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Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia

It is vital to design effective nitrogen fixation systems that operate under mild conditions, and to this end we recently reported an example of the catalytic formation of ammonia using a dinitrogen-bridged dimolybdenum complex bearing a pincer ligand, where up to twenty three equivalents of ammonia...

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Autores principales: Tanaka, Hiromasa, Arashiba, Kazuya, Kuriyama, Shogo, Sasada, Akira, Nakajima, Kazunari, Yoshizawa, Kazunari, Nishibayashi, Yoshiaki
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2014
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4015321/
https://www.ncbi.nlm.nih.gov/pubmed/24769530
http://dx.doi.org/10.1038/ncomms4737
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author Tanaka, Hiromasa
Arashiba, Kazuya
Kuriyama, Shogo
Sasada, Akira
Nakajima, Kazunari
Yoshizawa, Kazunari
Nishibayashi, Yoshiaki
author_facet Tanaka, Hiromasa
Arashiba, Kazuya
Kuriyama, Shogo
Sasada, Akira
Nakajima, Kazunari
Yoshizawa, Kazunari
Nishibayashi, Yoshiaki
author_sort Tanaka, Hiromasa
collection PubMed
description It is vital to design effective nitrogen fixation systems that operate under mild conditions, and to this end we recently reported an example of the catalytic formation of ammonia using a dinitrogen-bridged dimolybdenum complex bearing a pincer ligand, where up to twenty three equivalents of ammonia were produced based on the catalyst. Here we study the origin of the catalytic behaviour of the dinitrogen-bridged dimolybdenum complex bearing the pincer ligand with density functional theory calculations, based on stoichiometric and catalytic formation of ammonia from molecular dinitrogen under ambient conditions. Comparison of di- and mono-molybdenum systems shows that the dinitrogen-bridged dimolybdenum core structure plays a critical role in the protonation of the coordinated molecular dinitrogen in the catalytic cycle.
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spelling pubmed-40153212014-05-13 Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia Tanaka, Hiromasa Arashiba, Kazuya Kuriyama, Shogo Sasada, Akira Nakajima, Kazunari Yoshizawa, Kazunari Nishibayashi, Yoshiaki Nat Commun Article It is vital to design effective nitrogen fixation systems that operate under mild conditions, and to this end we recently reported an example of the catalytic formation of ammonia using a dinitrogen-bridged dimolybdenum complex bearing a pincer ligand, where up to twenty three equivalents of ammonia were produced based on the catalyst. Here we study the origin of the catalytic behaviour of the dinitrogen-bridged dimolybdenum complex bearing the pincer ligand with density functional theory calculations, based on stoichiometric and catalytic formation of ammonia from molecular dinitrogen under ambient conditions. Comparison of di- and mono-molybdenum systems shows that the dinitrogen-bridged dimolybdenum core structure plays a critical role in the protonation of the coordinated molecular dinitrogen in the catalytic cycle. Nature Pub. Group 2014-04-28 /pmc/articles/PMC4015321/ /pubmed/24769530 http://dx.doi.org/10.1038/ncomms4737 Text en Copyright © 2014, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by-nc-by/3.0/ This work is licensed under a Creative Commons Attribution 3.0 Unported License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/3.0/
spellingShingle Article
Tanaka, Hiromasa
Arashiba, Kazuya
Kuriyama, Shogo
Sasada, Akira
Nakajima, Kazunari
Yoshizawa, Kazunari
Nishibayashi, Yoshiaki
Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title_full Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title_fullStr Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title_full_unstemmed Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title_short Unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
title_sort unique behaviour of dinitrogen-bridged dimolybdenum complexes bearing pincer ligand towards catalytic formation of ammonia
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4015321/
https://www.ncbi.nlm.nih.gov/pubmed/24769530
http://dx.doi.org/10.1038/ncomms4737
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