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1. Tunable mechanical properties of [Fe(pyrazine){Au(CN)2}2]–PVDF composite films with spin transitions

Author

Yurii S. Bibik, José Elias Angulo-Cervera, Il'ya A. Gural'skiy, Rostyslav D. Lampeka, Department of Chemistry, Taras Shevchenko National University of Kyiv, Taras Shevchenko National University of Kyiv, UkrOrgSyntez Ltd. (UORSY), Équipe Microsystèmes électromécaniques (LAAS-MEMS), Laboratoire d'analyse et d'architecture des systèmes (LAAS), Université Toulouse - Jean Jaurès (UT2J)-Université Toulouse 1 Capitole (UT1), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse - Jean Jaurès (UT2J)-Université Toulouse 1 Capitole (UT1), Université Fédérale Toulouse Midi-Pyrénées, Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Toulouse Capitole (UT Capitole), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université Toulouse - Jean Jaurès (UT2J), Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université Toulouse Capitole (UT Capitole), Université de Toulouse (UT), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
optical properties, Materials science, Polymers and Plastics, Pyrazine, Composite number, Modulus, 02 engineering and technology, mechanical properties, 010402 general chemistry, 01 natural sciences, composites, Stress (mechanics), chemistry.chemical_compound, Ultimate tensile strength, Materials Chemistry, Composite material, Spin (physics), chemistry.chemical_classification, Organic Chemistry, Polymer, 021001 nanoscience & nanotechnology, 0104 chemical sciences, phase transitions, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Thermomechanical analysis, elastic properties, 0210 nano-technology
Abstract

International audience; Here we describe the elaboration and investigation of composites prepared from the spincrossover (SCO) complex [Fe(pyrazine){Au(CN) 2 } 2 ] and poly(vinylidene fluoride) matrix, with different contents of the active phase (10-35 wt%). Optical measurements demonstrated that all composites preserve temperature induced hysteretic spin transitions. Tensile mechanical analysis showed a non-linear change of the Young's modulus upon increase of the complex content. Thermomechanical analysis upon a constant strain demonstrated pronouncable alterations of the applied stress in the SCO region. Composites with smaller loads require less stress to attain a given strain in the high-spin state, however for those with high loads the behaviour is more sofisticated. The modelling of stress vs. temperature behaviour revealed that this may be interpreted through a miscellaneous interplay of expansion of both the polymer and the complex, the contribution of both components to the elastic properties of composites, and the effects of SCO on these properties.

Published
2022
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2. Influence of the ultra-slow nucleation and growth dynamics on the room-temperature hysteresis of spin-crossover single crystals

Author

A. A. Golub, Azzedine Bousseksou, Il'ya A. Gural'skiy, Gábor Molnár, Karl Ridier, Volodymyr M. Hiiuk, William Nicolazzi, Igor O. Fritsky, Department of Chemistry, Taras Shevchenko National University of Kyiv, Taras Shevchenko National University of Kyiv, UkrOrgSyntez Ltd. (UORSY), National University of Kyiv-Mohyla Academy (UKMA), Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), H2020-MSCA-RISE-2016 Project 734322, and Ministry of Education and Science of Ukraine - Projects 19BF037-01M and 19BF037-04

Subjects
Materials science, Orders of magnitude (temperature), Coordination polymer, Kinetics, Nucleation, Spin transition, General Physics and Astronomy, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Nucleation and growth dynamics, chemistry.chemical_compound, Optical microscope, Spin crossover, law, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Physical and Theoretical Chemistry, Hysteresis, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical physics, Single crystals, Defects, 0210 nano-technology
Abstract

International audience; Nucleation and growth phenomena associated with the thermally-induced spin transition was studied using optical microscopy in single crystals of a cyanoheterometallic coordination polymer [Fe(1,6-naphthyridine)2(Ag(CN)2)2]. Despite the fact that the spin-crossover phenomenon occurs near room temperature (ca. 290–300 K), the experimental results show the existence of significant kinetic effects on the hysteretic behaviour of the spin transition in this compound. Ultra-slow switching rates and phase-boundary propagation velocities were observed (down to 3 nm s−1), several orders of magnitude lower than customary. Our observations indicate that these peculiar spin-crossover properties (slow switching kinetics, scan-rate-dependent transition temperatures) are presumably related to the presence of numerous microstructural defects in the crystals, which is an intrinsic characteristic of this compound.

Published
2021
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3. Pressure gradient effect on spin-crossover materials: Experiment vs theory

Author

Il'ya A. Gural'skiy, Aurelian Rotaru, Gábor Molnár, Ionela Rusu, Ioan Cozmin Manolache-Rusu, Oleg Palamarciuc, Andrei Diaconu, MANSiD Research Center [Suceava], Universitatea Stefan cel Mare Suceava (USU), State University of Moldova, UkrOrgSyntez Ltd. (UORSY), Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), SPINSWITCH Project (No. H2020-MSCA-RISE-2016, Grant Agreement No. 734322), and EXCALIBUR Project Contract No. 18 PFE/16.10.2018

Subjects
010302 applied physics, Materials science, Thermal hysteresis, Condensed matter physics, Diagram, General Physics and Astronomy, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Loop (topology), Distribution (mathematics), Spin crossover, High pressure, 0103 physical sciences, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [CHIM.COOR]Chemical Sciences/Coordination chemistry, 0210 nano-technology, Pressure gradient
Abstract

We studied the effect of non-hydrostatic pressure on the hysteretic spin crossover in coordination complexes. By introducing into an Ising-like model a double distribution of the interactions and gap energy, respectively, we were able to generate the major hysteresis loop and the first-order reversal curve (FORC) diagram for spin-crossover systems of 106hysterons (like-spin domains). We show that, for high pressure gradients around the spin-crossover system, the thermal hysteresis loop takes an asymmetric shape, in good agreement with the experimental data on pressure effect recorded at low temperatures, below the solidification of the pressure transmitting medium. Interestingly, the FORC diagram method seems to be much more sensitive to local changes than the “bulk” parameters, which characterize the major hysteresis loop.

Published
2021
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4. Anomalous Pressure Effects on the Electrical Conductivity of the Spin Crossover Complex [Fe(pyrazine){Au(CN)2}2]

Author

Andrei-Cristian Gheorghe, Yurii S. Bibik, Andrei Diaconu, Aurelian Rotaru, Olesia I. Kucheriv, Ionela Rusu, Diana D. Barakhtii, Il'ya A. Gural'skiy, Marin-Vlad Boicu, Gábor Molnár, University Stefan cel Mare of Suceava (USU), MANSiD Research Center [Suceava], Universitatea Stefan cel Mare Suceava (USU), Department of Chemistry, Taras Shevchenko National University of Kyiv, Taras Shevchenko National University of Kyiv, UkrOrgSyntez Ltd. (UORSY), Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), European Commission through the SPINSWITCH project (H2020-MSCA-RISE-2016, Grant Agreement No. 734322), EXCALIBUR project (Contract No. 18 PFE/16.10.2018), and Ministry of Education and Science of Ukraine (grant No. 19BF037-01M)

Subjects
Materials science, Pyrazine, Spin states, Crossover, 02 engineering and technology, Conductivity, Charge transport, 010402 general chemistry, 01 natural sciences, lcsh:Chemistry, chemistry.chemical_compound, Electrical resistivity and conductivity, Spin crossover, Materials Chemistry, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Electrical conductor, Condensed matter physics, 021001 nanoscience & nanotechnology, Nanocrystalline material, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, High pressure, lcsh:QD1-999, chemistry, Chemistry (miscellaneous), Condensed Matter::Strongly Correlated Electrons, 0210 nano-technology
Abstract

International audience; We studied the spin-state dependence of the electrical conductivity of two nanocrystalline powder samples of the spin crossover complex [Fe(pyrazine){Au(CN) 2 } 2 ]. By applying an external pressure (up to 3 kbar), we were able to tune the charge transport properties of the material from a more conductive low spin state to a crossover point toward a more conductive high spin state. We rationalize these results by taking into account the spin-state dependence of the activation parameters of the conductivity.

Published
2020
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5. Generating Multibillion Chemical Space of Readily Accessible Screening Compounds.

Author

Grygorenko OO, Radchenko DS, Dziuba I, Chuprina A, Gubina KE, and Moroz YS

Abstract

An approach to the generation of ultra-large chemical libraries of readily accessible ("REAL") compounds is described. The strategy is based on the use of two- or three-step three-component reaction sequences and available starting materials with pre-validated chemical reactivity. After the preliminary parallel experiments, the methods with at least ∼80% synthesis success rate (such as acylation - deprotection - acylation of monoprotected diamines or amide formation - click reaction with functionalized azides) can be selected and used to generate the target chemical space. It is shown that by using only on the two aforementioned reaction sequences, a nearly 29-billion compound library is easily obtained. According to the predicted physico-chemical descriptor values, the generated chemical space contains large fractions of both drug-like and "beyond rule-of-five" members, whereas the strictest lead-likeness criteria (the so-called Churcher's rules) are met by the lesser part, which still exceeds 22 million., Competing Interests: The authors declare no competing interests., (© 2020 The Author(s).)

Published
2020
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6. Deoxofluorination of (Hetero)aromatic Acids.

Author

Trofymchuk S, Bugera MY, Klipkov AA, Razhyk B, Semenov S, Tarasenko K, Starova VS, Zaporozhets OA, Tananaiko OY, Alekseenko AN, Pustovit Y, Kiriakov O, Gerus II, Tolmachev AA, and Mykhailiuk PK

Abstract

Diverse trifluoromethyl-substituted compounds were synthesized by deoxofluorination of cinnamic and (hetero)aromatic carboxylic acids with sulfur tetrafluoride. The obtained products were used as starting materials in the preparation of novel fluorinated amino acids, anilines, and aliphatic amines - valuable building blocks for medicinal chemistry and agrochemistry.

Published
2020
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7. Expanding Synthesizable Space of Disubstituted 1,2,4-Oxadiazoles.

Author

Tolmachev A, Bogolubsky AV, Pipko SE, Grishchenko AV, Ushakov DV, Zhemera AV, Viniychuk OO, Konovets AI, Zaporozhets OA, Mykhailiuk PK, and Moroz YS

Subjects
Humans, Oximes chemical synthesis, Receptors, G-Protein-Coupled agonists, Structure-Activity Relationship, Carboxylic Acids chemistry, Nitriles chemistry, Oxadiazoles chemistry
Abstract

One-pot synthesis of 3,5-disubstituted 1,2,4-oxadiazoles from carboxylic acids and nitriles was optimized to parallel chemistry. The method was validated on a 141 member library; the desired products were recovered with a high success rate and in moderate yields. Practical application of the approach was demonstrated in the synthesis of bioactive compound pifexole and agonists of free fatty acid receptor 1. A library of 4 948 100 synthesizable drug-like 3,5-disubstituted 1,2,4-oxadiazoles was enumerated based on the method and available validated reagents.

Published
2016
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