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Cation doped cerium oxynitride with anion vacancies for Fe-based catalyst with improved activity and oxygenate tolerance for efficient synthesis of ammonia

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Humphreys, John, Lan, Rong, Chen, Shigang, Walker, Marc, Han, Yisong and Tao, Shanwen (2021) Cation doped cerium oxynitride with anion vacancies for Fe-based catalyst with improved activity and oxygenate tolerance for efficient synthesis of ammonia. Applied Catalysis B: Environmental . 119843. doi:10.1016/j.apcatb.2020.119843 ISSN 0926-3373.

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Official URL: http://dx.doi.org/10.1016/j.apcatb.2020.119843

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Abstract

For the first time, new Sm doped cerium oxynitrides with the formula Ce1-zSmzO2-xNy (z ≤ 0.5) are synthesized in order to maximize the concentration of anion vacancies. Single phase Sm-doped CeO2-xNy were confirmed by XRD, HRTEM and Rietveld refinement. These oxynitrides show a great promotion effect for the low-cost Fe catalyst for the ammonia synthesis. At 350 °C and 1 MPa, the activity of 80 wt% Fe- 20 wt% Ce1-zSmzO2xNy is one of the highest reported for non-Ru catalysts for the Haber-Bosch reaction. The apparent activation energy of the 80 wt% Fe- 20 wt% Ce1-zSmzO2xNy catalysts with z ≥ 0.3 is around 45 kJ/mol, which is in the lowest range among all reported ammonia synthesis catalysts. Introduction of nitrogen vacancies through doping may facilitate the mobility of nitrogen vacancies. This study demonstrates doped oxynitrides with a large concentration of anion vacancies, particularly nitrogen vacancies are excellent promoters/co-catalysts for ammonia synthesis.

Item Type: Journal Article
Subjects: Q Science > QC Physics
T Technology > TP Chemical technology
Divisions: Faculty of Science, Engineering and Medicine > Engineering > Engineering
Faculty of Science, Engineering and Medicine > Science > Physics
Library of Congress Subject Headings (LCSH): Ammonia -- Synthesis , Anions
Journal or Publication Title: Applied Catalysis B: Environmental
Publisher: Elsevier BV
ISSN: 0926-3373
Official Date: 15 May 2021
Dates:
DateEvent
15 May 2021Published
25 December 2020Available
7 December 2020Accepted
Article Number: 119843
DOI: 10.1016/j.apcatb.2020.119843
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Open Access (Creative Commons)
Date of first compliant deposit: 7 January 2021
Date of first compliant Open Access: 11 January 2021
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
EP/G01244X/1[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
Is Part Of: 1

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