Single-gold etching at the hypercarbon atom of C-centred hexagold(I) clusters protected by chiral N-heterocyclic carbenes

Xiao-Li Pei, Pei Zhao, Hitoshi Ube, Zhen Lei, Masahiro Ehara () and Mitsuhiko Shionoya ()
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Xiao-Li Pei: The University of Tokyo
Pei Zhao: Myodaiji
Hitoshi Ube: The University of Tokyo
Zhen Lei: The University of Tokyo
Masahiro Ehara: Myodaiji
Mitsuhiko Shionoya: The University of Tokyo

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Chemical etching of nano-sized metal clusters at the atomic level has a high potential for creating metal number-specific structures and functions that are difficult to achieve with bottom-up synthesis methods. In particular, precisely etching metal atoms one by one from nonmetallic element-centred metal clusters and elucidating the relationship between their well-defined structures, and chemical and physical properties will facilitate future materials design for metal clusters. Here we report the single-gold etching at a hypercarbon centre in gold(I) clusters. Specifically, C-centred hexagold(I) clusters protected by chiral N-heterocyclic carbenes are etched with bisphosphine to yield C-centred pentagold(I) (CAuI5) clusters. The CAuI5 clusters exhibit an unusually large bathochromic shift in luminescence, which is reproduced theoretically. The etching mechanism is experimentally and theoretically suggested to be a tandem dissociation-association-elimination pathway. Furthermore, the vacant site of the central carbon of the CAuI5 cluster can accommodate AuCl, allowing for post-functionalisation of the C-centred gold(I) clusters.

Date: 2024
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DOI: 10.1038/s41467-024-49295-w

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