Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 41, Pages 22293-22300Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202106311
Keywords
doping; hydrides; rhodium; silver nanoclusters; superatoms
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Funding
- National Research Foundation of Korea (NRF) [NRF-2017R1A2B3006651]
- NRF - Ministry of Science and ICT, Republic of Korea [2020M3H7A1096344]
- NRF [NRF-2020R1A2C2007468]
- MSIT
- Pohang Accelerator Laboratory (PAL), Korea
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The study presents the first synthesis of a [RhHAg24(SPhMe2)18]2- nanocluster, incorporating a Rh atom as a dopant, and demonstrates that a superatom can be incorporated into a cluster superatom to generate a stable nanocluster.
Heterometal doping is a powerful method for tuning the physicochemical properties of metal nanoclusters. While the heterometals doped into such nanoclusters predominantly include transition metals with closed d-shells, the doping of open d-shell metals remains largely unexplored. Herein, we report the first synthesis of a [RhHAg24(SPhMe2)(18)](2-) nanocluster, in which a Rh atom with open d-shells ([Kr]4d(8)5s(1)) is incorporated into the Ag-24 framework by forming a RhH superatom with closed d-shells ([Kr]4d(10)). Combined experimental and theoretical investigations showed that the Ag-24 framework was co-doped with Rh and hydride and that the RhH dopant was a superatomic construct of a Pd atom. Additional studies demonstrated that the [RhHAg24(SPhMe2)(18)](2-) nanocluster was isoelectronic to the [PdAg24(SPhMe2)(18)](2-) nanocluster with the superatomic 8-electron configuration (1S(2)1P(6)). This study demonstrated for the first time that a superatom could be incorporated into a cluster superatom to generate a stable superatom-in-superatom nanocluster.
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