Influence of sulfation on CeO2-ZrO2 catalysts for NO reduction with NH3

doi:10.1016/S1872-2067(16)62581-0

Chinese Journal of Catalysis ›› 2017, Vol. 38 ›› Issue (1): 160-167.DOI: 10.1016/S1872-2067(16)62581-0

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Influence of sulfation on CeO₂-ZrO₂ catalysts for NO reduction with NH₃

He Zhang^a, Yonggang Zou^a, Yue Peng^b

a State Key Laboratory of High Power Semiconductor Lasers, Changchun University of Science and Technology, Changchun 130022, Jilin, China;
b School of Civil and Environmental Engineering and the Brook Byers Institute for Sustainable Systems, Georgia Institute of Technology, 800 West Peachtree Street, Suite 400 F-H, Atlanta, Georgia, 30332-0595, United States

Received:2016-09-09 Revised:2016-10-18 Online:2017-01-18 Published:2017-01-18
Contact: Yue Peng,Tel:+1-404-483-8691;Fax:+1-404-894-5676;E-mail:pengyue2015@sina.com;Yonggang Zou,Tel:+86-431-85583395;Fax:+86-431-85582473;E-mail:zouyg@cust.edu.cn
Supported by:
This work was supported by the Science Fund for Yong Scholars at Changchun University of Science and Technology (XQNJJ-2014-15).

Abstract

Abstract:

CeO₂-ZrO₂ (CeZr) and sulfated CeO₂-ZrO₂ (S-CeZr) catalysts were prepared for the selective catalytic reduction of NO with NH₃. The CeZr catalysts exhibited higher activity at low temperatures (<200℃) and lower activity at high temperatures (> 200℃) than the S-CeZr catalysts. The sulfation of CeZr was studied in terms of surface acidity, redox properties and NO adsorption-desorption by temperature-dependent experiments and in situ infrared spectroscopy. S-CeZr displayed high con-centrations of acidic sites and increased surface acidities, but poor reducibility compared with CeZr. The high acidity of S-CeZr was attributed to the presence of Brønsted acid sites, arising mainly from the surface sulfates. Because the surface was covered with sulfate species, S-CeZr showed lower NO adsorption and weaker oxidation ability than CeZr. The adsorption of NH₃ on the Brønsted acid sites restricted the reaction with NO at low temperatures, but the selective catalytic reduction cycle oc-curred easily at relatively low temperatures (150℃), and the weakly bound nitrite was partially activated on the S-CeZr catalyst at relatively high temperatures (300℃). The catalytic mechanisms for the CeZr and S-CeZr catalysts at 150 and 300℃ were also studied.

Key words: Sulfation, Removal of nitrogen oxides, Selective catalytic reduction, Ceria, Zirconia

He Zhang, Yonggang Zou, Yue Peng. Influence of sulfation on CeO₂-ZrO₂ catalysts for NO reduction with NH₃[J]. Chinese Journal of Catalysis, 2017, 38(1): 160-167.

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Influence of sulfation on CeO₂-ZrO₂ catalysts for NO reduction with NH₃

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