Poisoning effect of SO2 on Mn-Ce/TiO2 catalysts for NO reduction by NH3 at low temperature

YAN Dong-jie; YU Ya; HUANG Xue-min; LIU Shu-jun; LIU Ying-hui

Feb 2016

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JOURNAL OF MECHANICAL ENGINEERING > 2016 > 44(2): 232-238.

YAN Dong-jie, YU Ya, HUANG Xue-min, LIU Shu-jun, LIU Ying-hui. Poisoning effect of SO2 on Mn-Ce/TiO2 catalysts for NO reduction by NH3 at low temperature[J]. JOURNAL OF MECHANICAL ENGINEERING, 2016, 44(2): 232-238.

Citation:

YAN Dong-jie, YU Ya, HUANG Xue-min, LIU Shu-jun, LIU Ying-hui. Poisoning effect of SO₂ on Mn-Ce/TiO₂ catalysts for NO reduction by NH₃ at low temperature[J]. JOURNAL OF MECHANICAL ENGINEERING, 2016, 44(2): 232-238.

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Poisoning effect of SO₂ on Mn-Ce/TiO₂ catalysts for NO reduction by NH₃ at low temperature

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Corresponding author: YAN Dong-jie, E-mail: yandongjie_2000@163.com
Received Date: 09 Jun 2015
Rev Recd Date: 14 Sep 2015

Abstract

Abstract

Effects of SO₂ on performance of Mn-Ce/TiO₂ catalysts were investigated in the selective catalytic reduction of NO with NH₃.The catalysts were characterized by BET surface area, X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), respectively.The results show that SO₂ has inhibitory effect on the selective catalytic reduction (SCR), and NO_x conversion decreases from 84% to 42% at 140℃.This is mainly because the presence of SO₂ results in the decrease of the specific surface area of the catalysis and the pore size distribution of 5-10 nm.SO₂ can cause TiO₂ transformation from anatase to rutile phase, the crystallization phenomenon of active components MnO_x, and the decrease of the strong interaction between Mn and Ti.The variations of physical and chemical properties of poisoned Mn-Ce/TiO₂ catalyst block the O₂^-→O^-→O^2- conversion path, which reduces the proportion of higher catalytic activity component MnO₂ in MnO_x, weakens oxygen storage ability of CeO_x, and accumulates absorbed oxygen on the catalyst surface decreasing the adsorption and desorption of NO on active sites.Ammonium sulfate formed on the catalyst surface covers the Lewis acid sites and decreases the adsorption amount of NH₃.
- low temperature SCR,
- Mn-Ce/TiO₂ catalyst,
- SO₂,
- poisoning effect

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References(24)

References

[1]	TIAN W, YANG H S, FAN X Y, ZHANG X B.Catalytic reduction of NO_x with NH₃ over different-shaped MnO₂ at low temperature[J].J Hazard Mater, 2011, 188(1/3):105-109. http://www.baidu.com/link?url=80YIJxJbjne19v8geYKMSkwxIu2s6-bjIrO39SBypIsGXFbeiowN3SNAvTPhzHY1sLo34BcAYy75ZyBBysz_WNcgESPamvMgWPTZO_ebVlHF5E9aJAlfvJhElFoQhi91aAjEsUSo3UJpzDimT9HgqMwwZYcDSmoszxIILj7e4ckDv5k4ng-svI26PP9J-S1JgViCFyqcxmwyNaQvqmAzS0XV6_jLBTUfjN-tKy6EYB_NCp97dCOjCD5nbZpcnCc4tM43G0hR8ccl113OZSTEi2m3g73mrmWDbbSfyjZ4CNJLxCSzkGP-WWqFXBHhX8XhqLX1rGNMXf1vtukE1mYZyRSjZBuSBf0FZ6owGiDYKfG&wd=&eqid=df6359fc00045d4d0000000558bfe207
[2]	LIU W, TONG Z Q, LUO J.Low temperature selective catalytic reduction of NO with NH₃ over Ce-Mn/TiO₂ catalyst[J].Acta Sci Circumst, 2006, 26(8):1240-1245. http://www.baidu.com/link?url=jMmLX6xLi2U4qWstlNdqqEHTKuThRx7SvWkAaSlTO_2OpiEnBdZSCTKgahYM4z9KqTpeG_TvQZzlhxx80PeHD3pCWzgBy1VArXO5IRUuu2YYN7Erht14paEAuuCjIqCf__DS4jRwAUvREWZodggTp2ZfuIsaMRIQk5UUT2cgFqcZqvL4qbDTmuHHsLzf4arq6B9F6SzuLAeHwhtMJLLu4gKtJ4FPatnWaLHa-YQ0fq_k4scOmuJlIeQR9yCjx4UBa_nNbHXdke6nDDtoANusMFp8RhnrOT-pvHz87iCRsAxzhX2e9viAncmxCk00Kak6RjodXvBCqXDk0arVslta7njCUJtVIG7Q9fN_IrlImGTzdnlHyZu_VnabiEAK1r2_uWazYbFurLt5_PHSt_jjxMyEyT7k4RHxsgCiK_ncKs6fbNeANIKidHkgbXqPszxvEEOXjqLQU5wHhZRVAgPWxcyHH54pbieo4nmJl-V_HWPv_qlNVOZCSUdI8_aPYzmR5yaX2BWwrTsjlw6DH3i2y71z1cihd-kK7NJr7JpMrurzkpj_DLfn3uro5rdWE6B5tCPTuJyn0s98Les08412P_6jmzBjaCyIdRvUix_kVMk_mt1ozXk8zAl81ICtz1fa&wd=&eqid=db5e8554000416d80000000558bfe214
[3]	BUSCA G, LIETTI L, RAMIS G, BERTI F.Chemical and mechanistic aspects of the selective catalytic reduction of NO_x by ammonia over oxide catalysts[J].Appl Catal B:Environ, 1998, 18(1/2):1-36. http://www.baidu.com/link?url=k441JPF6WV26JNHtp9h_ouEAEpO45Qt6CWAatH0eG5lIa02dmDWIrZYzMWNYiclHAx0guNjqA1oplhYWZxzYPCjZOiNvaBMzOcwI8xWADv2Bvqa6sabwdmGrEoCEIEHBKh639Fdz4coj7aSH8KILZun2TRRx_Blag0ifx_gJwsRFLZv1OIbf0v-FwCVsWnf8Xx32yIhilm7WaV-VSI0cQsqDBA5urt15jFp86UEJXXcaEVLUBzgu98i7D1RfwBZbgohlM4oE8_LnBE4j79xn3nrsGhDPU5zmW3U7zBtdavIDzQowIB0xJf2krdgW4io7UBuoyS8y6Rf1ItCirdiwQLYyMh9IhKcDtZErvLPQpav-mf7adyQNNKsqhA2YncXdnOkzMdU8-p-4HqUsmOtiD_&wd=&eqid=df322c6a0004154a0000000558bfe222
[4]	FORZATTI P.Present ststus and perspective in de-NO_x SCR catalysis[J].Appl Catal A:Gen, 2001, 222(1/2):221-236. http://www.baidu.com/link?url=LFUxFi0vmMQO6rnAOpFMe60qrPFsYRpDA_B-e-tE4wpVLchgzOQtuMYJFR4qeryBP5LzhbkFTEZ5beFSj84-vvZD2nQ2jC3kLR5J1shY56pNG2Ni5nAiq7hJpVjdw9Vs5VtSHoun4nF8sG7KmighxPKtPoosP1uo9dyL_Ib3DhvTPsox8ZdsL5NZQF1jPhP36AjrD2LgIj3ussDQkKC7tVLKziplJrRqZxjeI5emsk5-naG_mHV65iHglMcnvKC3bI42SPWazO-3zfT_z-EMH_LNIOTTMa_7qkbKguMJIaKsBBPBAopc_agJZdUGrwxu&wd=&eqid=dd2cedc20003f1330000000558bfe22e
[5]	CHEN Z H, YANG Q, LI H, LI X H, WANG L F, TSANG C.Cr-MnO_x mixed-oxide catalysts for selective catalytic reduction of NO_x with NH₃ at low temperature[J].J Catal, 2010, 276(1):56-65. doi: 10.1016/j.jcat.2010.08.016
[6]	ZUO J L, CHEN Z H, WANG F R, YU Y H, WANG L F, LI X H.Low-temperature selective catalytic reduction of NO_x with NH₃ over novel Mn-Zr mixed oxide catalysts[J].Ind Eng Chem Res, 2014, 53(7):2647-2655. doi: 10.1021/ie404224y
[7]	CHEN Z H, WANG F R, LI H, YANG Q, WANG L F, LI X H.Low-temperature selective catalytic reduction of NO_x with NH₃ over Fe-Mn mixed-oxide catalysts containing Fe₃Mn₃O₈ phase[J].Ind Eng Chem Res, 2012, 51(1):202-212. doi: 10.1021/ie201894c
[8]	LIU Z M, ZHU J Z, LI J H, MA L L, WOO S L.Novel Mn-Ce-Ti mixed-oxide catalyst for the selective catalytic reduction of NO_x with NH₃[J].ACS Appl Mater Inter, 2014, 6(16):14500-14508. doi: 10.1021/am5038164
[9]	GU T T, JIN R B, LIU Y, LIU H F, WENG X L, WU Z B.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(3):30-38.
[10]	WU Z B, JIN R B, WANG H Q, LIU Y.Effect of ceria doping on SO₂ resistance of Mn/TiO₂ for selective catalytic reduction of NO with NH₃ at low temperature[J].Catal Commun, 2009, 10(6):935-939. doi: 10.1016/j.catcom.2008.12.032
[11]	JIN R B, LIU Y, WANG Y, CEN W L, WU Z B, WANG H Q, WENG X L.The role of cerium in the improved SO₂ tolerance for NO reduction with NH₃ over Mn-Ce/TiO₂ catalyst at low temperature[J].Appl Catal B:Environ, 2014, 148/149(4):582-588. http://www.baidu.com/link?url=fj92pPb2jgSsUjmya46VVgcdKzdE8ulOz4m6MdwOp4tiwB380a5r41FtQLfvNAtCtD8OqFP5UWCb4M0F8G1Zj0j2P6_5nTej0hsd-pKjinwv40SfMiY3zDVRraBZ2oXtjcfv-7IgUp9OyrHXCMpvDFRw9BSI638jT0XfAKWeMu3SXweQhEm8nwkt0gaFpRyqPngUW2sVchn_Wq03K--K_MIeZ8lTbGjI3-nSgkJjhyUkZuZKmkxOJmnMf_zxCuma57_U1YciEArsYHaexVQDsfSfITJvJBBReVp8yY4seL9E27m-3e_ELc8PPzdL17NaibrTbBz5YW7njm6TxuyVHn4CPj2JZpFK6-XrOzeaCfvaVUWhc25Ru-HJBe3sd6R-Huxkrz5tfi8T-tyEdptmWq&wd=&eqid=df322c6a000418d40000000558bfe248
[12]	SING K S W, EVEWETT D H, HAUL R A W, MOSCOU L, PIEROTTO R A, ROUQUÉROL J, SIEMIENIEWSKA T.Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity[J].Pure Appl Chem, 1985, 57(4):603-619.
[13]	TANG X L, HAO J M, YI H H.Low-temperature SCR of NO with NH₃ over AC/C supported manganese-catalysts[J].Catal Today, 2007, 126(3/4):406-411.
[14]	ZHANG X, JI L Y, ZHANG S C, YANG W S.Synthesis of a novel polyaniline-intercalated layered manganese oxide nanocomposite as electrode material for electrochemical capacitor[J].J Power Sources, 2007, 173(2):1017-1023. doi: 10.1016/j.jpowsour.2007.08.083
[15]	KAPTEIJN F, SINGOREDJO L, ANDREINI A, MOULIJN J A.Activity and selectivity of pure manganese oxides in the selective catalytic reduction of nitric oxide with ammonia[J].Appl Catal B:Environ, 1994, 3(2/3):173-189.
[16]	PAPARAZZO E.Some notes on XPS Mn 2p and Ce 3d spectra of MnO_x-ceria catalysts[J].Catal Today, 2012, 185(1):319-321. doi: 10.1016/j.cattod.2012.02.014
[17]	GUO Y F, LIAO X B, HE J H, QU W J, YE D Q.Effect of manganese oxide catalyst on the dielectric barrier discharge decomposition of toluene[J].Catal Today, 2010, 153(3/4):176-183.
[18]	YE Q, ZHAO J S, HUO F F, WANG J, CHENG S Y, KANG T F, DAI H X.Nanosized Ag/α-MnO₂ catalysts highly active for the low-temperature oxidation of carbon monoxide and benzene[J].Catal Today, 2011, 175(1):603-609. doi: 10.1016/j.cattod.2011.04.008
[19]	JARRIGE J, VERVISCH P.Plasma-enhanced catalysis of propane and isopropyl alcohol at ambient temperature on a MnO₂-based catalyst[J].Appl Catal B:Environ, 2009, 90(1):74-82.
[20]	陈建军.锰基催化剂研制及其低温选择催化还原NO_x机理研究[D].北京:清华大学, 2007. CHEN Jian-jun.Study on Mn-based catalysts and mechanism for selective catalytic reduction of NO_x at low-temperature[D].Beijing:Tsinghua University, 2007.
[21]	REDDY B M, SREEKANTH P M, YAMADA Y, XU Q, KOBAYASHI T.Surface characterization of sulfate, molybdate, and tungstate promoted TiO₂-ZrO₂ solid acid catalysts by XPS and other techniques[J].Appl Catal A:Gen, 2002, 228(1/2):269-278.
[22]	陈博吴, 马运生, 丁良兵, 许令顺, 邬宗芸, 袁青, 黄伟新.NO在Cu (111) 表面吸附和分解的XPS和TPD研究:不同氧物种的影响[J].催化学报, 2013, 34(5):964-972. doi: 10.1016/S1872-2067(12)60585-3 CHEN Bo-wu, MA Yun-sheng, DING Liang-bing, XU Ling-shun, WU Zong-yun, YUAN Qing, HUANG Wei-xin.XPS and TPD study of NO interaction with Cu (111):Role of different oxygen species[J].Chin J Catal, 2013, 34(5):964-972. doi: 10.1016/S1872-2067(12)60585-3
[23]	ROMANO E J, SCHULZ K H.A XPS investigation of SO₂ adsorption on ceria-zirconia mixed-metal oxides[J].Appl Surf Sci, 2005, 246(1/3):262-270.
[24]	TAUSTER S J, FUNG S C, BAKER R T, HORSLEY J A.Strong interactions in supported-metal catalysts[J].Science, 1981, 211(4487):1121-1125. doi: 10.1126/science.211.4487.1121

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Poisoning effect of SO₂ on Mn-Ce/TiO₂ catalysts for NO reduction by NH₃ at low temperature

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Poisoning effect of SO₂ on Mn-Ce/TiO₂ catalysts for NO reduction by NH₃ at low temperature