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非常温常压下阴离子自由基多中心双电子键的电荷密度研究。

Charge density studies of multicentre two-electron bonding of an anion radical at non-ambient temperature and pressure.

作者信息

Milašinović Valentina, Molčanov Krešimir, Krawczuk Anna, Bogdanov Nikita E, Zakharov Boris A, Boldyreva Elena V, Jelsch Christian, Kojić-Prodić Biserka

机构信息

Department of Physical Chemistry, Rudjer Bošković Institute, Bijenička 54, Zagreb 10000, Croatia.

Institute of Inorganic Chemistry, University of Göttingen, Tammannstrasse 4, Göttingen 37077, Germany.

出版信息

IUCrJ. 2021 Jun 12;8(Pt 4):644-654. doi: 10.1107/S2052252521005273. eCollection 2021 Jul 1.

DOI:10.1107/S2052252521005273
PMID:34258012
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8256703/
Abstract

The variation of charge density of two-electron multicentre bonding (pancake bonding) between semi-quinone radicals with pressure and temperature was studied on a salt of 5,6-di-chloro-2,3-di-cyano-semi-quinone radical anion (DDQ) with 4-cyano--methyl-pyridinium cation (4-CN) using the Transferable Aspheric Atom Model (TAAM) refinement. The pancake-bonded radical dimers are stacked by non-bonding π-interactions. With rising pressure, the covalent character of interactions between radicals increases, and above 2.55 GPa, the electron density indicates multicentric covalent interactions throughout the stack. The experimental charge densities were verified and corroborated by periodic DFT computations. The TAAM approach has been tested and validated for atomic resolution data measured at ambient pressure; this work shows this approach can also be applied to diffraction data obtained at pressures up to several gigapascals.

摘要

利用可转移非球形原子模型（TAAM）精修方法，研究了5,6-二氯-2,3-二氰基半醌自由基阴离子（DDQ）与4-氰基甲基吡啶鎓阳离子（4-CN）形成的盐中，半醌自由基之间双电子多中心键合（薄饼状键合）的电荷密度随压力和温度的变化。薄饼状键合的自由基二聚体通过非键π相互作用堆叠。随着压力升高，自由基间相互作用的共价特性增强，在2.55 GPa以上，电子密度表明整个堆叠中存在多中心共价相互作用。周期性密度泛函理论（DFT）计算验证并证实了实验电荷密度。TAAM方法已针对在常压下测量的原子分辨率数据进行了测试和验证；这项工作表明该方法也可应用于高达几吉帕压力下获得的衍射数据。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/f1973f34d1b9/m-08-00644-fig16.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/f1973f34d1b9/m-08-00644-fig16.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/8e11f77d457c/m-08-00644-fig1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/442236b58055/m-08-00644-fig2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/e903c43cc23a/m-08-00644-fig3.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/4cea292f6f79/m-08-00644-fig8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/aa9d1cc883a8/m-08-00644-fig9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/cf4efe99eced/m-08-00644-fig10.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/20d58388f3aa/m-08-00644-fig11.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/cb5714b754f2/m-08-00644-fig12.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/13af02b6c997/m-08-00644-fig13.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/71ed/8256703/f1973f34d1b9/m-08-00644-fig16.jpg

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