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Missing Link in the Growth of Lead-Based Zintl Clusters: Isolation of the Dimeric Plumbaspherene [Cu4Pb22]4.

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We report here the structure of an endohedral plumbaspherene, [Cu4Pb22]4-, the gold analogue of which was previously postulated to be a "missing link" in the growth of larger clusters containing… Click to show full abstract

We report here the structure of an endohedral plumbaspherene, [Cu4Pb22]4-, the gold analogue of which was previously postulated to be a "missing link" in the growth of larger clusters containing three and four icosahedral subunits. The cluster contains two [Cu2Pb11]2- subunits linked through a Cu2Pb4 trigonal antiprism. Density functional theory reveals that the striking ability of mixed Pb/coinage metal Zintl clusters to oligomerize and, in the case of Au, to act as a site of nucleation for additional metal atoms, is a direct consequence of their nd10(n + 1)s0 configuration, which generates both a low-lying (n + 1)s-based LUMO and also a high-lying Pb-centered HOMO. Cluster growth and nucleation is then driven by this amphoteric character, allowing the clusters to form donor-acceptor interactions between adjacent icosahedral units or to additional metal atoms.

Keywords: growth; link growth; plumbaspherene cu4pb22; missing link; zintl clusters

Journal Title: Journal of the American Chemical Society
Year Published: 2022

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