Rational design of an argon-binding superelectrophilic anion

Author:

Mayer MartinORCID,van Lessen Valentin,Rohdenburg MarkusORCID,Hou Gao-LeiORCID,Yang ZhengORCID,Exner Rüdiger M.,Aprà EdoardoORCID,Azov Vladimir A.ORCID,Grabowsky SimonORCID,Xantheas Sotiris S.ORCID,Asmis Knut R.ORCID,Wang Xue-BinORCID,Jenne CarstenORCID,Warneke JonasORCID

Abstract

Chemically binding to argon (Ar) at room temperature has remained the privilege of the most reactive electrophiles, all of which are cationic (or even dicationic) in nature. Herein, we report a concept for the rational design of anionic superelectrophiles that are composed of a strong electrophilic center firmly embedded in a negatively charged framework of exceptional stability. To validate our concept, we synthesized the percyano-dodecoborate [B12(CN)12]2−, the electronically most stable dianion ever investigated experimentally. It serves as a precursor for the generation of the monoanion [B12(CN)11], which indeed spontaneously binds Ar at 298 K. Our mass spectrometric and spectroscopic studies are accompanied by high-level computational investigations including a bonding analysis of the exceptional B-Ar bond. The detection and characterization of this highly reactive, structurally stable anionic superelectrophile starts another chapter in the metal-free activation of particularly inert compounds and elements.

Funder

Deutsche Forschungsgemeinschaft

U.S. Department of Energy

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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