Effect of sulfate species on the performance of Ce-Fe-Ox catalysts in the selective catalytic reduction of NO by NH3

ZHANG Xue-jun; ZHANG Ting-ji; SONG Zhong-xian; LIU Wei; XING Yun

doi:10.1016/S1872-5813(21)60021-X

Volume 49 Issue 6

Jun. 2021

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ZHANG Xue-jun, ZHANG Ting-ji, SONG Zhong-xian, LIU Wei, XING Yun. Effect of sulfate species on the performance of Ce-Fe-Ox catalysts in the selective catalytic reduction of NO by NH3[J]. Journal of Fuel Chemistry and Technology, 2021, 49(6): 844-852. doi: 10.1016/S1872-5813(21)60021-X

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ZHANG Xue-jun, ZHANG Ting-ji, SONG Zhong-xian, LIU Wei, XING Yun. Effect of sulfate species on the performance of Ce-Fe-O_x catalysts in the selective catalytic reduction of NO by NH₃[J]. Journal of Fuel Chemistry and Technology, 2021, 49(6): 844-852. doi: 10.1016/S1872-5813(21)60021-X

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Effect of sulfate species on the performance of Ce-Fe-O_x catalysts in the selective catalytic reduction of NO by NH₃

doi: 10.1016/S1872-5813(21)60021-X

1.
College of Environmental and Safety Engineering, Shenyang University of Chemical Technology, Shenyang 110142, China
2.
Faculty of Environmental and Municipal Engineering, Henan Key Laboratory of Water Pollution Control and Rehabilitation Technology, Henan University of Urban Construction, Pingdingshan 467036, China

Funds: The project was supported by the National Natural Science Foundation of China (21872096), the Educational Department of Liaoning Province (LZ2019002), Natural Science Youth Fund of Henan Province (202300410034), Key Scientific and Technological Project of Henan Province (202102310341), Young Teacher Foundation of Henan University of Urban Construction (YCJQNGGJS201903), Henan Key Scientific Research Projects (20A610003), Innovative Training Program for College Students in Henan Province (202011765035), Doctoral Research Start-up Project of Henan University of Urban Construction (990/Q2017011).

Received Date: 2020-10-27
Rev Recd Date: 2020-12-28

Available Online: 2021-03-30

Publish Date: 2021-06-30

Abstract

Abstract

A series of Ce-Fe-O_x catalysts containing sulfate species was prepared by four different methods including sol-gel (Fe-SG), hydrothermal (Fe-HT), co-precipitation (Fe-10) and solid state grinding synthesis (Fe-SSGS) methods. The Ce-Fe-O_x catalysts were used in the selective catalytic reduction (SCR) of NO_x by NH₃ and the effect of sulfate species on the catalytic performance was investigated. The results indicate that the Fe-HT catalyst prepared by the hydrothermal method exhibits excellent performance in the NH₃-SCR of NO, with a NO conversion of nearly 100% even at 250 °C. The Fe-HT catalyst contains proper amount of sulfate, which can decrease the CeO₂ crystallinity and enhance the catalytic performance in the NH₃-SCR of NO. The Fe-HT catalyst has a high content of surface Ce³⁺ and Fe³⁺ and there is a synergy between the Fe and Ce species, which can improve the redox capacity and greatly increase the quantity of chemisorbed oxygen. In contrast, excessive amount of sulfate species in Fe-SSGS and Fe-SG may reduce the synergy between Fe and Ce and then impair the catalytic performance of Ce-Fe-O_x in NH₃-SCR.
- selective catalytic reduction,
- sulfates,
- surface acidity,
- chemisorption oxygen

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References(53)

References

[1]	SCHNEIDER H, SCHARF U, WOKAUN A, BAIKER A. Chromia on titania: IV. Nature of active sites for selective catalytic reduction of NO by NH₃[J]. J Catal,1994,146(2):545−556. doi: 10.1006/jcat.1994.1093
[2]	BRANDENBERGER S, KRÖCHER O, TISSLER A, ALTHOFF R. The state of the art in selective catalytic reduction of NO_x by Ammonia using metal-exchanged zeolite catalysts[J]. Catal Rev Sci Eng,2008,50(4):492−531. doi: 10.1080/01614940802480122
[3]	GU T, JIN R, LIU Y, WENG X, WU Z. Promoting effect of calcium doping on the performances of MnO_x/TiO₂ catalysts for NO reduction with NH₃ at low temperature[J]. Appl Catal B: Environ,2013,129:30−38. doi: 10.1016/j.apcatb.2012.09.003
[4]	LI J, CHEN J, KE R, LUO C, HAO J. Effects of precursors on the surface Mn species and the activities for NO reduction over MnO_x/TiO₂ catalysts[J]. Catal Commun,2007,8(12):1896−1900. doi: 10.1016/j.catcom.2007.03.007
[5]	GAO X, JIANG Y, FU Y, ZHONG Y, LUO Z, CEN K. Preparation and characterization of CeO₂/TiO₂ catalysts for selective catalytic reduction of NO with NH₃[J]. Catal Commun,2010,11(5):465−469. doi: 10.1016/j.catcom.2009.11.024
[6]	SONG Z, ZHANG Q, NING P, FAN J, DUAN Y, LIU X, HUANG Z. Effect of CeO₂ support on the selective catalytic reduction of NO with NH₃ over PW/CeO₂[J]. J Taiwan Inst Chem Eng,2016,65:149−161. doi: 10.1016/j.jtice.2016.04.034
[7]	SONG Z, NING P, ZHANG Q, LIU X, ZHANG J, WANG Y, DUAN Y, HUANG Z. The role of surface properties of silicotungstic acid doped CeO₂ for selective catalytic reduction of NO_x by NH₃: Effect of precipitant[J]. J Mol Catal A: Chem,2016,413:15−23. doi: 10.1016/j.molcata.2015.12.009
[8]	SONG Z, YIN L, ZHANG Q, NING P, DUAN Y, WANG J, LIU X, LONG K, HUANG Z. Relationship between the WO₃ states and reaction pathway over CeO₂-ZrO₂-WO₃ catalysts for selective catalytic reduction of NO with NH₃[J]. Mol Catal,2017,437:95−104. doi: 10.1016/j.mcat.2017.04.033
[9]	TOPSØE N Y. Mechanism of the selective catalytic reduction of nitric oxide by ammonia elucidated by in situ on-line Fourier transform infrared spectroscopy[J]. Science,1994,265(5176):1217−1219. doi: 10.1126/science.265.5176.1217
[10]	SUN Y, GUO Y, SU W, WEI Y. Low-temperature selective catalytic reduction of NO with NH₃ over Fe-Ce-O_x catalysts[J]. Trans Tianjin Univ,2017,23(1):35−42. doi: 10.1007/s12209-016-0017-y
[11]	HU W, GAO X, DENG Y, QU R, ZHENG C, ZHU X, CEN K. Deactivation mechanism of arsenic and resistance effect of SO₄²⁻ on commercial catalysts for selective catalytic reduction of NO_x with NH₃[J]. Chem Eng J,2016,293:118−128. doi: 10.1016/j.cej.2016.02.095
[12]	YAO X, WANG Z, YU S, YANG F, DONG L. Acid pretreatment effect on the physicochemical property and catalytic performance of CeO₂ for NH₃-SCR[J]. Appl Catal A: Gen,2017,542:282−288. doi: 10.1016/j.apcata.2017.06.003
[13]	AZAMBRE B, ZENBOURY L, WEBER J V, BURG P. Surface characterization of acidic ceria–zirconia prepared by direct sulfation[J]. Appl Surf Sci,2010,256(14):4570−4581. doi: 10.1016/j.apsusc.2010.02.049
[14]	LIU Z, XING L, MA H, CHENG L, LIU J, YANG J, ZHANG Q. Sulfated Ce-doped TiO₂ as visible light driven photocatalyst: Preparation, characterization and promotion effects of Ce doping and sulfation on catalyst performance[J]. Environ Prog Sustain Energy,2017,36(2):494−504. doi: 10.1002/ep.12511
[15]	张秋林, 张金辉, 宁平, 宋忠贤, 王燕彩, 徐利斯, 唐小苏. SO₄^2-改性对Ce、Ti基催化剂NH₃-SCR脱硝性能的影响[J]. 昆明理工大学学报(自然科学版),2014,(6):110−115. ZHANG Qiu-lin, ZHANG Jin-hui, NING Ping, SONG Zhong-xian, WANG Yan-cai, XU Li-si, TANG Xiao-su. Enhanced effect of SO₄²⁻ on Ce and Ti-based catalysts for selective catalytic reduction of NO_x with NH₃[J]. J Kunming Univ Sci Technol (Nat Sci),2014,(6):110−115.
[16]	ZHANG X, WANG J, SONG Z, ZHAO H, XING Y, ZHAO M, ZHAO J, MA Z, ZHANG P, TSUBAKI, N. Promotion of surface acidity and surface species of doped Fe and SO₄²⁻ over CeO₂ catalytic for NH₃-SCR reaction[J]. Mol Catal,2019,463:1−7. doi: 10.1016/j.mcat.2018.11.002
[17]	边雪, 肖坤宇, 王书豪, 邱保龙. Fe、Ce改性锰钛催化剂的制备及其低温脱硝性能研究[J]. 功能材料,2019,50(7):07090−07095. doi: 10.3969/j.issn.1001-9731.2019.07.016 BIAN Xue, XIAO Kun-yu, WANG Shu-hao, QIU Bao-long. Preparation and the study on low-temperature denitrification of Fe, Ce modified manganese titanium catalyst[J]. J Funct Mater,2019,50(7):07090−07095. doi: 10.3969/j.issn.1001-9731.2019.07.016
[18]	LIU J, LI X, ZHAO Q, KE J, XIAO H, LV X, LIU S, TADÉ M, WANG, S. Mechanistic investigation of the enhanced NH₃-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FT-IR analysis for structure-activity correlation[J]. Appl Catal B: Environ,2017,200:297−308. doi: 10.1016/j.apcatb.2016.07.020
[19]	QU R, GAO X, CEN K, LI J. Relationship between structure and performance of a novel cerium-niobium binary oxide catalyst for selective catalytic reduction of NO with NH₃[J]. Appl Catal B: Environ,2013,142:290−297.
[20]	TAKITA Y, MORIYAMA J, NISHIGUCHI H, ISHIHARA T, HAYANO F, NAKAJO T. Decomposition of CCl₂F₂ over metal sulfate catalysts[J]. Catal Today,2004,88(3/4):103−109. doi: 10.1016/j.cattod.2003.11.003
[21]	YAO X, CHEN L, CAO J, YANG F, TAN W, DONG L. Morphology and crystal-plane effects of CeO₂ on TiO₂/CeO₂ catalysts during NH₃-SCR reaction[J]. Ind Eng Chem Res,2018,57(37):12407−12419. doi: 10.1021/acs.iecr.8b02830
[22]	PETROV K I, IVANOV V I, PERVYKH V G. Vibrational spectra of lanthanum, cerium, praseodymium, and neodymium sulfate pentahydrates[J]. J Struct Chem,1967,8(2):310−312. doi: 10.1007/BF00745659
[23]	GAO S, WANG P, CHEN X, WANG H, WU Z, LIU Y, WENG X. Enhanced alkali resistance of CeO₂/SO₄²⁻–ZrO₂ catalyst in selective catalytic reduction of NO_x by ammonia[J]. Catal Commun,2014,43:223−226. doi: 10.1016/j.catcom.2013.10.017
[24]	YU Y, CHEN C, MA M, DOUTHWAITE M, HE C, MIAO J, CHEN J, LI C. SO₂ promoted in situ recovery of thermally deactivated Fe₂(SO₄)₃/TiO₂ NH₃-SCR catalysts: from experimental work to theoretical study[J]. Chem Eng J,2019,361:820−829. doi: 10.1016/j.cej.2018.12.149
[25]	LI Y, SONG W, LIU J, ZHAO Z, GAO M, WEI Y, WANG Q, DENG J. The protection of CeO₂ thin film on Cu-SAPO-18 catalyst for highly stable catalytic NH₃-SCR performance[J]. Chem Eng J,2017,330:926−935. doi: 10.1016/j.cej.2017.08.025
[26]	MEUNIER F C, ROSS J R H. Effect of ex situ treatments with SO₂ on the activity of a low loading silver–alumina catalyst for the selective reduction of NO and NO₂ by propene[J]. Appl Catal B: Environ,2000,24(1):23−32. doi: 10.1016/S0926-3373(99)00088-0
[27]	SCHILL L, PUTLURU S S R, FEHRMANN R, JENSEN A D. Low-temperature NH₃-SCR of NO on mesoporous Mn_0.6Fe_0.4/TiO₂ prepared by a hydrothermal method[J]. Catal Lett,2014,144(3):395−402. doi: 10.1007/s10562-013-1176-2
[28]	WANG D, PENG Y, XIONG S C, LI B, GAN L N, LU C M, CHEN J J, MA Y L, LI J H. De-reducibility mechanism of titanium on maghemite catalysts for the SCR reaction: an in situ DRIFTS and quantitative kinetics study[J]. Appl Catal B: Environ,2018,221:556−564. doi: 10.1016/j.apcatb.2017.09.045
[29]	FEYZI M, IRANDOUST M, MIRZAEI A A. Effects of promoters and calcination conditions on the catalytic performance of iron-manganese catalysts for fischer-tropsch synthesis[J]. Fuel Process Technol,2011,92(5):1136−1143. doi: 10.1016/j.fuproc.2011.01.010
[30]	ABDELSAYED V, SHEKHAWAT D, SMITH M W. Effect of Fe and Zn promoters on Mo/HZSM-5 catalyst for methane dehydroaromatization[J]. Fuel,2015,139:401−410. doi: 10.1016/j.fuel.2014.08.064
[31]	LIU X L, GUO J X, CHU Y H, LUO D M, YIN H Q, SUN M C, YAVUZ R. Desulfurization performance of iron supported on activated carbon[J]. Fuel,2014,123:93−100. doi: 10.1016/j.fuel.2014.01.068
[32]	SOH B W, NAM I S. Effect of support morphology on the sulfur tolerance of V₂O₅/Al₂O₃ catalyst for the reduction of NO by NH₃[J]. Ind Eng Chem Res,2003,42(13):2975−2986. doi: 10.1021/ie020861b
[33]	KIJLSTRA W S, BIERVLIET M, POELS E K, BLIEK A. Deactivation by SO₂ of MnO_x/Al₂O₃ catalysts used for the selective catalytic reduction of NO with NH₃ at low temperatures[J]. Appl Catal B: Environ,1998,16(4):327−337. doi: 10.1016/S0926-3373(97)00089-1
[34]	LEE K J, KUMAR P A, MAQBOOL M S, RAO K N, SONG K H, HA H P. Ceria added Sb-V₂O₅/TiO₂ catalysts for low temperature NH₃-SCR: Physico-chemical properties and catalytic activity[J]. Appl Catal B: Environ,2013,142/143(10):705−717.
[35]	CHANG H, LI J, YUAN J, CHEN L, DAI Y, ARANDIYAN H, XU J, HAO J. Ge, Mn-doped CeO₂-WO₃ catalysts for NH₃-SCR of NO_x: effects of SO₂ and H₂ regeneration[J]. Catal Today,2013,201(1):139−144.
[36]	SHEN Y, MA Y, ZHU S. Promotional effect of zirconium additives on Ti_0.8Ce_0.2O₂ for selective catalytic reduction of NO[J]. Catal Sci Technol,2012,2(3):589−599. doi: 10.1039/C2CY00363E
[37]	SULTANA A, SASAKI M, HAMADA H. Influence of support on the activity of Mn supported catalysts for SCR of NO with ammonia[J]. Catal Today,2012,185(1):284−289. doi: 10.1016/j.cattod.2011.09.018
[38]	DAMYANOVA S, PEREZ C A, SCHMAL M, BUENO J M C. Characterization of ceria-coated alumina carrier[J]. Appl Catal A: Gen,2002,234(1/2):271−282. doi: 10.1016/S0926-860X(02)00233-8
[39]	MURUGAN B, RAMASWAMY A V. Chemical states and redox properties of Mn/CeO₂−TiO₂ nanocomposites prepared by solution combustion route[J]. J Phys Chem C,2008,112(51):20429−20442. doi: 10.1021/jp806316x
[40]	OTSUKA K, WANG Y, NAKAMURA M. Direct conversion of methane to synthesis gas through gas-solid reaction using CeO₂-ZrO₂ solid solution at moderate temperature[J]. Appl Catal A: Gen,1999,183(2):317−324. doi: 10.1016/S0926-860X(99)00070-8
[41]	LI Y, SUN Q, KONG M, SHI W, HUANG J, TANG J, ZHAO X. Coupling oxygen ion conduction to photocatalysis in mesoporous nanorod-like ceria significantly improves photocatalytic efficiency[J]. J Phys Chem C,2011,115(29):14050−14057. doi: 10.1021/jp202720g
[42]	ZHANG Z, CHEN L, LI Z, LI P, YUAN F, NIU X, ZHU Y. Activity and SO₂ resistance of amorphous Ce_aTiO_x catalysts for the selective catalytic reduction of NO with NH₃: in situ DRIFT studies[J]. Catal Sci Technol,2016,6(19):7151−7162. doi: 10.1039/C6CY00475J
[43]	LIU X, ZHOU K, WANG L, WANG B, LI Y. Oxygen vacancy clusters promoting reducibility and activity of ceria nanorods[J]. J Am Chem Soc,2009,131(9):3140−3141. doi: 10.1021/ja808433d
[44]	CHANG H, CHEN X, LI J, MA L, WANG C, LIU C, SCHWANK J W, HAO J. Improvement of activity and SO₂ tolerance of Sn-modified MnO_x-CeO₂ catalysts for NH₃-SCR at low temperatures[J]. Environ Sci Technol,2013,47(10):5294−5301. doi: 10.1021/es304732h
[45]	GUO M, LIU Q, ZHAO P, HAN J, LI X, HA Y, FU Z, SONG C, JI N, LIU C, MA D, LI Z. Promotional effect of SO₂ on Cr₂O₃ catalysts for the marine NH₃-SCR reaction[J]. Chem Eng J,2019,361:830−838. doi: 10.1016/j.cej.2018.12.100
[46]	GUO R T, LU C Z, PAN W G, ZHEN W L, WANG Q S, CHEN Q L, DING H L, YANG N Z. A comparative study of the poisoning effect of Zn and Pb on Ce/TiO₂ catalyst for low temperature selective catalytic reduction of NO with NH₃[J]. Catal Commun,2015,59:136−139. doi: 10.1016/j.catcom.2014.10.006
[47]	DU X, ZHANG D, SHI L, GAO R, ZHANG J. Morphology dependence of catalytic properties of Ni/CeO₂ nanostructures for carbon dioxide reforming of methane[J]. J Phys Chem C,2012,116(18):10009−10016. doi: 10.1021/jp300543r
[48]	KRISHNA K, BUENO-LÓPEZ A, MAKKEE M, MOULIJN J A. Potential rare-earth modified CeO₂ catalysts for soot oxidation part Ⅱ: Characterisation and catalytic activity with NO + O₂[J]. Appl Catal B: Environ,2007,75(3/4):201−209. doi: 10.1016/j.apcatb.2007.04.007
[49]	HU W, ZHANG Y, LIU S, ZHENG C, GAO X, NOVA I, TRONCONI E. Improvement in activity and alkali resistance of a novel V-Ce(SO₄)₂/Ti catalyst for selective catalytic reduction of NO with NH₃[J]. Appl Catal B: Environ,2017,206:449−460. doi: 10.1016/j.apcatb.2017.01.036
[50]	DELAHAY G, VALADE D, GUZMAN-VARGAS A, COQ B. Selective catalytic reduction of nitric oxide with ammonia on Fe-ZSM-5 catalysts prepared by different methods[J]. Appl Catal B: Environ,2005,55(2):149−155. doi: 10.1016/j.apcatb.2004.07.009
[51]	GENG Y, CHEN X, YANG S, LIU F, SHAN W. Promotional Effects of Ti on a CeO₂-MoO₃ Catalyst for the Selective Catalytic Reduction of NO_x with NH₃[J]. ACS Appl Mater Interfaces,2017,9(20):16951−16958. doi: 10.1021/acsami.6b05380
[52]	ZHANG Q, ZHANG J, SONG Z, NING P, LI H, LIU X. A novel and environmentally friendly SO₄²⁻/CeO₂ catalyst for the selective catalytic reduction of NO with NH₃[J]. J Ind Eng Chem,2016,34:165−171. doi: 10.1016/j.jiec.2015.11.006
[53]	中本一雄, 黄德如. 无机和配位化合物的红外和拉曼光谱[M]. 北京: 化学工业出版社, 1986. NAKAMOTO K, HUANG De-ru. Infrared and Raman Spectra of Inorganic Coordination Compound[M]. Beijing: Chemical Indusry Press, 1986.