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Nitrogen reduction by the Fe sites of synthetic Mo3S4Fe cubes
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Journal Article
Nitrogen reduction by the Fe sites of synthetic Mo3S4Fe cubes
2022
Overview
Nitrogen (N
2
) fixation by nature, which is a crucial process for the supply of bio-available forms of nitrogen, is performed by nitrogenase. This enzyme uses a unique transition-metal–sulfur–carbon cluster as its active-site co-factor ([(
R
-homocitrate)MoFe
7
S
9
C], FeMoco)
1
,
2
, and the sulfur-surrounded iron (Fe) atoms have been postulated to capture and reduce N
2
(refs.
3
–
6
). Although there are a few examples of synthetic counterparts of the FeMoco, metal–sulfur cluster, which have shown binding of N
2
(refs.
7
–
9
), the reduction of N
2
by any synthetic metal–sulfur cluster or by the extracted form of FeMoco
10
has remained elusive, despite nearly 50 years of research. Here we show that the Fe atoms in our synthetic [Mo
3
S
4
Fe] cubes
11
,
12
can capture a N
2
molecule and catalyse N
2
silylation to form N(SiMe
3
)
3
under treatment with excess sodium and trimethylsilyl chloride. These results exemplify the catalytic silylation of N
2
by a synthetic metal–sulfur cluster and demonstrate the N
2
-reduction capability of Fe atoms in a sulfur-rich environment, which is reminiscent of the ability of FeMoco to bind and activate N
2
.
Iron atoms in a synthetic metal–sulfur cluster can capture nitrogen and catalyse its silylation, demonstrating successful nitrogen reduction by iron atoms in a sulfur-rich environment.
