Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation

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 exhibi...

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Main Authors: Liu, Jie, Li, Xin Yong, Zhao, Q., Ke, Jun, Xiao, H., Lv, X., Liu, Shaomin, Tadé, Moses, Wang, Shaobin
Format: Journal Article
Published: Elsevier BV 2017
Online Access:http://purl.org/au-research/grants/arc/DP150103026
http://hdl.handle.net/20.500.11937/18001
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author Liu, Jie
Li, Xin Yong
Zhao, Q.
Ke, Jun
Xiao, H.
Lv, X.
Liu, Shaomin
Tadé, Moses
Wang, Shaobin
author_facet Liu, Jie
Li, Xin Yong
Zhao, Q.
Ke, Jun
Xiao, H.
Lv, X.
Liu, Shaomin
Tadé, Moses
Wang, Shaobin
author_sort Liu, Jie
building Curtin Institutional Repository
collection Online Access
description 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.
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publisher Elsevier BV
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spelling curtin-20.500.11937-180012022-10-26T06:25:17Z Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation Liu, Jie Li, Xin Yong Zhao, Q. Ke, Jun Xiao, H. Lv, X. Liu, Shaomin Tadé, Moses Wang, Shaobin 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. 2017 Journal Article http://hdl.handle.net/20.500.11937/18001 10.1016/j.apcatb.2016.07.020 http://purl.org/au-research/grants/arc/DP150103026 Elsevier BV restricted
spellingShingle Liu, Jie
Li, Xin Yong
Zhao, Q.
Ke, Jun
Xiao, H.
Lv, X.
Liu, Shaomin
Tadé, Moses
Wang, Shaobin
Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title_full Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title_fullStr Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title_full_unstemmed Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title_short Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation
title_sort mechanistic investigation of the enhanced nh3-scr on cobalt-decorated ce-ti mixed oxide: in situ ftir analysis for structure-activity correlation
url http://purl.org/au-research/grants/arc/DP150103026
http://hdl.handle.net/20.500.11937/18001