Monocarboxylate-protected two-electron superatomic silver nanoclusters with high photothermal conversion performance - Archive ouverte HAL
Article Dans Une Revue Nanoscale Année : 2023

Monocarboxylate-protected two-electron superatomic silver nanoclusters with high photothermal conversion performance

Résumé

The first series of monocarboxylate-protected superatomic silver nanoclusters was synthesized and fully characterized by X-ray diffraction, fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and electrospray ionization mass spectrometry (ESI-MS). Specifically, compounds [Ag(16)(L)(8)(9-AnCO(2))(12)](2+) (L = Ph(3)P (I), (4-ClPh)(3)P (II), (2-furyl)(3)P (III), and Ph(3)As (IV)) were prepared by a solvent-thermal method under alkaline conditions. These clusters exhibit a similar unprecedented structure containing a [Ag(8)@Ag(8)](6+) metal kernel, of which the 2-electron superatomic [Ag(8)](6+) inner core shows a flattened and puckered hexagonal bipyramid of S(6) symmetry. Density functional theory calculations provide a rationalization of the structure and stability of these 2-electron superatoms. Results indicate that the 2 superatomic electrons occupy a superatomic molecular orbital 1S that has a substantial localization on the top and bottom vertices of the bipyramid. The π systems of the anthracenyl groups, as well as the 1S HOMO, are significantly involved in the optical and photothermal behavior of the clusters. The four characterized nanoclusters show high photothermal conversion performance in sunlight. These results show that the unprecedented use of mono-carboxylates in the stabilization of Ag nanoclusters is possible, opening the door for the introduction of various functional groups on their cluster surface.

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Cristallographie
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Dates et versions

hal-04088945 , version 1 (11-05-2023)

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Hao-Hai Wang, Jianyu Wei, Fahime Bigdeli, Farzaneh Rouhani, Hai-Feng Su, et al.. Monocarboxylate-protected two-electron superatomic silver nanoclusters with high photothermal conversion performance. Nanoscale, 2023, 15 (18), pp.8245-8254. ⟨10.1039/d3nr00571b⟩. ⟨hal-04088945⟩
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