Structural Evolution of Atomically Precise Thiolated Bimetallic [Au<sub>12+<i>n</i></sub>Cu<sub>32</sub>(SR)<sub>30+<i>n</i></sub>]<sup>4–</sup> (<i>n</i> = 0, 2, 4, 6) Nanoclusters
Créateur:
HuaYu JuaXi
Hôte:
A series
of all-thiol stabilized bimetallic Au–Cu nanoclusters,
[Au12+nCu32(SR)30+n]4– (n = 0, 2,
4, 6 and SR = SPhCF3), are successfully synthesized and
characterized by X-ray single-crystal analysis and density functional
theory (DFT) calculations. Each cluster consists of a Keplerate two-shell
Au12@Cu20 core protected by (6 – n) units of Cu2(SR)5 and n units of Cu2Au(SR)6 (n =
0, 2, 4, 6) motifs on its surface. The size and structural evolution
of the clusters is atomically controlled by the Au precursors and
countercations used in the syntheses. The clusters exhibit similar
optical absorption properties that are not dependent on the number
of surface Cu2Au(SR)6 units. Although DFT suggests
an electronic structure with an 18-electron superatom shell closure,
the clusters display different thermal stabilities. [Au12+nCu32(SR)30+n]4– clusters with n = 0 and 2
are more stable than those with n = 4 and 6. Moreover,
an oxidation product of the clusters, [Au13Cu12(SR)20]4–, is structurally identified
to gain insight into how the clusters are oxidized.
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