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In-situ infrared spectroscopic study of the mechanism of the low temperature selective catalytic reduction of NO surface by Mn/ bastnaesite concentrate.

Authors :
Chen, Zedong
Li, Na
Zhang, Kai
Hou, Limin
Wu, Wenfei
Source :
International Journal of Hydrogen Energy. Jul2022, Vol. 47 Issue 59, p24777-24795. 19p.
Publication Year :
2022

Abstract

The Mn/bastnaesite concentrate and Mn/Al 2 O 3 catalysts were prepared by impregnation method, and their NH 3 -SCR denitrification performance was tested. The results showed that the Mn/bastnaesite concentrate catalyst achieved up to 95% NO conversion rate at 150 °C, and the Mn/Al 2 O 3 catalyst reached 76% at 300 °C. A series of characterisation results showed that the bastnaesite concentrate can better interact with MnOx species and promote mutual dispersion compared to Al 2 O 3. The Mn/bastnaesite concentrate has a stronger redox capacity, and good NH 3 and NO adsorption capacity at low temperatures. The multi-element coexistence system of bastnaesite concentrate itself is a significant advantage of its use as a carrier. In-situ Fourier transform infrared (FTIR) results showed that the Mn/bastnaesite concentrate catalyst follows an L-H mechanism throughout the reaction, with NH 4 + species in the Brønsted acidic site on the catalyst surface being the main reactant species. Most of NO is converted to monodentate nitrite, which is formed by bonding with Mn3+ provided by the supported Mn species, rare earth elements and transition metal ions contained in the carrier itself to form O–N–O–Mn3+ intermediates, which participate in the reaction together, and then combined with the adsorbed NH 4 +/NH 3 species to produce N 2 and H 2 O. An E-R mechanism was also present on the catalyst surface, NO participates directly in the reaction in gaseous form, and the NO [NH 2 ](ads) intermediate species produced by interaction with NH 4 + species in the acidic position of Brønsted was further decomposed to N 2 and H 2 O. By comparing the reaction mechanism with the commonly used catalyst carrier Al 2 O 3 for NH 3 -SCR, it can be concluded that bastnaesite concentrate as a carrier not only has the performance of conventional carriers, but also has certain catalytic activity and can interact with the active components to give it excellent performance, which provides a theoretical basis for rare earth minerals as denitrification catalysts. • The first use of bastnaesite concentrate from Baiyun Ebo as a carrier for NH 3 -SCR catalysts. • Mn/bastnaesite concentrate Catalyst with Excellent Low Temperature Denitrification Performance. • The Ce 7 O 12 species has a better mutual promotion with Mn. • The Mn3+ will bond with the monodentate nitrate species to form O–N–O–Mn3+ species involved in the reaction. • Mn/bastnaesite concentrate surface was a dual-mechanism coexistence with more reaction pathways. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
03603199
Volume :
47
Issue :
59
Database :
Academic Search Index
Journal :
International Journal of Hydrogen Energy
Publication Type :
Academic Journal
Accession number :
158310581
Full Text :
https://doi.org/10.1016/j.ijhydene.2022.05.249