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.
引用
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页数:11
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