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Sorption and Magnetic Properties of Oxalato-Based Trimetallic Open Framework Stabilized by Charge-Assisted Hydrogen Bonds

1
Faculty of Chemistry, Nicolaus Copernicus University in Toruń, Gagarina 7, 87-100 Toruń, Poland
2
Faculty of Chemistry, Jagiellonian University, Gronostajowa 2, 30-387 Kraków, Poland
3
Institute of Nuclear Physics of Polish Academy of Sciences, Radzikowskiego 152, 31-342 Kraków, Poland
*
Author to whom correspondence should be addressed.
Academic Editor: Robert Ivkov
Int. J. Mol. Sci. 2022, 23(3), 1556; https://doi.org/10.3390/ijms23031556
Received: 29 December 2021 / Revised: 19 January 2022 / Accepted: 27 January 2022 / Published: 29 January 2022
(This article belongs to the Section Materials Science)
We report a new structure of {[Co(bpy)2(ox)][{Cu2(bpy)2(ox)}Fe(ox)3]}n·8.5nH2O NCU-1 presenting a rare ladder topology among oxalate-based coordination polymers with anionic chains composed of alternately arranged [Cu2(bpy)2(ox)]2+ and [Fe(ox)3]3− moieties. Along the a axis, they are separated by Co(III) units to give porous material with voids of 963.7 Å3 (16.9% of cell volume). The stability of this structure is assured by a network of stacking interactions and charge-assisted C-H…O hydrogen bonds formed between adjacent chains, adjacent cobalt(III) units, and alternately arranged cobalt(III) and chain motifs. The soaking experiment with acetonitrile and bromobenzene showed that water molecules (8.5 water molecules dispersed over 15 positions) are bonded tightly, despite partial occupancy. Water adsorption experiments are described by a D’arcy and Watt model being the sum of Langmuir and Dubinin–Serpinski isotherms. The amount of primary adsorption sites calculated from this model is equal 8.2 mol H2O/mol, being very close to the value obtained from the XRD experiments and indicates that water was adsorbed mainly on the primary sites. The antiferromagnetic properties could be only approximately described with the simple CuII-ox-CuII dimer using H = −J·S1·S2, thus, considering non-trivial topology of the whole Cu-Fe chain, we developed our own general approach, based on the semiclassical model (SC) and molecular field (MF) model, to describe precisely the magnetic superexchange interactions in NCU-1. We established that Cu(II)-Cu(II) coupling dominates over multiple Cu(II)-Fe(III) interactions, with JCuCu = −275(29) and JCuFe = −3.8(1.6) cm−1 and discussed the obtained values against the literature data. View Full-Text
Keywords: coordination polymer; oxalate complex; single crystal XRD; magnetic properties; sorption properties; charge assisted hydrogen bonds coordination polymer; oxalate complex; single crystal XRD; magnetic properties; sorption properties; charge assisted hydrogen bonds
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MDPI and ACS Style

Muzioł, T.M.; Tereba, N.; Podgajny, R.; Pełka, R.; Czernia, D.; Wiśniewski, M.; Koter, S.; Wrzeszcz, G. Sorption and Magnetic Properties of Oxalato-Based Trimetallic Open Framework Stabilized by Charge-Assisted Hydrogen Bonds. Int. J. Mol. Sci. 2022, 23, 1556. https://doi.org/10.3390/ijms23031556

AMA Style

Muzioł TM, Tereba N, Podgajny R, Pełka R, Czernia D, Wiśniewski M, Koter S, Wrzeszcz G. Sorption and Magnetic Properties of Oxalato-Based Trimetallic Open Framework Stabilized by Charge-Assisted Hydrogen Bonds. International Journal of Molecular Sciences. 2022; 23(3):1556. https://doi.org/10.3390/ijms23031556

Chicago/Turabian Style

Muzioł, Tadeusz M., Natalia Tereba, Robert Podgajny, Robert Pełka, Dominik Czernia, Marek Wiśniewski, Stanisław Koter, and Grzegorz Wrzeszcz. 2022. "Sorption and Magnetic Properties of Oxalato-Based Trimetallic Open Framework Stabilized by Charge-Assisted Hydrogen Bonds" International Journal of Molecular Sciences 23, no. 3: 1556. https://doi.org/10.3390/ijms23031556

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