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https://hdl.handle.net/2440/114380
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Type: | Journal article |
Title: | Mechanistic investigation of the enhanced NH₃-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation |
Other Titles: | Mechanistic investigation of the enhanced NH(3)-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation |
Author: | Liu, J. Li, X. Zhao, Q. Ke, J. Xiao, H. Lv, X. Liu, S. Tadé, M. Wang, S. |
Citation: | Applied Catalysis B: Environmental, 2017; 200:297-308 |
Publisher: | Elsevier BV |
Issue Date: | 2017 |
ISSN: | 0926-3373 1873-3883 |
Statement of Responsibility: | Jie Liu, Xinyong Li, Qidong Zhao, Jun Ke, Huining Xiao, Xiaojuan Lv, Shaomin Liu, Moses Tadé, Shaobin Wang |
Abstract: | A series of transition metals (Co, Cu and Fe) were selected to decorate Ce-Ti mixed oxide to elevate the low-temperature activity of selective catalytic reduction of NOx by NH3 (NH3-SCR) reaction, by adjusting the ratio of surface Ce3+ species and oxygen vacancies. Among them, Co-Ce-Ti sample exhibited the excellent low-temperature activity and broadened temperature window, which could be attributed to the improvement of the physico-chemical properties and the acceleration of the reactions in the Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. Owing to the different ionic sizes of Co2+ and Ce4+, the lattice distortion of Ce-Ti mixed oxide was greatly aggravated and subsequently increased the ratio of Ce3+ and the surface adsorbed oxygen, which benefited the generation of adsorbed NOx species and improved the reaction in the L-H mechanism. Meanwhile, the coordinatively unsaturated cationic sites over the Co-Ce-Ti sample induced more Lewis acid sites and enhanced the formation of the adsorbed NH3 species bounded with Lewis acid sites, which were considered as the crucial intermediates in E-R mechanism, and therefore facilitating the reaction between the adsorbed NH3 species and NO molecules. The enhancements in both the reactions from L-H and E-R mechanisms appeared to directly correlated with the improved deNOx performance on the Co-Ce-Ti sample, and the L-H mechanism could be the dominate one at low temperatures due to its rapid reaction rate. |
Keywords: | Low-temperature NH₃-SCR; nitrogen oxides (NO×); surface Ce³⁺ species; In situ FTIR; reaction mechanism |
Description: | Available online 16 July 2016 |
Rights: | © 2016 Published by Elsevier B.V. |
DOI: | 10.1016/j.apcatb.2016.07.020 |
Grant ID: | 21507029 21501138 2016MS109 2015ZD25 http://purl.org/au-research/grants/arc/DP150103026 |
Published version: | http://dx.doi.org/10.1016/j.apcatb.2016.07.020 |
Appears in Collections: | Aurora harvest 3 Chemical Engineering publications |
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