期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 116, 期 17, 页码 8167-8172出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1820812116
关键词
superelectrophilic anions; multiple-charged anions; Ar compounds; photoelectron spectroscopy; dodecaborates
资金
- Fritz-Haber-Institute of the Max-Planck-Society
- German Research Foundation for an Emmy Noether Fellowship [GR 4451/1-1]
- Center for Scalable Predictive Methods for Excitations and Correlated Phenomena (SPEC) - US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, Computational Chemical Sciences Progr
- US DOE, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences at PNNL
- Office of Science of the US DOE [DE-AC02-05CH11231]
- Office of Biological and Environmental Research
- Alexander von Humboldt Foundation
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 [B-12(CN)(12)](2-) the electronically most stable dianion ever investigated experimentally. It serves as a precursor for the generation of the monoanion [B-12(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.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据