In situ IR studies of selective catalytic reduction of NO with NH3 on Ce-Ti amorphous oxides

doi:10.1016/S1872-2067(14)60154-6

Chinese Journal of Catalysis ›› 2014, Vol. 35 ›› Issue (8): 1289-1298.DOI: 10.1016/S1872-2067(14)60154-6

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In situ IR studies of selective catalytic reduction of NO with NH₃ on Ce-Ti amorphous oxides

Qian Li^a,b, Huachun Gu^a, Ping Li^a, Yuhao Zhou^a, Ying Liu^a, Zhongnan Qi^a, Ying Xin^a, Zhaoliang Zhang^a,b

a. School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, Shandong, China;
b. Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Sciences and Engineering, Nanjing University of Information Sciences and Engineering, Nanjing 210044, Jiangsu, China

Received:2014-03-31 Revised:2014-05-23 Online:2014-08-01 Published:2014-08-05
Supported by:
This work was supported by the National Natural Science Foundation of China (21277060 and 21107030), the Development Program of the Science and Technology of Shandong Province (2011GSF11702), the Foundation for Outstanding Young Scientist in Shandong Province (BS2011HZ002), the Natural Science Foundation of Shandong Province (ZR2013BQ003), and the Open Project from Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control of Nanjing University of Information Science and Technology (KHK1116), Jiangsu Province Innovation Platform for Superiority Subject of Environmental Science and Engineering.

Abstract

Abstract:

A series of in situ infrared (IR) studies of the selective catalytic reduction (SCR) of NO_x with NH₃ on the short-range ordered structure Ce-O-Ti sites in amorphous Ce-Ti mixed oxides were performed. Under the reaction conditions, the catalyst surface was mainly covered by NH₃ ad-species and no NO_x ad-species were detected. The reaction order of 0.5-0.6 with respect to NO confirmed a hybrid Langmuir-Hinshelwood and Eley-Rideal mechanism. A possible route may involve the reaction of NH₃ ad-species and weakly adsorbed NO_x to form an active intermediate, NH_yNO₃ (y = 0-4); this was confirmed by GAUSSIAN calculations and the in situ IR results. The Ce-O-Ti structure, with Ce-Ti interactions on the atomic scale, enhanced the redox properties in the active temperature window of the SCR reactions.

Key words: Selective catalytic reduction, Nitrogen oxide, Ammonia, Amorphous Ce-Ti mixed oxide, In situ infrared, Mechanism

Qian Li, Huachun Gu, Ping Li, Yuhao Zhou, Ying Liu, Zhongnan Qi, Ying Xin, Zhaoliang Zhang. In situ IR studies of selective catalytic reduction of NO with NH₃ on Ce-Ti amorphous oxides[J]. Chinese Journal of Catalysis, 2014, 35(8): 1289-1298.

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In situ IR studies of selective catalytic reduction of NO with NH₃ on Ce-Ti amorphous oxides

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