Unexpected increase in low-temperature NH3-SCR catalytic activity over Cu-SSZ-39 after hydrothermal aging

被引:60
作者
Du, Jinpeng [1 ,2 ]
Shan, Yulong [1 ]
Sun, Yu [1 ,2 ]
Gao, Meng [1 ,2 ]
Liu, Zhongqi [1 ,2 ]
Shi, Xiaoyan [1 ,2 ]
Yu, Yunbo [1 ,2 ]
He, Hong [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China
基金
中国国家自然科学基金;
关键词
NOx reduction; NH3-SCR; Cu-SSZ-39; Hydrothermal aging; CuxOy species; HIGH-SILICA LTA; SITU-DRIFTS; NOX; REDUCTION; CU/SAPO-34; ZEOLITES; NH3; SCR; STABILITY; TRANSIENT;
D O I
10.1016/j.apcatb.2021.120237
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
The control of nitrogen oxides (NOx) from heavy-duty diesel vehicles is becoming increasingly urgent due to its detrimental effects on the environment. Cu-SSZ-39, with its exceptional NH3-SCR activity and hydrothermal stability, has attracted more and more attention in the field of diesel vehicle emission control. In this work, an unexpected phenomenon was observed for Cu-SSZ-39 after hydrothermal aging. Generally, the hydrothermal aging process causes deterioration of the catalytic performance of catalysts. However, a remarkable increase in low-temperature NH3-SCR catalytic activity was observed in Cu-SSZ-39 after it was exposed to 850 degrees C hydrothermal aging conditions for 16 h. EPR, DRIFTS, H-2-TPR, UV-vis and XANES were utilized to detect the changes in Cu species. It was determined that a portion of the Cu2+ ions near double six-membered rings (d6r) transformed into CuxOy species after hydrothermal treatment. These CuxOy species facilitated the production of nitrate species which were critical intermediates in the NH3-SCR process, resulting in an increase in low-temperature catalytic activity.
引用
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页数:10
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