INORGANIC MATERIALS AND CERAMIC MATRIX COMPOSITES |
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Study on NH3-SCR Performance over Cu-SSZ-13 and Fe-β Mixed Catalysts |
LI Yuan, HOU Yukun, ZHAO Liguo, TAN Xiaoyao
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School of Chemical Engineering and Technology Tiangong University, Tianjin 300387, China |
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Abstract Copper modified SSZ-13 molecular sieve (Cu-SSZ-13) is an efficient NH3 selective reduction catalyst for NOx removal, but the NOx removal activity of Cu-SSZ-13 at high temperature (>400 ℃) is poor. Compared with Cu-SSZ-13, Fe modified β molecular sieve catalyst (Fe-β) is cheaper and has better denitration performance at high temperature, so Fe-β has attracted much attention. The low temperature activity of Fe-β catalyst is improved after Cu doping, but cryogenic active temperature window and the maximum removal rate of SCR denitration catalyst still need to be improved. In this work, the composite catalyst was prepared by mechanical mixing of Cu-SSZ-13 and Fe-β to expand the temperature window of the catalyst. Cu-SSZ-13 was prepared by ion exchange of different concentrations of Cu(NO3)2 solution with commercial SSZ-13. The NH3-SCR test results show that Cu-SSZ-13 prepared by exchange of Cu(NO3)2 solution with the concentration of 0.04 mol/L has the best denitration activity, and the NOx removal rate is close to 100% at 200—400 ℃. The catalysts were characterized by powder X-ray diffraction (XRD), electron scanning microscope (SEM) and a series of other means. Reaction performance test results show that mechanical mixing of Cu-SSZ-13+Fe-β does not affect the low temperature activity window of NH3-SCR of Cu-SSZ-13, but the high temperature performance of catalyst is improved after mechanical mixing.
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Published: 10 October 2022
Online: 2022-10-12
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Fund:National Natural Science Foundation of China (91745116) |
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1 Shan W P, Liu F D, He H. Chinese Science Bulletin, 2014, 59, 2540. 2 Peng Z L. Optimization of in situ synthesis conditions of Cu-SSZ-13 denitration catalyst. Master's Thesis, Taiyuan University of Technology, China, 2015(in Chinese). 彭兆亮. Cu-SSZ-13脱硝催化剂原位合成条件的优化.硕士学位论文, 太原理工大学,2015. 3 Kaspar J, Fornasiero P, Hickey N. Catalysis Today, 2003, 77(4), 419. 4 Zhang Y, Wang H N, Chen R Y. RSC Advances, 2015, 5(83), 67841. 5 Guo K, Zhu Y X, Yan Z, et al. Chemical Engineering Journal, 2020, 389, 124271. 6 Liang J, Ma Y, Song G, et al. Journal of Hazardous Materials, 2020, 398, 122986. 7 Granger P, Parvulescu V I. Chemical Reviews, 2011, 111(5), 3155. 8 Liu F D, Yu Y B, He H. Chemical Communications, 2014, 50, 8445. 9 Han J, Guan B, Peng X S, et al. Chemical Engineering Journal, 2019, 379, 122358. 10 Liu L P, Wu X D, Ma Y, et al. Chemical Engineering Journal, 2019, 383, 123080. 11 Zones S I. Journal of the Chemical Society Faraday Transactions, 1991, 87(22), 3709. 12 Gonzale Martinez J, Villa A. Catalysis Letters, 2021, 151(10), 1. 13 Lomachenko K A, Borfecchia E, Negri C, et al. Journal of the American Chemical Society, 2016, 138(37), 12025. 14 Xi Y, Su C, Ottinger N A, et al. Applied Catalysis B: Environmental, 2021, 284, 119749. 15 Liang J, Tao J X, Mi Y Y, et al. Chemical Engineering Journal, 2021, 409 (13), 128238. 16 Zhao R. One-step synthesis of Fe-Cu-SZ-13 catalyst and its catalytic performance of NH3-SCR. Master's Thesis, Zhejiang University, China, 2017(in Chinese). 赵茹. Fe-Cu-SSZ-13催化剂一步法合成及其NH3-SCR催化性能的研究. 硕士学位论文, 浙江大学, 2017. 17 Wen C. Isomorphic substitution of SSZ-13 zeolite based on density functional theory. Master's Thesis, Taiyuan University of Technology, China, 2016(in Chinese). 文翠. 基于密度泛函理论对SSZ-13分子筛同晶取代的研究. 硕士学位论文, 太原理工大学, 2016. 18 Xu L, Shi C, Chen B B, et al. Microporous and Mesoporous Materials, 2016, 236(1), 211. 19 Xiao F S, Zhang L, Wu Q M, et al. Reaction Chemistry & Engineering, 2019, 4(6), 975. 20 Wang A Y, Wang Y L, Walter E D, et al. Catalysis Today, 2017, 320, 91. 21 Wang X H. Preparation, modification and denitrification performance of SSZ-13 molecular sieve catalyst. Master's Thesis, Beijing University of Chemical Technology, China, 2020(in Chinese). 王晓花. SSZ-13分子筛催化剂的制备,改性及脱硝性能的研究. 硕士学位论文, 北京化工大学, 2020. 22 Xie L J, Liu F D, Ren L M, et al. Environmental Science & Technology, 2014, 48(1),566. 23 Xie L J, Liu F D, Shi X Y, et al. Applied Catalysis B: Environmental, 2015, 179,206. 24 Chen Z X, Wang J, Wang J M, et al. Industrial & Engineering Chemistry Research, 2019,58(45), 20610. 25 Song J, Wang Y L, Walter E D, et al. ACS Catalysis, 2017, 7, 8214. 26 Gao F, Walter E D, Kollar M, et al. Journal of Catalysis, 2014, 319, 1. 27 Zhang D, Yang R T. Energy & Fuels, 2018, 32(2), 2170. 28 Zhang T, Qiu F, Chang H Z, et al. Catalysis Science & Technology, 2016, 6(16), 6294. 29 Gao F, Walter E D, Washton N M, et al. Applied Catalysis B Environmental, 2015, 162, 501. 30 Ma Y H, Zhao H W, Zhang C J, et al. Catalysis Today, 2019, 355, 627. 31 Zhang R R. Selective catalytic reduction of NO by NH3 over modified Cu-SSZ-13 zeolite. Master's Thesis, Tianjin University, China, 2015 (in Chinese). 张冉冉. 改性Cu-SSZ-13分子筛上NH3选择性催化还原NO的性能研究. 硕士学位论文, 天津大学, 2015. 32 Gao F, Walter E D, Karp E M, et al. Journal of Catalysis, 2013, 300, 20. 33 Beale A M, Lezcano-Gonzalez I, Slawinksi W A, et al. Chemical Communications, 2016, 52(36), 6170. 34 Wang J Q. Study on the performance and mechanism of selective catalytic reduction of NO by NH3 over Ce-modified Cu-SSZ-13 zeolite. Master's Thesis, Taiyuan University of Technology, China, 2018(in Chinese). 王俊强. Ce改性Cu-SSZ-13分子筛上NH3选择性催化还原NO的性能与机理研究. 硕士学位论文, 太原理工大学, 2018. 35 Han S, Ye Q, Cheng S Y, et al. Catalysis Science & Technology, 2017, 7, 703. 36 Chen B H, Xu R N, Zhang R D, et al. Evironmental Science & Technology, 2014, 48(23), 13909. 37 Niu C, Shi X Y, Liu F D, et al. Chemical Engineering Journal, 2016, 294, 254. 38 Kwak J H, Zhu H Y, Lee J H, et al. Chemical Communications, 2012, 48(39), 4758. 39 Ma L, Cheng Y S, Cavataio G, et al. Chemical Engineering Journal, 2013, 225(3), 323. 40 Cao Y, Zou S, Lan L, et al. Journal of Molecular Catalysis A Chemical, 2015, 398, 304. 41 Han M J, Jiao Y L, Zhou C H, et al. Rare Metals, 2019, 38(3), 210. 42 Fan C, Chen Z, Pang L, et al. Applied Catalysis A: General, 2018, 550, 256. 43 Zhao F, Li Y, Zhang Y, et al. Fine Chemicals, 2017, 34(2), 179. 赵飞, 李渊, 张岩, 等. 精细化工, 2017, 34(2), 179. 44 Stacey I Z. U.S. patent, US4544538, 1985. 45 Liang J, Mi Y Y, Song G, et al. Journal of Hazardous Materials, 2020, 398, 122986. 46 Wang D, Jangjou Y, Liu Y, et al. Applied Catalysis B Environmental, 2015, 165,438. |
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