Some Supramolecular Nanostructures Based on Catalytic Active Nickel and Iron Heteroligand Complexes. Functional Models of Ni(Fe) Dioxygenases

Matienko, L. I.; Binyukov, V. I.; Mosolova, L. A.; Mil, E. M.; Заиков, Г. Е.

doi:10.23939/chcht08.03.339

Cited by 4 publications

(7 citation statements)

References 22 publications

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“…We assumed that one of the reasons for the different activity of Ni(Fe)ARD in the functioning of enzymes in relation to the common substrates (acireductone and O 2 ) can be the association of catalyst in various macrostructure due to intermolecular H-bonds. These assumptions were confirmed by our AFM-studies [6][7][8].…”

Section: Methodssupporting

confidence: 80%

“…AFM SOLVER P47/SMENA/ with Silicon Cantilevers NSG11S (NT MDT) with curvature radius 10 nm, tip height 10-15 µm and cone angle £22° in taping mode on resonant frequency 150 KHz was used [6][7][8].…”

Section: Methodsmentioning

confidence: 99%

“…In our previous works, we have shown that formation of multidimensional forms based on nickel complexes, in particular, forming of the stable nano structures based on Ni 2 (acac)(OAc) 3 ×NMP×2H 2 O, that are structural and functional model of NiARD, can be one of the regulating ways of two enzymes activity [6][7][8].…”

Section: Role Of Tyr-fragment In the Mechanism Of (Ni)ard Action On Mmentioning

confidence: 99%

“…We were the first to make the assumption that the stability of the triple complexes Ni(acac)2•L2•PhOH can also be connected with the formation of stable supramolecular macrostructures due to intra-and intermolecular hydrogen bonds [2,5]. Formation of supramolecular macrostructures based on ternary compexes Ni(acac) 2 •L 2 •PhOH due to intermolecular (phenol-carboxylate) H-bonds and, possibly, other non-covalent interactions, established by us with the AFM-method [6][7][8] is in favor of this hypothesis (Fig. 2).…”

Section: Role Of Tyr-fragment In the Mechanism Of (Ni)ard Action On Mmentioning

confidence: 99%

“…x (acac) y 18C6 m (H 2 O) n ("B"), {Ni(acac) 2 ×L 2 ×PhOH} ("C") (L 2 = NMP, HMPA, MSt (M = Na, Li)) (NMP = Nmethyl-2-pyrrolidone). Complexes are effective catalysts for the oxidation of alkylarens by molecular oxygen to hydroperoxides [5], and structural and functional models of acireductone dioxygenase Ni(Fe)ARD ("A"-"C") [6][7][8][9] and Fe II -Dke1 ("B") [6][7][8][9][10]. The stability of catalysts ("A"-"C") seemed to be caused by the formation during the catalytic reaction of stable supramolecular structures due to intermolecular H-bonds.…”

Section: Introductionmentioning

confidence: 99%

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Role of Supramolecular Strucutres in Mechanisms of Catalytic Oxidation and Action of Ni(Fe)ARD Dioxygenases on Model Systems

Matienko¹,

Binykov²,

Mil³

et al. 2020

ChChT

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The AFM technique was used to research the possibility of the supramolecular structures formation due to H-bonds based on Ni(Fe)(acac) n-systems, that are catalysts of alkylarens oxidations and also models Ni(Fe)ARD dioxygenases: {M(acac) n +L 2 +L 3 } triple systems (M=Ni II , Fe III , L 2 = NMP (NMP = N-methyl-2pirrolidone), L-histidine, L 3 = PhOH, L-tyrosine), n = 2, 3). Role of H-bonding and supramolecular structures in alkylarens oxidations, catalyzed with Ni(or Fe) complexes catalysts, and also role of supramolecular structures and Tyrfragment in mechanisms of Ni(Fe)ARD-actions is discussed.

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Section: Methodssupporting

confidence: 80%

Section: Methodsmentioning

confidence: 99%

Section: Role Of Tyr-fragment In the Mechanism Of (Ni)ard Action On Mmentioning

confidence: 99%

Section: Role Of Tyr-fragment In the Mechanism Of (Ni)ard Action On Mmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Role of Supramolecular Strucutres in Mechanisms of Catalytic Oxidation and Action of Ni(Fe)ARD Dioxygenases on Model Systems

Matienko¹,

Binykov²,

Mil³

et al. 2020

ChChT

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AFM Research of Supramolecular Structures

Matienko

Mil

Binyukov

2020

Russ. J. Phys. Chem. B

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AFM Research in Catalysis and Medicine

Matienko

Mickhailovna

Ivanovich

et al. 2020

COCAT

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Background: In Account, we show that the AFM method allows not only monitoring the morphological changes of biological structures fixed on the surface due to H-bonds. The AFM method also makes it possible to study the self-organization of metal complexes simulating the active center of enzymes due to intermolecular H-bonds into stable nanostructures, the sizes of which are much smaller than the studied biological objects. The possible role of intermolecular hydrogen bonds in the formation of stable supramolecular metal complexes, which are effective catalysts for the oxidation of alkylarenes to hydro peroxides by molecular oxygen and mimic the selective active sites of enzymes, was first studied by AFM. Methods and Results: The formation of supramolecular structures due tointermolecular hydrogen bonds and, possibly, other non-covalent interactions,based on homogenous catalysts and models of active centers enzymes,heteroligand nickel and iron complexes, was proven by AFM-technique. AFMstudies of supramolecular structures were carried out using NSG30 cantileverwith a radius of curvature of 2 nm, in the tapping mode. To form nanostructureson the surface of a hydrophobic chemically modified silicon surface as asubstrate, the sample was prepared using a spin-cotting process from solutionsof the nickel and iron complexes. The composition and the structure of thecomplex Ni2(acac)(OAc)3∙NMP∙2H2O weredetermined in earlier works [6] using various methods: mass spectrometry, UV- andIR-spectroscopy, elemental analysis, polarography. Self-assembly of supramolecular structures isdue to intermolecular interactions with a certain coordination of theseinteractions, which may be a consequence of the properties of the componentsthemselves, the participation of hydrogen bonds and other non-covalentinteractions, as well as the balance of the interaction of these componentswith the surface. UsingAFM, approaches have been developed for fixing on the surface andquantifying parameters of cells. Conclusion: This Account summarizes the authors' achievements in using the atomic force microscopy (AFM) method to study, the role of intermolecular hydrogen bonds (and other non-covalent interactions) and supramolecular structures in the mechanisms of catalysis. The obtained data of AFM based on nickel and iron complexes, which are effective catalysts and models of active sites of enzymes, indicate a high probability of the formation of supramolecular structures in real conditions of catalytic oxidation, and can bring us closer to understanding enzymes activity. With sensitive AFM method, it is possible to observe the self-organization of model systems into stable nanostructures due to H-bonds and possibly other non-covalent interactions, which can be considered as a step towards modeling the active sites of enzymes. Methodical approaches of atomic force microscopy for the study of morphological changes of cells have been developed.

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Some Supramolecular Nanostructures Based on Catalytic Active Nickel and Iron Heteroligand Complexes. Functional Models of Ni(Fe) Dioxygenases

Cited by 4 publications

References 22 publications

Role of Supramolecular Strucutres in Mechanisms of Catalytic Oxidation and Action of Ni(Fe)ARD Dioxygenases on Model Systems

Role of Supramolecular Strucutres in Mechanisms of Catalytic Oxidation and Action of Ni(Fe)ARD Dioxygenases on Model Systems

AFM Research of Supramolecular Structures

AFM Research in Catalysis and Medicine

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