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

Abstract:

: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.

journal_name

Nat Commun

journal_title

Nature communications

authors

Tanaka H,Arashiba K,Kuriyama S,Sasada A,Nakajima K,Yoshizawa K,Nishibayashi Y

doi

10.1038/ncomms4737

subject

Has Abstract

pub_date

2014-04-28 00:00:00

pages

3737

issn

2041-1723

pii

ncomms4737

journal_volume

5

pub_type

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