NHC-Stabilized Au10 Nanoclusters and Their Conversion to Au25 Nanoclusters
Lummis, P. A., Osten, K. M., Levchenko, T. I., Sabooni Asre Hazer, M., Malola, S., Owens-Baird, B., Veinot, A. J., Albright, E. L., Schatte, G., Takano, S., Kovnir, K., Stamplecoskie, K. G., Tsukuda, T., Häkkinen, H., Nambo, M., & Crudden, C. M. (2022). NHC-Stabilized Au10 Nanoclusters and Their Conversion to Au25 Nanoclusters. JACS Au, 2(4), 875-885. https://doi.org/10.1021/jacsau.2c00004
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2022Copyright
© 2022 the Authors
Herein, we describe the synthesis of a toroidal Au10 cluster stabilized by N-heterocyclic carbene and halide ligands via reduction of the corresponding NHC−Au−X complexes (X = Cl, Br, I). The significant effect of the halide ligands on the formation, stability, and further conversions of these clusters is presented. While solutions of the chloride derivatives of Au10 show no change even upon heating, the bromide derivative readily undergoes conversion to form a biicosahedral Au25 cluster at room temperature. For the iodide derivative, the formation of a significant amount of Au25 was observed even upon the reduction of NHC−Au−I. The isolated bromide derivative of the Au25 cluster displays a relatively high (ca. 15%) photoluminescence quantum yield, attributed to the high rigidity of the cluster, which is enforced by multiple CH−π interactions within the molecular structure. Density functional theory computations are used to characterize the electronic structure and optical absorption of the Au10 cluster. 13C-Labeling is employed to assist with characterization of the products and to observe their conversions by NMR spectroscopy.
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The Natural Sciences and Engineering Research Council of Canada (NSERC) and the Canada Foundation for Innovation (CFI) are thanked for financial support of this work in terms of operating and equipment grants. K.M.O thanks JSPS for funding through the JSPS International Research Fellow program. T.I.L. thanks NSERC for a postdoctoral fellowship. A.J.V thanks NSERC for a Vanier Scholarship and also the Walter C. Sumner Foundation for a Walter C. Sumner Memorial Fellowship. E.L.A thanks NSERC CREATEMaterials for the Advanced Photonics and Sensing (MAPS) Program. This work was supported by KAKENHI from JSPS (17H03030 and 21H01949 to C.M.C.; 20H00370 to T.T.), JST CREST (JPMJCR20B2 to T. T.), and PRF (59632-ND3 to C.M.C). JSPS and NU are acknowledged for funding of this research through the World Premier International Research Centre Initiative (WPI) Program. K.K. is thankful to the National Science Foundation DMR-2003783 grant for support. The theory work was supported by the Academy of Finland (grants 294217, 319208, and HH’s Academy Professorship). The computations were made at the Jyväskylä node of the Finnish Grid and Cloud infrastructure (FGCI). ...License
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