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Structural transformation and catalytic hydrogenation activity of amidinate-protected copper hydride clusters
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Structural transformation and catalytic hydrogenation activity of amidinate-protected copper hydride clusters
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Structural transformation and catalytic hydrogenation activity of amidinate-protected copper hydride clusters
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Journal Article
Structural transformation and catalytic hydrogenation activity of amidinate-protected copper hydride clusters
2022
Overview
Copper hydrides are important hydrogenation catalysts, but their poor stability hinders the practical applications. Ligand engineering is an effective strategy to tackle this issue. An amidinate ligand, N,N′-Di(5-trifluoromethyl-2-pyridyl)formamidinate (Tf-dpf) with four N-donors has been applied as a protecting agent in the synthesis of stable copper hydride clusters: Cu
11
H
3
(Tf-dpf)
6
(OAc)
2
(
Cu
11
) with three interfacial
μ
5
-H and [Cu
12
H
3
(Tf-dpf)
6
(OAc)
2
]·OAc (
Cu
12
) with three interstitial
μ
6
-H. A solvent-triggered reversible interconversion between
Cu
11
and
Cu
12
has been observed thanks to the flexibility of Tf-dpf.
Cu
11
shows high activity in the reduction of 4-nitrophenol to 4-aminophenol, while
Cu
12
displays very low activity. Deuteration experiments prove that the type of hydride is the key in dictating the catalytic activity, for the interfacial
μ
5
-H species in
Cu
11
are involved in the catalytic cycle whereas the interstitial
μ
6
-H species in
Cu
12
are not. This work highlights the role of hydrides with regard to catalytic hydrogenation activity.
Copper hydrides have been studied for their exciting structural chemistry and applications in hydrogenation catalysis. Here, the authors uncover the role of the amidinate ligand in yielding two closely related copper hydride clusters with quite different catalytic hydrogenation activity.
