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This is an early access version, the complete PDF, HTML, and XML versions will be available soon.
Article

Selective Catalysis by Complexes Including Ni and Redox-Inactive Alkali Metals (Li, Na, or K) in Oxidation Processes: The Role of Hydrogen Bonds and Supramolecular Structures

by
Ludmila I. Matienko
*,
Elena M. Mil
,
Anastasia A. Albantova
* and
Alexander N. Goloshchapov
N.M. Emanuel Institution of Biochemical Physics Russian Academy of Science, 4 Kosygin Str., 119334 Moscow, Russia
*
Authors to whom correspondence should be addressed.
Int. J. Mol. Sci. 2025, 26(3), 1166; https://doi.org/10.3390/ijms26031166
Submission received: 16 December 2024 / Revised: 20 January 2025 / Accepted: 26 January 2025 / Published: 29 January 2025
(This article belongs to the Section Materials Science)
Review Reports Versions Notes

Abstract

It is known that the presence of redox-inactive metals in the active center of an enzyme has a significant effect on its activity. In this regard and for other reasons, the effect of redox-inactive metals on redox processes, such as electron transfer, oxygen and hydrogen atom transfer, as well as the breaking and formation of O–O bonds in reactions catalyzed by transition metals, has been widely studied. Many questions about the role of redox-inactive metals in the mechanisms of these reactions remain open. In this paper, the mechanism of catalysis by bi- and triple hetero-binuclear heteroligand complexes including Ni and redox-inactive alkali metals ((A) {Ni(acac)2∙L2} and (B) {Ni(acac)2∙L2∙PhOH} (L2 = MSt (M = Li, Na, or K)) in the process of the selective oxidation of ethylbenzene by molecular oxygen into α-phenyl ethyl hydroperoxide is considered. The activity of A and B complexes towards O2, ROOH, and RO2• radicals was studied. Based on kinetic data, we suggest that the high catalytic efficiency of B triple complexes in oxidation processes may be associated with the role of outer-sphere regulatory interactions, with the formation of stable supramolecular structures due to intermolecular H bonds. This assumption was confirmed using the AFM method. Prospects for studying catalysis by complexes ({Ni(acac)2∙L2} and {Ni(acac)2∙L2∙PhOH}) that are models of NiARD (Ni-Acyreductone dioxygenase) are discussed.
Keywords: triple binuclear complexes Ni(acac)2∙MSt∙PhOH (M = Li, Na, or K); H bonds; catalysis; oxidation; nanostructures; NiARD models triple binuclear complexes Ni(acac)2∙MSt∙PhOH (M = Li, Na, or K); H bonds; catalysis; oxidation; nanostructures; NiARD models

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MDPI and ACS Style

Matienko, L.I.; Mil, E.M.; Albantova, A.A.; Goloshchapov, A.N. Selective Catalysis by Complexes Including Ni and Redox-Inactive Alkali Metals (Li, Na, or K) in Oxidation Processes: The Role of Hydrogen Bonds and Supramolecular Structures. Int. J. Mol. Sci. 2025, 26, 1166. https://doi.org/10.3390/ijms26031166

AMA Style

Matienko LI, Mil EM, Albantova AA, Goloshchapov AN. Selective Catalysis by Complexes Including Ni and Redox-Inactive Alkali Metals (Li, Na, or K) in Oxidation Processes: The Role of Hydrogen Bonds and Supramolecular Structures. International Journal of Molecular Sciences. 2025; 26(3):1166. https://doi.org/10.3390/ijms26031166

Chicago/Turabian Style

Matienko, Ludmila I., Elena M. Mil, Anastasia A. Albantova, and Alexander N. Goloshchapov. 2025. "Selective Catalysis by Complexes Including Ni and Redox-Inactive Alkali Metals (Li, Na, or K) in Oxidation Processes: The Role of Hydrogen Bonds and Supramolecular Structures" International Journal of Molecular Sciences 26, no. 3: 1166. https://doi.org/10.3390/ijms26031166

APA Style

Matienko, L. I., Mil, E. M., Albantova, A. A., & Goloshchapov, A. N. (2025). Selective Catalysis by Complexes Including Ni and Redox-Inactive Alkali Metals (Li, Na, or K) in Oxidation Processes: The Role of Hydrogen Bonds and Supramolecular Structures. International Journal of Molecular Sciences, 26(3), 1166. https://doi.org/10.3390/ijms26031166

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