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SO2 promoted in situ recovery of thermally deactivated Fe2(SO4)3/TiO2 NH3-SCR catalysts: from experimental work to theoretical study

Yu, Yanke, Chen, Changwei, Ma, Mudi, Douthwaite, Mark, He, Chi, Miao, Jifa, Chen, Jinsheng and Li, Can 2019. SO2 promoted in situ recovery of thermally deactivated Fe2(SO4)3/TiO2 NH3-SCR catalysts: from experimental work to theoretical study. Chemical Engineering Journal 361 , pp. 820-829. 10.1016/j.cej.2018.12.149
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Abstract

Due to high catalytic activity and excellent resistance to SO2 and H2O, sulfate materials are considered to be promising vanadium-free catalysts for selective catalytic reduction of NOx with NH3 (NH3-SCR). Despite this, investigations about thermal stability of sulfate SCR catalysts are limited, which is surprising given that sulfates are typically susceptible to thermal decomposition. In this work, the thermal stability of Fe2(SO4)3/TiO2 catalysts was investigated. It was determined that the thermal decomposition of Fe2(SO4)3 resulted in NOx conversion decreased from 90% to 60% at 350 °C. Interestingly however, the introduction of SO2 into the gas stream was found to reverse the effects of the thermal deactivation and the NOx conversion of 90% (350 °C) was once again observed. Extensive characterization of each catalyst sample and density functional theory (DFT) calculations were subsequently conducted. The reduction in catalytic activity after the thermal treatment was attributed to the transformation of Fe2(SO4)3 to α-Fe2O3, which reduced the quantity of Brønsted acid sites on the catalyst. The presence of SO2 in the gas stream was found to reverse this phase transformation which ultimately led to the recovery of Brønsted acid sites. DFT calculations indicated that SO2 adsorbed selectively on Fe atoms of the thermal deactivated catalysts and S-Fe bond should mainly be formed by electrons from p orbitals of S and Fe atoms. Then NH3 could be adsorbed on the surface by N-S bond with SO2. The recoverable property of this catalyst provides a promising outlook for the commercial application, especially given that industrial flue gas streams regularly contain SO2.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Elsevier
ISSN: 1385-8947
Date of First Compliant Deposit: 9 May 2019
Date of Acceptance: 27 December 2018
Last Modified: 02 Jul 2019 19:34
URI: http://orca-mwe.cf.ac.uk/id/eprint/122297

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