FeO-CeO@AlO Nanoarrays on Al-Mesh as SO-Tolerant Monolith Catalysts for NO Reduction by NH.

Environ Sci Technol

Department of Chemistry, College of Sciences, Research Center of Nano Science and Technology, School of Materials Science and Engineering , Shanghai University, Shanghai , 200444 , China.

Published: May 2019

Currently, selective catalytic reduction of NO with NH in the presence of SO is still challenging at low temperatures (<300 °C). In this study, enhanced NO reduction was achieved over a SO-tolerant Fe-based monolith catalyst, which was originally developed through in situ construction of AlO nanoarrays (na-AlO) on the monolithic Al-mesh by a steam oxidation method followed by anchoring FeO and CeO onto the na-AlO@Al-mesh composite by an impregnation method. The optimum catalyst delivered more than 90% NO conversion and N selectivity above 98% within 250-430 °C as well as excellent SO tolerance at 270 °C. The strong interaction between FeO and CeO enabled favorable electron transfers from FeO to CeO while generating more oxygen vacancies and active oxygen species, consequently accelerating the redox cycle. The improved reactivity of NH with nitrates following the Langmuir-Hinshelwood mechanism and active NH species that directly reacted with gaseous NO following the Eley-Rideal mechanism enhanced the NO reduction efficiency at low temperatures. The preferential sulfation of CeO alleviated the sulfation of FeO while maintaining the high reactivities of NH and NH species. Especially, the SCR reaction following the Eley-Rideal mechanism largely improved the SO tolerance because NO does not need to compete with sulfates to adsorb on the catalyst surface as nitrates or nitrites. This work paves a way for the development of high-performance SO-tolerant SCR monolith catalysts.

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http://dx.doi.org/10.1021/acs.est.9b01217DOI Listing

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