期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 45, 页码 15404-15409出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201301234
关键词
electron affinity; fullerenes; photoelectron spectroscopy; radicals; superhalogen
资金
- US NSF [CHE-1012468]
- NIH [5R21A140080-03]
- Colorado State University Research Foundation
- US Department of Energy (DOE), Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences
- DOE's Office of Biological and Environmental Research
- DFG [PO1602/1-1]
Hexasubstituted fullerenes with the skew pentagonal pyramid (SPP) addition pattern are predominantly formed in many types of reactions and represent important and versatile building blocks for supramolecular chemistry, biomedical and optoelectronic applications. Regioselective synthesis and characterization of the new SPP derivative, C-60(CF3)(4)(CN)H, in this work led to the experimental identification of the new family of superhalogen fullerene radicals, species with the gas-phase electron affinity higher than that of the most electronegative halogens, F and Cl. Low-temperature photoelectron spectroscopy and DFT studies of different C60X5 radicals reveal a profound effect of X groups on their electron affinities (EA), which vary from 2.76eV (X=CH3) to 4.47eV (X=CN). The measured gas-phase EA of the newly synthesized C-60(CF3)(4)CN equals 4.28(1)eV, which is about 1eV higher than the EA of Cl atom. An observed remarkable stability of C-60(CF3)(4)CN- in solution under ambient conditions opens new venues for design of air-stable molecular complexes and salts for supramolecular structures of electroactive functional materials.
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