Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NOx with NH3

MENG Peng-tong; FAN Chao; LÜ Wen-ting; WU Zhi-wei; JIAO Wei-yong; LI Jun-fen; QIN Zhang-feng; FAN Wei-bin; WANG Jian-guo

Volume 48 Issue 10

Oct. 2020

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2020 > 48(10): 1216-1223

MENG Peng-tong, FAN Chao, LÜ Wen-ting, WU Zhi-wei, JIAO Wei-yong, LI Jun-fen, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NOx with NH3[J]. Journal of Fuel Chemistry and Technology, 2020, 48(10): 1216-1223.

Citation:

MENG Peng-tong, FAN Chao, LÜ Wen-ting, WU Zhi-wei, JIAO Wei-yong, LI Jun-fen, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃[J]. Journal of Fuel Chemistry and Technology, 2020, 48(10): 1216-1223.

Citation:

MENG Peng-tong, FAN Chao, LÜ Wen-ting, WU Zhi-wei, JIAO Wei-yong, LI Jun-fen, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃[J]. Journal of Fuel Chemistry and Technology, 2020, 48(10): 1216-1223.

PDF( 5010 KB)

Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Funds:

The Strategic Program of Coal-based Technology of Shanxi Province of China MQ2014-11

The Strategic Program of Coal-based Technology of Shanxi Province of China MQ2014-10

The Strategic Priority Research Program of the Chinese Academy of Sciences XDA21020500

More Information

Corresponding author: LI Jun-fen, E-mail:lijunfen@sxicc.ac.cn; LI Jun-fen, E-mail:lijunfen@sxicc.ac.cn
Received Date: 2020-07-09
Rev Recd Date: 2020-08-08

Available Online: 2021-01-23

Publish Date: 2020-10-10

Abstract

Abstract

A series of monolithic cordierite supported Cu-SSZ-13 catalysts (Cu-SSZ-13/Cordierite) was prepared by coating the Cu-SSZ-13 molecular sieves on the cellular cordierite through ultrasonic dispersion with polyvinyl alcohol (PVA) or pseudo boehmite powder (SB) as assisting agent and used in the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR). With the help of XRD, nitrogen sorption, SEM and H₂-TPR characterization techniques, the influence of coating assistant agent on the firmness of the Cu-SSZ-13 layer, catalytic activity in the NH₃-SCR of NO, hydrothermal stability and resistance against SO₂ poisoning was then investigated. The results indicate that by using PVA as the coating assistant agent, a firm layer of Cu-SSZ-13 can be formed on the surface of monolithic Cu-SSZ-13/Cordierite catalyst. Moreover, the Cu-SSZ-13(PVA)/Cordierite exhibits high catalytic activity in the NH₃-SCR of NO_x (close to that of the pristine Cu-SSZ-13 molecular sieve), high hydrothermal stability and good tolerance to SO₂, displaying great potential as a practicable catalyst for the removal of NO_x from exhausts of both the mobile and the stationary sources.
- Cu-SSZ-13,
- cordierite,
- monolithic catalyst,
- selective catalytic reduction of NO_x with NH₃,
- denitrification

FullText(HTML)

References(41)

References

[1]	BOSCH H, JANSSEN F. Formation and control of nitrogen oxides[J]. Catal Today, 1988, 2(4):369-379. http://www.sciencedirect.com/science/article/pii/0920586188800026
[2]	HERNÁNDEZ-GIMÉNEZ A M, LOZANO-CASTELLÓ D, BUENO-LÓPEZ A. Effect of CO₂, H₂O and SO₂ in the ceria-catalyzed combustion of soot under simulated diesel exhaust conditions[J]. Appl Catal B:Environ, 2014, 148-149:406-414. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=47ff4da17d95a70ba331013d86609d0b
[3]	刘小文, 李俊, 李加兴, 倪钟孝, 易秀乐, 陆新.烟气脱硝技术综述[J].广州化工, 2019, 47(24):53-55. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=gzhg201924020 LIU Xiao-wen, LI Jun, LI Jia-xing, NI Zhong-xiao, YI Xiu-le, LU Xin. Overview of flue gas denitrification technology[J]. Guangzhou Chem Ind (China), 2019, 47(24):53-55. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=gzhg201924020
[4]	QI G, YANG R, RINALDI F. Selective catalytic reduction of nitric oxide with hydrogen over Pd-based catalysts[J]. J Catal, 2006, 237(2):381-392. http://www.sciencedirect.com/science/article/pii/S0021951705004550
[5]	LI J, CHANG H, MA L, HAO J, YANG R T. Low-temperature selective catalytic reduction of NO_x with NH₃ over metal oxide and zeolite catalysts-A review[J]. Cataly Today, 2011, 175(1):147-156. http://www.sciencedirect.com/science/article/pii/S0920586111002434
[6]	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. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=277a26bc87ad6c96721f19cc69d98d90
[7]	BONINGARI T, KOIRALA R, SMIRNIOTIS P G. Low-temperature selective catalytic reduction of NO with NH₃ over V/ZrO₂ prepared by flame-assisted spray pyrolysis:Structural and catalytic properties[J]. Appl Catal B:Environ, 2012, 127:255-264. http://www.sciencedirect.com/science/article/pii/S0926337312003566
[8]	CHEN Z, YANG Q, LI H, LI X, WANG L, CHI TSANG S. 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. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=8109262
[9]	SCHNEIDER H, MACIEJEWSKI M, KOHLER K, WOKAUN A, BAIKER A. Chromia supported on titania:Ⅳ. Properties of different chromium oxide phases in the catalytic reduction of no by NH₃ studied by in situ diffuse reflectance FTIR spectroscopy[J]. J Catal, 1995, 157:312-320. http://www.sciencedirect.com/science/article/pii/S0021951785712961
[10]	SMIRNIOTIS P G, PENÃ D A, UPHADE B S. Low-temperature selective catalytic reduction (SCR) of NO with NH₃ by using Mn, Cr, and Cu oxides supported on hombikat TiO₂[J]. Angew Chem Int Ed, 2001, 40(13):2479-2482. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=e6162682f1b94e539588446374a86834
[11]	XIN Y, LI Q, ZHANG Z. Zeolitic materials for DeNO_x selective catalytic reduction[J]. ChemCatChem, 2018, 10(1):29-41. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=10.1002/cctc.201700854
[12]	CHEN L, LI J, GE M. DRIFT study on cerium-tungsten titiania catalyst for selective catalytic reduction of NO_x with NH₃[J]. Environ Sci Technol, 2010, 44(24):9590-9596. doi: 10.1021/es102692b
[13]	LIU F, ASAKURA K, HE H, SHAN W, SHI X, ZHANG C. Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NO_x with NH₃[J]. Appl Catal B:Environ, 2011, 103(3/4):369-377. http://www.sciencedirect.com/science/article/pii/S0926337311000622
[14]	ZHU Q, KONDO J N, OHNUMA R, KUBOTA Y, YAMAGUCHI M, TATSUMI T. The study of methanol-to-olefin over proton type aluminosilicate CHA zeolites[J]. Microporous Mesoporous Mater, 2008, 112(1/3):153-161. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cc7d73c543f52e0afd687143c7a618d7
[15]	BLEKEN F, BJØRGEN M, PALUMBO L, BORDIGA S, SVELLE S, LILLERUD K-P, OLSBYE U. The effect of acid strength on the conversion of methanol to olefins over acidic microporous catalysts with the CHA topology[J]. Top Catal, 2009, 52(3):218-228. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=e8edb27e4d70101cb50692e2c2cbaeb6
[16]	FICKEL D W, LOBO R F. Copper coordination in Cu-SSZ-13 and Cu-SSZ-16 investigated by variable-temperature XRD[J]. J Phys Chem C, 2010, 114(3):1633-1640. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=90670d2b7c29e13e5559d3c55fbb7e16
[17]	DEKA U, JUHIN A, EILERTSEN E A, EMERICH H, GREEN M A, KORHONEN S T, WECKHUYSEN B M, BEALE A M. Confirmation of isolated Cu²⁺ ions in SSZ-13 zeolite as active sites in NH₃-selective catalytic reduction[J]. J Phys Chem C, 2012, 116(7):4809-4818. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=591f7753708a4d216d8108acb395827c
[18]	FICKEL D W, D'ADDIO E, LAUTERBACH J A, LOBO R F. The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites[J]. Appl Catal B:Environ, 2011, 102(3/4):441-448. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=0fb9994b0a77714b0529c2edbe512293
[19]	BOGER T, HEIBEL A K, SORENSEN C M. Monolithic catalysts for the chemical industry[J]. Ind Eng Chem Res, 2004, 43(16):4602-4611. doi: 10.1002/chin.200439250
[20]	LIU Q, LIU Z, WU W. Effect of V₂O₅ additive on simultaneous SO₂ and NO removal from flue gas over a monolithic cordierite-based CuO/Al₂O₃ catalyst[J]. Catal Today, 2009, 147S:S285-S289. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=f57363d3c198098483ab07e883079a20
[21]	ZONES S I. Zeolite SSZ-13 and its method of preparation: US, 4544538[P]. 1985.
[22]	范超, 罗莉, 吴志伟, 朱华青, 秦张峰.整体式Pd/ZSM-5/Cordierite催化剂的制备及其低浓度甲烷燃烧催化性能[J].陕西师范大学学报(自然科学版), 2019, 47(1):94-100. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=sxsfdxxb201901014 FAN Chao, LUO Li, WU Zhi-wei, ZHU Hua-qing, QIN Zhang-feng. Preparation of monolithic Pd/ZSM-5/Cordierite catalyst for the combustion of lean methane[J]. J Shaanxi Normal Univ (Nat Sci Ed), 2019, 47(1):94-100. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=sxsfdxxb201901014
[23]	HE D, WANG Z, DENG D, DENG S, HE H, LIU L. Synthesis of Cu-SSZ-13 catalyst by using different silica sources for NO-SCR by NH₃[J]. Mol Catal, 2020, 484:110738. http://www.sciencedirect.com/science/article/pii/S2468823119306029
[24]	WANG Y, XIE L, LIU F, RUAN W. Effect of preparation methods on the performance of CuFe-SSZ-13 catalysts for selective catalytic reduction of NO_x with NH₃[J]. J Environ Sci, 2019, 81:195-204. doi: 10.1016/j.jes.2019.01.013
[25]	RICHTER M, FAIT M, ECKELT R, SCHNEIDER M, RADNIK J, HEIDEMANN D, FRICKE R. Gas-phase carbonylation of methanol to dimethyl carbonate on chloride-free Cu-precipitated zeolite Y at normal pressure[J]. J Catal, 2007, 245(1):11-24. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=4e01dd1282792c4a80ab722518b459a6
[26]	GAO F, WALTER E D, KARP E M, LUO J, TONKYN R G, KWAK J H, SZANYI J, PEDEN C H F. Structure-activity relationships in NH₃-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies[J]. J Catal, 2013, 300:20-29. doi: 10.1016/j.jcat.2012.12.020
[27]	KEFIROV R, PENKOVA A, HADJⅡVANOV K, DZWIGAJ S, CHE M. Stabilization of Cu⁺ ions in BEA zeolite:Study by FTIR spectroscopy of adsorbed CO and TPR[J]. Microporous Mesoporous Mater, 2008, 116(1/3):180-187. http://www.sciencedirect.com/science/article/pii/S1387181108001765
[28]	刘世成, 秦瑞香, 肖瑞, 张春雪, 王单, 刘通, 王金波.铜基ZSM-5分子筛催化氮氧化物的NH₃-SCR反应性能[J].重庆科技学院学报(自然科学版), 2019, 21(5):108-111. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cqsygdzkxxxb201905027 LIU Shi-cheng, QIN Rui-xiang, XIAO Rui, ZHANG Chun-xue, WANG Dan, LIU Tong, WANG Jin-bo. NH₃-SCR reaction of nitrogen oxides catalyzed by Cu-based ZSM-5 zeolite[J]. J Chongqing Univ Sci Technol(Nat Sci Ed), 2019, 21(5):108-111. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cqsygdzkxxxb201905027
[29]	DOU B, LV G, WANG C, HAO Q, HUI K. Cerium doped copper/ZSM-5 catalysts used for the selective catalytic reduction of nitrogen oxide with ammonia[J]. Chem Eng J, 2015, 270:549-556. doi: 10.1016/j.cej.2015.02.004
[30]	SULTANA A, SASAKI M, SUZUKI K, HAMADA H. Tuning the NO_x conversion of Cu-Fe/ZSM-5 catalyst in NH₃-SCR[J]. Catal Commun, 2013, 41:21-25. doi: 10.1016/j.catcom.2013.06.028
[31]	SJÖVALL H, OLSSON L, FRIDELL E, BLINT R J. Selective catalytic reduction of NO_x with NH₃ over Cu-ZSM-5-The effect of changing the gas composition[J]. Appl Catal B:Environ, 2006, 64:180-188. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=dfc71c904d667ae8c88f000dc1b6c14b
[32]	WANG C, WANG C, WANG J, WANG J, SHEN M, LI W. Effects of Na⁺ on Cu/SAPO-34 for ammonia selective catalytic reduction[J]. J Environ Sci, 2018, 70:20-28.
[33]	XIE K, LEISTNER K, WIJAYANTI K, KUMAR A, KAMASAMUDRAM K, OLSSON L. Influence of phosphorus on Cu-SSZ-13 for selective catalytic reduction of NO_x by ammonia[J]. Catal Today, 2017, 297:46-52. http://www.sciencedirect.com/science/article/pii/S0920586117304996
[34]	HAMMERSHØI P S, JANGJOU Y, EPLING W S, JENSEN A D, JANSSENS T V W. Reversible and irreversible deactivation of Cu-CHA NH₃-SCRcatalysts by SO₂ and SO₃[J]. Appl Catal B:Environ, 2018, 226:38-45. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=c25108693c8e96c4d365404b3fdcdda1
[35]	HAMMERSHØI P S, VENNESTRØM P N R, FALSIG H, JENSEN A D, JANSSENS T V W. Importance of the Cu oxidation state for the SO₂-poisoning of a Cu-SAPO-34 catalyst in the NH₃-SCR reaction[J]. Appl Catal B:Environ, 2018, 236:377-383. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=76dda9bf0ff01d8c0b89ea3c33ba46dc
[36]	JANGJOU Y, DO Q, GU Y, LIM L-G, SUN H, WANG D, KUMAR A, LI J, GRABOW L C, EPLING W S. Nature of Cu active centers in Cu-SSZ-13 and their responses to SO₂ exposure[J]. ACS Catal, 2018, 8(2):1325-1337. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=d8e0d423adb8ade658e9999615bcf17b
[37]	ZHANG L, WANG D, LIU Y, KAMASAMUDRAM K, LI J, EPLING W. SO₂ poisoning impact on the NH₃-SCR reaction over a commercial Cu-SAPO-34 SCR catalyst[J]. Appl Catal B:Environ, 2014, 156-157:371-377. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=4e74299b00dc25a2f8e041fc9c08dbf7
[38]	JANGJOU Y, WANG D, KUMAR A, LI J, EPLING W S. SO₂ poisoning of the NH₃-SCR reaction over Cu-SAPO-34:Impact of ammonium sulfate versus other S-containing species[J]. ACS Catal, 2016, 6(10):6612-6622. http://smartsearch.nstl.gov.cn/paper_detail.html?id=ac8656054151718e654efb7b72c2d617
[39]	FERRIZZ R M, GORTE R J, VOHS J M. TPD and XPS investigation of the interaction of SO₂ with model ceria catalysts[J]. Catal Lett, 2002, 82:123-129. doi: 10.1023/A:1020512713021
[40]	KONG L, ZOU S, MEI J, GENG Y, ZHAO H, YANG S. Outstanding resistance of H₂S-modified Cu/TiO₂ to SO₂ for capturing gaseous Hg(0) from nonferrous metal smelting flue gas:Performance and reaction mechanism[J]. Environ Sci Technol, 2018, 52(17):10003-10010. http://smartsearch.nstl.gov.cn/paper_detail.html?id=c6e5758536eee1cfdb9e0a4e24468bc7
[41]	THEGE I K. DSC investigation of the thermal behaviour of (NH₄)₂SO₄, NH₄HSO₄ and NH₄NH₂SO₃[J]. Thermochim Acta, 1983, 60(2):149-159. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=10.1002/chin.198314019