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Issue 44, 2019
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Selectivity of tungsten mediated dinitrogen splitting vs. proton reduction

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Abstract

Mo complexes are currently the most active catalysts for nitrogen fixation under ambient conditions. In comparison, tungsten platforms are scarcely examined. For active catalysts, the control of N2vs. proton reduction selectivities remains a difficult task. We here present N2 splitting using a tungsten pincer platform, which has been proposed as the key reaction for catalytic nitrogen fixation. Starting from [WCl3(PNP)] (PNP = N(CH2CH2PtBu2)2), the activation of N2 enabled the isolation of the dinitrogen bridged redox series [(N2){WCl(PNP)}2]0/+/2+. Protonation of the neutral complex results either in the formation of a nitride [W(N)Cl(HPNP)]+ or H2 evolution and oxidation of the W2N2 core, respectively, depending on the acid and reaction conditions. Examination of the nitrogen splitting vs. proton reduction selectivity emphasizes the role of hydrogen bonding of the conjugate base with the protonated intermediates and provides guidelines for nitrogen fixation.

Graphical abstract: Selectivity of tungsten mediated dinitrogen splitting vs. proton reduction

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Supplementary files

Article information


Submitted
30 Jul 2019
Accepted
19 Sep 2019
First published
24 Sep 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 10275-10282
Article type
Edge Article

Selectivity of tungsten mediated dinitrogen splitting vs. proton reduction

B. Schluschaß, J. Abbenseth, S. Demeshko, M. Finger, A. Franke, C. Herwig, C. Würtele, I. Ivanovic-Burmazovic, C. Limberg, J. Telser and S. Schneider, Chem. Sci., 2019, 10, 10275
DOI: 10.1039/C9SC03779A

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