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A spin promotion effect in catalytic ammonia synthesis

The need for efficient ammonia synthesis is as urgent as ever. Over the past two decades, many attempts to find new catalysts for ammonia synthesis at mild conditions have been reported and, in particular, many new promoters of the catalytic rate have been introduced beyond the traditional K and Cs...

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Autores principales: Cao, Ang, Bukas, Vanessa J., Shadravan, Vahid, Wang, Zhenbin, Li, Hao, Kibsgaard, Jakob, Chorkendorff, Ib, Nørskov, Jens K.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9061734/
https://www.ncbi.nlm.nih.gov/pubmed/35501341
http://dx.doi.org/10.1038/s41467-022-30034-y
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author Cao, Ang
Bukas, Vanessa J.
Shadravan, Vahid
Wang, Zhenbin
Li, Hao
Kibsgaard, Jakob
Chorkendorff, Ib
Nørskov, Jens K.
author_facet Cao, Ang
Bukas, Vanessa J.
Shadravan, Vahid
Wang, Zhenbin
Li, Hao
Kibsgaard, Jakob
Chorkendorff, Ib
Nørskov, Jens K.
author_sort Cao, Ang
collection PubMed
description The need for efficient ammonia synthesis is as urgent as ever. Over the past two decades, many attempts to find new catalysts for ammonia synthesis at mild conditions have been reported and, in particular, many new promoters of the catalytic rate have been introduced beyond the traditional K and Cs oxides. Herein, we provide an overview of recent experimental results for non-traditional promoters and develop a comprehensive model to explain how they work. The model has two components. First, we establish what is the most likely structure of the active sites in the presence of the different promoters. We then show that there are two effects dictating the catalytic activity. One is an electrostatic interaction between the adsorbed promoter and the N-N dissociation transition state. In addition, we identify a new promoter effect for magnetic catalysts giving rise to an anomalously large lowering of the activation energy opening the possibility of finding new ammonia synthesis catalysts.
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spelling pubmed-90617342022-05-04 A spin promotion effect in catalytic ammonia synthesis Cao, Ang Bukas, Vanessa J. Shadravan, Vahid Wang, Zhenbin Li, Hao Kibsgaard, Jakob Chorkendorff, Ib Nørskov, Jens K. Nat Commun Article The need for efficient ammonia synthesis is as urgent as ever. Over the past two decades, many attempts to find new catalysts for ammonia synthesis at mild conditions have been reported and, in particular, many new promoters of the catalytic rate have been introduced beyond the traditional K and Cs oxides. Herein, we provide an overview of recent experimental results for non-traditional promoters and develop a comprehensive model to explain how they work. The model has two components. First, we establish what is the most likely structure of the active sites in the presence of the different promoters. We then show that there are two effects dictating the catalytic activity. One is an electrostatic interaction between the adsorbed promoter and the N-N dissociation transition state. In addition, we identify a new promoter effect for magnetic catalysts giving rise to an anomalously large lowering of the activation energy opening the possibility of finding new ammonia synthesis catalysts. Nature Publishing Group UK 2022-05-02 /pmc/articles/PMC9061734/ /pubmed/35501341 http://dx.doi.org/10.1038/s41467-022-30034-y Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Cao, Ang
Bukas, Vanessa J.
Shadravan, Vahid
Wang, Zhenbin
Li, Hao
Kibsgaard, Jakob
Chorkendorff, Ib
Nørskov, Jens K.
A spin promotion effect in catalytic ammonia synthesis
title A spin promotion effect in catalytic ammonia synthesis
title_full A spin promotion effect in catalytic ammonia synthesis
title_fullStr A spin promotion effect in catalytic ammonia synthesis
title_full_unstemmed A spin promotion effect in catalytic ammonia synthesis
title_short A spin promotion effect in catalytic ammonia synthesis
title_sort spin promotion effect in catalytic ammonia synthesis
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9061734/
https://www.ncbi.nlm.nih.gov/pubmed/35501341
http://dx.doi.org/10.1038/s41467-022-30034-y
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