Abstract
We report a new strategy that provides stringent control for the size and dispersity of ultrasmall nanoclusters through preparation of gold complex distributions formed from the precursor, AuClPPh3 (PPh3 = triphenylphosphine), and the L6 (L6 = 1,6-bis(diphenylphosphino) hexane) ligand prior to reduction with NaBH4 in 1:1 methanol/chloroform solutions. Monodisperse nanoclusters of distinct nuclearity are obtained for specific ligand ratios; [L6]/[PPh3] = 4 yields [Au8L64]2+, [L6]/[PPh3] = 0.4 yields [Au9L64Cl]2+, and [L6]/[PPh3] = 8 yields ligated Au10 cores in the form of [Au10L64]2+ and [Au10L65]2+. Polyhedral skeletal electron pair theory accounts for the stability of [Au9L64Cl]2+, which is the smallest closed-shell chlorinated cluster reported. Electrospray mass spectrometry and UV−vis spectra indicate that [Au9L64Cl]2+ and [Au10L6x]2+ (x = 4, 5) result from reactions involving [Au8L64]2+. Syntheses of small gold clusters containing chloride ligands open the possibility of constructing larger clusters via ligand exchange.
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