Catalytic deactivation mechanism research over Cu/SAPO-34 catalysts for NH3-SCR (II): The impact of copper loading

被引：43

作者：

Tang, Jiaojiao ^{[1
]}

Xu, Minhong ^{[1
]}

Yu, Tie ^{[1
,2
,4
]}

Ma, Hongfei ^{[2
]}

Shen, Meiqing ^{[1
,3
]}

Wang, Jun ^{[1
,3
]}

机构：

[1] Tianjin Univ, Sch Chem Engn & Technol, State Educ Minist, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China

[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Zhongshan Rd 457, Dalian 116023, Peoples R China

[3] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China

[4] Chem Sci & Mat Syst Lab, Gen Motors Global Res & Dev, 3500 Mound Rd, Warren, MI 48090 USA

来源：

CHEMICAL ENGINEERING SCIENCE | 2017年 / 168卷

基金：

中国国家自然科学基金;

关键词：

Cu/SAPO-34; NH3-SCR; 950 degrees C hydrothermal treatment; Structure stability; IN-SITU SYNTHESIS; CU-SAPO-34; CATALYSTS; MOLECULAR-SIEVE; HYDROTHERMAL STABILITY; LOW-TEMPERATURE; NOX; REDUCTION; SAPO-34; AMMONIA; SCR;

D O I：

10.1016/j.ces.2017.04.053

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

Four Cu/SAPO-34 samples by one-pot method are utilized to examine their durability after 950 degrees C hydrothermal treatment and its relation with copper loading, The SCR results show fresh Cu/SAP0-34 with 3.91% copper loading (F-Cu-3.91) performs the superior NO conversion, wide temperature window and excellent nitrogen selectivity among fresh samples, and NO conversion is mainly determined by isolated Cu2+ contents at low temperature. After 950 degrees C aging treatment, Cu/SAPO-34 catalysts with copper loading under 1.70% present good stability, while the ones with copper loading above 3.91% show activity and crystallinity decline. Ex-situ DRIFTs, XRD and NH3-TPD results reveal the 950 degrees C aging process leads to Si-OH-Al bonds breakage and phase transition of chabazite support over Cu/SAPO-34 samples with high copper loading, meanwhile, the EPR and TPR outcomes prove the copper oxides' further dispersion and coordination variation due to skeleton collapse. Finally, this work is trying to manifest the appropriate copper loading for a stable Cu/SAPO-34 catalyst and its deactivation mechanism during extreme working situation. (C) 2017 Elsevier Ltd. All rights reserved.

引用

页码：414 / 422

页数：9

共 31 条

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