, 161–167.
[37] R. D. Zhang, H. Alamdari, S. Kaliaguine, Appl. Catal. A, 2008, 340, 140–151.
[38] D. Fang, J. L. Xie, H. Hu, H. Yang, F. He, Z. B. Fu, Chem. Eng. J., 2015, 271, 23–30.
[39] L. B. Xiong, J. L. Li, B. Yang, Y. Yu, J. Nanomater., 2012, 2012(5-8), 9.
[40] Y. Izumi, Y. Iwata, K. I. Aika, J. Phys. Chem., 1996, 100, 9421–9428.
[41] M. Stanciulescu, G. Caravaggio, A. Dobri, J. Moir, R. Burich, J. P. Charland, P. Bulsink, Appl. Catal. B, 2012, 123-124, 229–240.
[42] Q. Li, X. X. Hou, H. S. Yang, Z. X. Ma, J. W. Zheng, F. Liu, X. B. Zhang, Z. Y. Yuan, J. Mol. Catal. A, 2012, 356, 121–127.
[43] Q. Y. Liu, Z. Y. Liu, C. Y. Li, Chin. J. Catal., 2006, 27, 636–646.
[44] Q. Li, H. S. Yang, F. M. Qiu, X. B. Zhang, J. Hazard. Mater., 2011, 192, 915–921.
[45] W. Tian, H. S. Yang, X. Y. Fan, X. B. Zhang, J. Hazard. Mater., 2011, 188, 105–109.
[46] M. Romeo, K. Bak, J. El. Fallah, F. Le. Normand, L. Hilaire, Surf. Interface Anal., 1993, 20, 508–512.
[47] M. Kang, E. D. Park, J. M. Kim, J. E. Yie, Appl. Catal. A, 2007, 327, 261–269.
[48] F. Wang, H. X. Dai, J. G. Deng, G. M. Bai, K. M. Ji, Y. X. Liu, Environ. Sci. Technol., 2012, 46, 4034–4041.
[49] X. Gao, Y. Jiang, Y. Zhong, Z. Y. Luo, K. F. Cen, J. Hazard. Mater., 2010, 174, 734–739.
[50] C. J. Tang, H. L. Zhang, L. Dong, Catal. Sci. Technol., 2016, 6, 1248–1264.
[51] G. Qi, R. T. Yang, R. Chang, Appl. Catal. B, 2004, 51, 93–106.
[52] G. Qi, R. T. Yang, Appl. Catal. B, 2003, 44, 217–225.
[53] Z. X. Ma, H. S. Yang, Q. Li, J. W. Zheng, X. B. Zhang, Appl. Catal. A, 2012, 427–428, 43–48.
[54] X. D. Huang, Z. X. Ma, W. H. Lin, F. Liu, H. S. Yang, Catal. Commun., 2017, 91, 53–56.

Performance enhancement mechanism of Mn-based catalysts prepared under N₂ for NO_x removal: Evidence of the poor crystallization and oxidation of MnO_x

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

[1]	Xiaona Liu, Yi Cao, Nana Yan, Chao Ma, Lei Cao, Peng Guo, Peng Tian, Zhongmin Liu. Cu-SAPO-17: A novel catalyst for selective catalytic reduction of NO_x [J]. Chinese Journal of Catalysis, 2020, 41(11): 1715-1722.
[2]	Shujun Ming, Lei Pang, Chi Fan, Wen Guo, Yahao Dong, Peng Liu, Zhen Chen, Tao Li. Chemical deactivation of Cu-SAPO-18 deNO_x catalyst caused by basic inorganic contaminants in diesel exhaust [J]. Chinese Journal of Catalysis, 2019, 40(4): 590-599.
[3]	Chuanmin Chen, Yue Cao, Songtao Liu, Jianmeng Chen, Wenbo Jia. Review on the latest developments in modified vanadium-titanium-based SCR catalysts [J]. Chinese Journal of Catalysis, 2018, 39(8): 1347-1365.
[4]	Jun Yang, Yupeng Chang, Weili Dai, Guangjun Wu, Naijia Guan, Landong Li. Bimetallic Cr-In/H-SSZ-13 for selective catalytic reduction of nitric oxide by methane [J]. Chinese Journal of Catalysis, 2018, 39(5): 1004-1011.
[5]	Zhongyi Sheng, Dingren Ma, Danqing Yu, Xiang Xiao, Bingjie Huang, Liu Yang, Sheng Wang. Synthesis of novel MnO_x@TiO₂ core-shell nanorod catalyst for low-temperature NH₃-selective catalytic reduction of NO_x with enhanced SO₂ tolerance [J]. Chinese Journal of Catalysis, 2018, 39(4): 821-830.
[6]	Yarong Fang, Yanbing Guo. Copper-based non-precious metal heterogeneous catalysts for environmental remediation [J]. Chinese Journal of Catalysis, 2018, 39(4): 566-582.
[7]	Xiaoxia Dai, Weiyu Jiang, Wanglong Wang, Xiaole Weng, Yuan Shang, Yehui Xue, Zhongbiao Wu. Supercritical water syntheses of transition metal-doped CeO₂nano-catalysts for selective catalytic reduction of NO by CO: An in situ diffuse reflectance Fourier transform infrared spectroscopy study [J]. Chinese Journal of Catalysis, 2018, 39(4): 728-735.
[8]	Yexuan Wen, Shuang Cao, Xiaoqi Fei, Haiqiang Wang, Zhongbiao Wu. One-step synthesized SO₄^2--TiO₂ with exposed (001) facets and its application in selective catalytic reduction of NO by NH₃ [J]. Chinese Journal of Catalysis, 2018, 39(4): 771-778.
[9]	Lei Chen, Ding Weng, Jiadao Wang, Duan Weng, Li Cao. Low-temperature activity and mechanism of WO₃-modified CeO₂-TiO₂ catalyst under NH₃-NO/NO₂ SCR conditions [J]. Chinese Journal of Catalysis, 2018, 39(11): 1804-1813.
[10]	Wei Li, Cheng Zhang, Xin Li, Peng Tan, Anli Zhou, Qingyan Fang, Gang Chen. Ho-modified Mn-Ce/TiO₂ for low-temperature SCR of NO_x with NH₃: Evaluation and characterization [J]. Chinese Journal of Catalysis, 2018, 39(10): 1653-1663.
[11]	Wenjin Xu, Guangxu Zhang, Hanwei Chen, Guomeng Zhang, Yang Han, Yichuan Chang, Peng Gong. Mn/beta and Mn/ZSM-5 for the low-temperature selective catalytic reduction of NO with ammonia: Effect of manganese precursors [J]. Chinese Journal of Catalysis, 2018, 39(1): 118-127.
[12]	Tiaoyun Zhou, Qing Yuan, Xiulian Pan, Xinhe Bao. Growth of Cu/SSZ-13 on SiC for selective catalytic reduction of NO with NH₃ [J]. Chinese Journal of Catalysis, 2018, 39(1): 71-78.
[13]	Xiaojiang Yao, Li Chen, Tingting Kong, Shimin Ding, Qiong Luo, Fumo Yang. Support effect of the supported ceria-based catalysts during NH₃-SCR reaction [J]. Chinese Journal of Catalysis, 2017, 38(8): 1423-1430.
[14]	Xiao Xiang, Pengfei Wu, Yi Cao, Lei Cao, Quanyi Wang, Shutao Xu, Peng Tian, Zhongmin Liu. Investigation of low-temperature hydrothermal stability of Cu-SAPO-34 for selective catalytic reduction of NO_x with NH₃ [J]. Chinese Journal of Catalysis, 2017, 38(5): 918-927.
[15]	PiJun Gong, JunLin Xie, De Fang, Da Han, Feng He, FengXiang Li, Kai Qi. Effects of surface physicochemical properties on NH₃-SCR activity of MnO₂ catalysts with different crystal structures [J]. Chinese Journal of Catalysis, 2017, 38(11): 1925-1934.