Tuning Molecular Electron Affinities against Atomic Electronegativities by Spatial Expansion of a π-System

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В журнале  ChemPhysChem (IF 3,520) опубликована статья с участием сотрудников Института: к.х.н. Е.А. Чулановой (нс, ЛГетС), Е.А. Радюш (мнс, ЛГетС), к.х.н. Н.А. Семенова (зав.лаб. ЛГетС),  к.х.н. И.Г. Иртеговой (снс, ЛЭАСМ), Ю.С. Косенковой (инженер ЛГетС), д.х.н. И.Ю. Багрянской (рук. ГРСА), д.х.н.  Л.А. Шурдрина (зав. лаб. ЛЭАСМ) и д.х.н. А.В. Зибарева (гнс, ЛГетС):

Tuning Molecular Electron Affinities against Atomic Electronegativities by Spatial Expansion of a π-System

Elena A. Chulanova, Ekaterina A. Radiush, Nikolay A. Semenov, Emanuel Hupf, Irina G. Irtegova, Yulia S. Kosenkova, Irina Yu. Bagryanskaya, Leonid A Shundrin, Jens Beckmann, Andrey V. Zibarev  


ChemPhysChem,  Volume 24, Issue 9, May 2, 2023, e202200876

 https://doi.org/10.1002/cphc.202200876

Abstract

With 2,1,3-benzochalcogenadiazoles C6R4N2E (E/R; E = S, Se, Te; R = H, F, Cl, Br, I) and C6H2R2N2E (E/R’; E = S, Se, Te; R = Br, I) – 10π-electron hetarenes, it is shown by CV / EPR measurements, DFT calculations, and QTAIM and ELI-D analyses that their molecular electron affinities (EAs) increase with decreasing Allen electronegativities and electron affinities of the E and non-hydrogen R (except Cl) atoms. DFT calculations for E/R + e·– → [E/R]·– electron capture reveal negative ΔG values numerically increasing with increasing atomic numbers of the E and R atoms; positive ΔS has a minor influence. It is suggested that the increased EAs are caused by more effective charge / spin delocalization in the radical anions of heavier derivatives due to contributions from diffuse (a real-space expanded) p-AOs of the heavier E and R atoms; and that this counterintuitive effect might be of the general character.

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