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Selective catalytic reduction of N2 to N2H4 by a simple Fe complex

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Title: Selective catalytic reduction of N2 to N2H4 by a simple Fe complex
Authors: Hill, PJ
Doyle, LR
Crawford, AD
Myers, WK
Ashley, AE
Item Type: Journal Article
Abstract: The catalytic fixation of N2 by molecular Fe compounds is a rapidly developing field, yet thus far few complexes can effect this transformation, and none are selective for N2H4 production. Herein we report that the simple Fe(0) complex Fe(Et2PCH2CH2PEt2)2(N2) (1) is an efficient catalyst for the selective conversion of N2 (> 25 molecules N2 fixed) into N2H4, attendant with the production of ca. one molecule of NH3. Notably, the reductant (CoCp*2) and acid (Ph2NH2OTf) used are considerably weaker than conventional chemical H+ and e– sources used in previous demonstrations of N2 turnover by synthetic Fe compounds. These results show that the direct catalytic conversion of N2 to the hydrazine oxidation state on molecular Fe complexes is viable, and indicates that the mechanism of NH3 formation by such systems may proceed via Fe-N2H4 intermediates.
Issue Date: 4-Oct-2016
Date of Acceptance: 4-Oct-2016
URI: http://hdl.handle.net/10044/1/41174
DOI: 10.1021/jacs.6b08802
ISSN: 1520-5126
Publisher: American Chemical Society
Start Page: 13521
End Page: 13524
Journal / Book Title: Journal of the American Chemical Society
Volume: 138
Issue: 41
Copyright Statement: This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Sponsor/Funder: The Royal Society
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (EPSRC)
Funder's Grant Number: UF110061
EP/K503733/1
EP/K030760/1
Keywords: Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
DINITROGEN
AMMONIA
HYDRAZINE
NITROGEN
MOLYBDENUM
CONVERSION
General Chemistry
03 Chemical Sciences
Publication Status: Published
Online Publication Date: 2016-10-11
Appears in Collections:Chemistry
Faculty of Natural Sciences