Control of Intermediates and Products by Combining Droplet Reactions and Ion Soft-Landing.

Autor: Yang F; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany., Urban RD; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany., Lorenz J; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany., Griebel J; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany., Koohbor N; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany., Rohdenburg M; Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry, University Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany., Knorke H; Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry, University Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany., Fuhrmann D; Institute for Inorganic Chemistry, University Leipzig, Johannisallee 29, 04103, Leipzig, Germany., Charvat A; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany.; Institute of Chemical Technology, University Leipzig, 04103, Leipzig, Germany., Abel B; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany.; Institute of Chemical Technology, University Leipzig, 04103, Leipzig, Germany., Azov VA; Department of Chemistry, University of the Free State, 9300, Bloemfontein, South Africa., Warneke J; Leibniz Institute of Surface Engineering (IOM), Permoserstrasse 15, 04318, Leipzig, Germany.; Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry, University Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Jan 22; Vol. 63 (4), pp. e202314784. Date of Electronic Publication: 2023 Dec 11.
DOI: 10.1002/anie.202314784
Abstrakt: Despite being recognized primarily as an analytical technique, mass spectrometry also has a large potential as a synthetic tool, enabling access to advanced synthetic routes by reactions in charged microdroplets or ionic thin layers. Such reactions are special and proceed primarily at surfaces of droplets and thin layers. Partial solvation of the reactants is usually considered to play an important role for reducing the activation barrier, but many mechanistic details still need to be clarified. In our study, we showcase the synergy between two sequentially applied "preparative mass spectrometry" methods: initiating accelerated reactions within microdroplets during electrospray ionization to generate gaseous ionic intermediates in high abundance, which are subsequently mass-selected and soft-landed to react with a provided reagent on a substrate. This allows the generation of products at a nanomolar scale, amenable to further characterization. In this proof-of-concept study, the contrasting reaction pathways between intrinsically neutral and pre-charged reagents, respectively, both in microdroplets and in layers generated by ion soft-landing are investigated. This provides new insights into the role of partially solvated reagents at microdroplet surfaces for increased reaction rates. Additionally, further insights into reactions of ions of the same polarity under various conditions is obtained.
(© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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