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Nature of SO3 poisoning on Cu/SAPO-34 SCR catalysts
被引:59
|作者:
Shen, Meiqing
[1
,3
,4
]
Zhang, Yun
[1
]
Wang, Jianqiang
[1
]
Wang, Chen
[2
]
Wang, Jun
[1
]
机构:
[1] Tianjin Univ, Sch Chem Engn & Technol, State Educ Minist, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China
[2] North Univ China, Sch Environm & Safety Engn, Taiyuan 030051, Shanxi, Peoples R China
[3] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
[4] Tianjin Univ, State Key Lab Engines, Tianjin 300072, Peoples R China
基金:
中国国家自然科学基金;
关键词:
Cu/SAPO-34;
SO3 poisoning mechanism;
Si-O(H)-Al breakage;
Dealumination;
Extra-framework species;
TRANSITION-METAL IONS;
DEACTIVATION MECHANISM;
NH3-SCR REACTION;
REDOX BEHAVIOR;
CU SITES;
REDUCTION;
ZEOLITE;
SULFUR;
IMPACT;
STABILITY;
D O I:
10.1016/j.jcat.2017.12.008
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
To reveal the nature of SO3 poisoning of Cu/SAPO-34 selective catalytic reduction (SCR) catalysts, CHA structure, copper species, and NOx conversion were probed. The Cu/SAPO-34 catalyst was treated with different ratios of SO3 to SOx (0, 6, 13, and 20%) at 250 degrees C. The breakage of Si-O(H)-Al bonds takes place and leads to aluminum sulfate formation upon SOx sulfation. More isolated Cu2+ transform to copper sulfate with an increment of the SO3/SOx ratio. Catalysts poisoned with SOx show lower NOx conversion at 150-300 degrees C, the reason for which is a reduced number of isolated Cu2+ sites, as their turnover frequencies (TOFs) are identical. The loss of isolated Cu2+ and Si-O(H)-Al bonds is responsible for the inferior activity above 300 degrees C. The presence of SO3 cannot be ignored because of the irreversible reaction with Cu/SAPO-34 when diesel oxidation catalysts are applied upstream of the SCR. (C) 2017 Elsevier Inc. All rights reserved.
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页码:277 / 286
页数:10
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