Insight into SO2 poisoning over Cu-SAPO-18 used for NH3-SCR

被引:31
作者
Ming, Shujun [1 ]
Pang, Lei [3 ]
Chen, Zhen [1 ]
Guo, Yanbing [2 ]
Guo, Lei [1 ]
Liu, Qian [1 ]
Liu, Peng [1 ]
Dong, Yahao [1 ]
Zhang, Shoute [1 ]
Li, Tao [1 ]
机构
[1] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Mat Chem & Serv Failure, Key Lab Mat Chem Energy Convers & Storage,Minist, Wuhan 430074, Peoples R China
[2] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China
[3] DongFeng Trucks R&D Ctr, Wuhan 430056, Peoples R China
基金
中国国家自然科学基金;
关键词
NH3-SCR; SO2; poisoning; Cu-SAPO-18; Sulfate species; Regeneration; SELECTIVE CATALYTIC-REDUCTION; IN-SITU DRIFTS; SCR CATALYSTS; NO OXIDATION; ACTIVE-SITES; CU-SSZ-13; NH3; SULFUR; DEACTIVATION; IMPACT;
D O I
10.1016/j.micromeso.2020.110294
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The impact of SO2 poisoning on Cu-SAPO-18 physicochemical properties and its NH3-SCR reaction mechanism was investigated. After exposing Cu-SAPO-18 to SO2+O-2 for 40 min, the sulfite and sulfate species were detected on Cu-SAPO-18 surface, which caused a small decrease in BET surface area and micropore volume, the increase in NH3 storage and the deactivation of some isolated Cu2+ sites. These could be interpreted by the slight micropore blocking, interaction between sulfates and NH3 forming new NH4+ species and the formation of Cu-sulfate, respectively. Additionally, it was observed that isolated Cu2+ ions in pear-shaped cavity of AEI structure, which are beneficial to good low-temperature deNO(x) activity, were more severely poisoned by SO2 than Cu2+ in the double 6-membered ring (D6R). Accordingly, the NH3-SCR activity below 350 degrees C was restrained by SO2. Moreover, the in-situ DRIFTS results indicate that Cu-SAPO-18 catalyzed NH3-SCR reaction predominantly proceeds through Langmuir-Hinshelwood (L-H) mechanism at low temperature. SO2 poisoning inhibited the adsorption of NO + O-2 and NH3 on Cu2+ sites, thereby decreasing the formation of Cu-NOx and Cu-NH3 intermediates, evidently, the L-H mechanism was suppressed by SO2. Interestingly, the deactivated Cu-SAPO-18 could be regenerated under SCR gas at 550 degrees C and resumed at least most NH3-SCR activity.
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页数:11
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共 64 条
[1]   Fe-H-BEA and Fe-H-ZSM-5 for NO2 removal from ambient air - A detailed in situ and operando FTIR study revealing an unexpected positive water-effect [J].
Ahrens, Mike ;
Marie, Olivier ;
Bazin, Philippe ;
Daturi, Marco .
JOURNAL OF CATALYSIS, 2010, 271 (01) :1-11
[2]   Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts [J].
Brookshear, D. William ;
Nam, Jeong-gil ;
Ke Nguyen ;
Toops, Todd J. ;
Binder, Andrew .
CATALYSIS TODAY, 2015, 258 :359-366
[3]   Cerium promotion on the hydrocarbon resistance of a Cu-SAPO-34 NH3-SCR monolith catalyst [J].
Cao, Yi ;
Lan, Li ;
Feng, Xi ;
Yang, Zhengzheng ;
Zou, Sha ;
Xu, Haidi ;
Li, Zheqi ;
Gong, Maochu ;
Chen, Yaoqiang .
CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (09) :4511-4521
[4]   Improvement of Activity and SO2 Tolerance of Sn-Modified MnOx-CeO2 Catalysts for NH3-SCR at Low Temperatures [J].
Chang, Huazhen ;
Chen, Xiaoyin ;
Li, Junhua ;
Ma, Lei ;
Wang, Chizhong ;
Liu, Caixia ;
Schwank, Johannes W. ;
Hao, Jiming .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5294-5301
[5]   Simultaneous Removal of SO2 and NOx by Calcium Hydroxide at Low Temperature: Effect of SO2 Absorption on NO2 Removal [J].
Chen, Guoqing ;
Gao, Jihui ;
Gao, Jianmin ;
Du, Qian ;
Fu, Xiaolin ;
Yin, Yijun ;
Qin, Yukun .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (23) :12140-12147
[6]   NO oxidation on zeolite supported Cu catalysts: Formation and reactivity of surface nitrates [J].
Chen, Hai-Ying ;
Wei, Zhehao ;
Kollar, Marton ;
Gao, Feng ;
Wang, Yilin ;
Szanyi, Janos ;
Peden, Charles H. F. .
CATALYSIS TODAY, 2016, 267 :17-27
[7]   DRIFT Study of CuO-CeO2-TiO2 Mixed Oxides for NOx Reduction with NH3 at Low Temperatures [J].
Chen, Lei ;
Si, Zhichun ;
Wu, Xiaodong ;
Weng, Duan .
ACS APPLIED MATERIALS & INTERFACES, 2014, 6 (11) :8134-8145
[8]   One-pot synthesis of high performance Cu-SAPO-18 catalyst for NO reduction by NH3-SCR: Influence of silicon content on the catalytic properties of Cu-SAPO-18 [J].
Chen, Zhen ;
Fan, Chi ;
Pang, Lei ;
Ming, Shujun ;
Guo, Wen ;
Liu, Peng ;
Chen, Hanping ;
Li, Tao .
CHEMICAL ENGINEERING JOURNAL, 2018, 348 :608-617
[9]   The different impacts of SO2 and SO3 on Cu/zeolite SCR catalysts [J].
Cheng, Yisun ;
Lambert, Christine ;
Kim, Do Heui ;
Kwak, Ja Hun ;
Cho, Sung June ;
Peden, Charles H. F. .
CATALYSIS TODAY, 2010, 151 (3-4) :266-270
[10]   Chemical aging of Cu-SSZ-13 SCR catalysts for heavy-duty vehicles - Influence of sulfur dioxide [J].
Dahlin, Sandra ;
Lantto, Cornelia ;
Englund, Johanna ;
Westerberg, Bjorn ;
Regali, Francesco ;
Skoglundh, Magnus ;
Pettersson, Lars J. .
CATALYSIS TODAY, 2019, 320 :72-83