TY - JOUR

T1 - Coordination Polymers between 3,4-Dicyano-1,2,5-telluradiazole and N,N,N′,N′-Tetramethylethane-1,2-diamine: The Decisive Role of Chalcogen Bonding

AU - Pushkarevsky, Nikolay A.

AU - Smolentsev, Anton I.

AU - Wang, Hui

AU - Shishova, Valeriya E.

AU - Chulanova, Elena A.

AU - Wei, Qiaoyu

AU - Balmohammadi, Yaser

AU - Radiush, Ekaterina A.

AU - Grabowsky, Simon

AU - Beckmann, Jens

AU - Woollins, J. Derek

AU - Semenov, Nikolay A.

AU - Zibarev, Andrey V.

N1 - The authors are grateful to the Russian Science Foundation (project no. 21-73-10291) for financial support of this work. Its instrumental support at the Center of Collective Usage (Institute of Inorganic Chemistry) and Multi-Access Chemical Research Center (Institute of Organic Chemistry) is gratefully acknowledged.

PY - 2024

Y1 - 2024

N2 - One-dimensional coordination polymers [1·2]∞ (two polymorphs) and [12·2]∞ were obtained by cocrystallization of 3,4-dicyano-1,2,5-telluradiazole (1) and N,N,N′,N′-tetramethylethane-1,2-diamine (2). In the presence of Solv (C6H6, C5H5N, or C4H4S), differently colored, depending on the conditions, {[12·2]·Solv}∞ clathrates were isolated: products synthesized in the light were green, whereas those synthesized in the dark were yellow. In {[12·2]·Solv}∞, the Solv molecules occupy cavities formed by methyl groups of 2. With pyridazine, the 1·(1,2-C4H4N2)2 discrete complex was synthesized, and no clathrates/complexes were observed with pyrazine (1,4-C4H4N2) and pyrrole (C4H5N). In the compounds, 2 connects two 1 or 12 by Te···N chalcogen bonding (ChB), which is decisive for their formation according to quantum theory of atoms in molecules (QTAIM), NBO, and Hirshfeld surface analyses. The ChB features orbital contribution/polarization. The second-order perturbation energies are structure-dependent, and those for {[12·2]·Solv}∞ are slightly higher than those for [1·2]∞ and [12·2]∞. Time-dependent density functional theory (TD-DFT) calculations on the X-ray diffraction (XRD) unit cells of green {[12·2]·Solv}∞ do not reproduce their longest-wavelength absorption, which might indicate minor light-induced side products.

AB - One-dimensional coordination polymers [1·2]∞ (two polymorphs) and [12·2]∞ were obtained by cocrystallization of 3,4-dicyano-1,2,5-telluradiazole (1) and N,N,N′,N′-tetramethylethane-1,2-diamine (2). In the presence of Solv (C6H6, C5H5N, or C4H4S), differently colored, depending on the conditions, {[12·2]·Solv}∞ clathrates were isolated: products synthesized in the light were green, whereas those synthesized in the dark were yellow. In {[12·2]·Solv}∞, the Solv molecules occupy cavities formed by methyl groups of 2. With pyridazine, the 1·(1,2-C4H4N2)2 discrete complex was synthesized, and no clathrates/complexes were observed with pyrazine (1,4-C4H4N2) and pyrrole (C4H5N). In the compounds, 2 connects two 1 or 12 by Te···N chalcogen bonding (ChB), which is decisive for their formation according to quantum theory of atoms in molecules (QTAIM), NBO, and Hirshfeld surface analyses. The ChB features orbital contribution/polarization. The second-order perturbation energies are structure-dependent, and those for {[12·2]·Solv}∞ are slightly higher than those for [1·2]∞ and [12·2]∞. Time-dependent density functional theory (TD-DFT) calculations on the X-ray diffraction (XRD) unit cells of green {[12·2]·Solv}∞ do not reproduce their longest-wavelength absorption, which might indicate minor light-induced side products.

UR - https://www.scopus.com/record/display.uri?eid=2-s2.0-85195294818&origin=inward&txGid=69d121b6a8fd03826b70b99f46939ea6

UR - https://www.mendeley.com/catalogue/321652db-91b7-33ba-82c0-38550b34aae4/

U2 - 10.1021/acs.cgd.4c00475

DO - 10.1021/acs.cgd.4c00475

M3 - Article

VL - 24

SP - 5236

EP - 5250

JO - Crystal Growth and Design

JF - Crystal Growth and Design

SN - 1528-7483

IS - 12

ER -