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.
引用
收藏
页码:277 / 286
页数:10
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