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

Author:

Chakraborty Papri12ORCID,Malola Sami3,Neumaier Marco1,Weis Patrick2,Häkkinen Hannu34,Kappes Manfred M.12ORCID

Affiliation:

1. Institute of Nanotechnology Karlsruhe Institute of Technology 76344 Eggenstein-Leopoldshafen Germany

2. Institute of Physical Chemistry Karlsruhe Institute of Technology 76131 Karlsruhe Germany

3. Department of Physics, Nanoscience Center University of Jyväskylä 40014 Jyväskylä Finland

4. Department of Chemistry, Nanoscience Center University of Jyväskylä 40014 Jyväskylä Finland

Abstract

AbstractFragmentation 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 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.

Funder

Alexander von Humboldt-Stiftung

Academy of Finland

Publisher

Wiley

Subject

General Chemistry,Catalysis

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