Intermetallic Competition in the Fragmentation of Trimetallic Au-Zn-Alkali Complexes

Chemistry : a European Journal
Johannes LangGereon Niedner-Schatteburg

Abstract

Cationization is a valuable tool to enable mass spectrometric studies on neutral transition-metal complexes (e.g., homogenous catalysts). However, knowledge of potential impacts on the molecular structure and catalytic reactivity induced by the cationization is indispensable to extract information about the neutral complex. In this study, we cationize a bimetallic complex [AuZnCl3 ] with alkali metal ions (M(+) ) and investigate the charged adducts [AuZnCl3 M](+) by electrospray ionization mass spectrometry (ESI-MS). Infrared multiple photon dissociation (IR-MPD) in combination with density functional theory (DFT) calculations reveal a μ(3) binding motif of all alkali ions to the three chlorido ligands. The cationization induces a reorientation of the organic backbone. Collision-induced dissociation (CID) studies reveal switches of fragmentation channels by the alkali ion and by the CID amplitude. The Li(+) and Na(+) adducts prefer the sole loss of ZnCl2 , whereas the K(+) , Rb(+) , and Cs(+) adducts preferably split off MCl2 ZnCl. Calculated energetics along the fragmentation coordinate profiles allow us to interpret the experimental findings to a level of subtle details. The Zn(2+) cation wins the competition for the nitrogen...Continue Reading

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Citations

Jun 8, 2018·Physical Chemistry Chemical Physics : PCCP·Johannes LangGereon Niedner-Schatteburg
Jan 30, 2018·Chemistry : a European Journal·Christoph KaubPeter W Roesky
Oct 13, 2021·Chemistry : a European Journal·Gereon Niedner-Schatteburg, Manfred M Kappes

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