Elucidating the Structures of Intermediate Fragments during Stepwise Dissociation of Monolayer‐Protected Silver Clusters
Chakraborty, P., Malola, S., Neumaier, M., Weis, P., Häkkinen, H., & Kappes, M. M. (2023). Elucidating the Structures of Intermediate Fragments during Stepwise Dissociation of Monolayer‐Protected Silver Clusters. Angewandte Chemie, 62(29), Article e202305836. https://doi.org/10.1002/anie.202305836
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Angewandte ChemieAuthors
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2023Copyright
© 2023 the Authors
Fragmentation dynamics of ligated coinage metal clusters reflects their structural and bonding properties. So far methodological challenges limited probing structures of the fragments. Herein, we resolve the geometric structures of the primary fragments of [Ag29L12]3-, i.e. [Ag24L9]2-, [Ag19L6]- and [Ag5L3]- (L is 1,3-benzene dithiolate). For this, we used trapped ion mobility mass spectrometry to determine collision cross sections of the fragments and compared them to structures calculated by density functional theory. We also report that following two sequential [Ag5L3]- elimination steps, further dissociation of [Ag19L6]- also involves a new channel of Ag2 loss and Ag-S and C-S bond cleavages. This reflects a competition between retaining the electronic stability of 8e- superatom cluster cores and increasing steric strain of ligands and staples. These results are also of potential interest for future soft-landing deposition studies aimed at probing catalytic behavior of Ag clusters on supports.
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This research was supported by DFG under CRC 1441 TrackAct, Project A2. P.C. gratefully acknowledges postdoctoral fellowship support by the Alexander von Humboldt Foundation. H.H. acknowledges support by the Academy of Finland under grant 315549.License
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