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Elucidating the Structures of Intermediate Fragments during Stepwise Dissociation of Monolayer‐Protected Silver Clusters

Chakraborty, Papri 1,2; Malola, Sami; Neumaier, Marco ORCID iD icon 2; Weis, Patrick 1; Häkkinen, Hannu; Kappes, Manfred M. 1,2
1 Institut für Physikalische Chemie (IPC), Karlsruher Institut für Technologie (KIT)
2 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)

Abstract:

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 [Ag$_{29}$L$_{12}$]$^{3−}$, i.e. [Ag$_{24}$L$_9$]$^{2−}$, [Ag$_{19}$L$_6$]$^−$ and [Ag$_5$L$_3$]$^−$ (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 [Ag$_5$L$_3$]$^−$ elimination steps, further dissociation of [Ag$_{19}$L$_6$]$^−$ also involves a new channel of Ag$_2$ loss and Ag−S and C−S bond cleavages. This reflects a competition between retaining the electronic stability of 8 e$^−$ 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.


Verlagsausgabe §
DOI: 10.5445/IR/1000160357
Veröffentlicht am 10.07.2023
Originalveröffentlichung
DOI: 10.1002/anie.202305836
Scopus
Zitationen: 6
Web of Science
Zitationen: 3
Dimensions
Zitationen: 5
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Institut für Physikalische Chemie (IPC)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 1433-7851, 1521-3773
KITopen-ID: 1000160357
HGF-Programm 43.31.01 (POF IV, LK 01) Multifunctionality Molecular Design & Material Architecture
Erschienen in Angewandte Chemie International Edition
Verlag John Wiley and Sons
Band 62
Heft 29
Seiten Art.Nr.: e202305836
Vorab online veröffentlicht am 12.06.2023
Schlagwörter Fragment Structures, Ion Mobility, Ligand-Protected Clusters, Mass Spectrometry. Silver Clusters
Nachgewiesen in Scopus
Web of Science
Dimensions
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