Oxidation of styrene by Mn (II)-pyridine-2,6-dicarboxylate complex: Synthesis, X-ray structure and DFT studies

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216224%3A14310%2F25%3A00143553" target="_blank" >RIV/00216224:14310/25:00143553 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S0022286025001292" target="_blank" >https://www.sciencedirect.com/science/article/pii/S0022286025001292</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.molstruc.2025.141440" target="_blank" >10.1016/j.molstruc.2025.141440</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Oxidation of styrene by Mn (II)-pyridine-2,6-dicarboxylate complex: Synthesis, X-ray structure and DFT studies

Popis výsledku v původním jazyce

A transition metal complex of Mn (II) formulated as [Mn(dipic)(phen)(H2O)].H2O (complex 1) was successfully synthesized, wherein dipic2- refers to pyridine-2,6-dicarboxylate, and phen refers to 1,10-phenanthroline. Complex 1 was characterized by single-crystal X-ray diffraction (SC-XRD), elemental analysis, and Fouriertransform infrared (FT-IR) spectroscopy. The crystallographic analysis of complex 1 was conducted at 120(2) K. The structure of complex 1 revealed a distorted octahedral geometry within a monoclinic crystal system, belonging to space group P21/c. The central Mn (II) ion was found to be coordinated with three oxygen and three nitrogen atoms originating from three unique ligands. The stability of complex 1 was investigated using density functional theory (DFT) computations. Interaction energy, energies of the most important molecular orbitals, molecular electrostatic potential (MEP) maps, aromaticity of the rings, and density of states (DOS) plots were surveyed. Results disclose that the formation of complex 1 is accompanied by a decrease/increase of negative charge/aromaticity of its rings compared to the ligands. Also, the energy gap (Egap) value of complex 1 is smaller than the parallel data for the ligands. Thus, complex 1 better passes electrons from the barrier to the conductive band than the free ligands. In the following, complex 1 was immobilized onto mesoporous SiO2 particles, yielding a recoverable catalyst [Mn(dipic)(phen)(H2O)].H2O/SiO2 (catalyst 1). Catalyst 1 was characterized using an energy-dispersive X-ray spectrometer (EDS), FT-IR spectroscopy, scanning electron micrograph (SEM), transmission electron microscopy (TEM), and powder X-ray diffraction pattern (PXRD (. Complex 1, and catalyst 1 catalyze the oxidation of styrene in a homogeneous and heterogeneous catalytic system consisting of H2O2. The results of oxidation reactions showed that catalyst 1 is a more effective catalyst for styrene oxidation than complex 1 due to the synergistic effects between metal and support. Finally, the reaction conditions were optimized for catalyst 1.

Název v anglickém jazyce

Oxidation of styrene by Mn (II)-pyridine-2,6-dicarboxylate complex: Synthesis, X-ray structure and DFT studies

Popis výsledku anglicky

A transition metal complex of Mn (II) formulated as [Mn(dipic)(phen)(H2O)].H2O (complex 1) was successfully synthesized, wherein dipic2- refers to pyridine-2,6-dicarboxylate, and phen refers to 1,10-phenanthroline. Complex 1 was characterized by single-crystal X-ray diffraction (SC-XRD), elemental analysis, and Fouriertransform infrared (FT-IR) spectroscopy. The crystallographic analysis of complex 1 was conducted at 120(2) K. The structure of complex 1 revealed a distorted octahedral geometry within a monoclinic crystal system, belonging to space group P21/c. The central Mn (II) ion was found to be coordinated with three oxygen and three nitrogen atoms originating from three unique ligands. The stability of complex 1 was investigated using density functional theory (DFT) computations. Interaction energy, energies of the most important molecular orbitals, molecular electrostatic potential (MEP) maps, aromaticity of the rings, and density of states (DOS) plots were surveyed. Results disclose that the formation of complex 1 is accompanied by a decrease/increase of negative charge/aromaticity of its rings compared to the ligands. Also, the energy gap (Egap) value of complex 1 is smaller than the parallel data for the ligands. Thus, complex 1 better passes electrons from the barrier to the conductive band than the free ligands. In the following, complex 1 was immobilized onto mesoporous SiO2 particles, yielding a recoverable catalyst [Mn(dipic)(phen)(H2O)].H2O/SiO2 (catalyst 1). Catalyst 1 was characterized using an energy-dispersive X-ray spectrometer (EDS), FT-IR spectroscopy, scanning electron micrograph (SEM), transmission electron microscopy (TEM), and powder X-ray diffraction pattern (PXRD (. Complex 1, and catalyst 1 catalyze the oxidation of styrene in a homogeneous and heterogeneous catalytic system consisting of H2O2. The results of oxidation reactions showed that catalyst 1 is a more effective catalyst for styrene oxidation than complex 1 due to the synergistic effects between metal and support. Finally, the reaction conditions were optimized for catalyst 1.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

JOURNAL OF MOLECULAR STRUCTURE

ISSN

0022-2860

e-ISSN

1872-8014

Svazek periodika

1330

Číslo periodika v rámci svazku

May

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

12

Strana od-do

1-12

Kód UT WoS článku

001411506600001

EID výsledku v databázi Scopus

2-s2.0-85215542692