Fe(III)-Based Phenylsilsesquioxane/Acetylacetonate Complexes: Synthesis, Cage-like Structure, and High Catalytic Activity

被引：4

作者：

Bilyachenko, Alexey N. ^{[1
,2
]}

Khrustalev, Victor N. ^{[2
,3
]}

Dorovatovskii, Pavel V. ^{[4
]}

Shul'pina, Lidia S. ^{[1
]}

Ikonnikov, Nikolay S. ^{[1
]}

Shubina, Elena S. ^{[1
]}

Lobanov, Nikolai N. ^{[2
]}

Aliyeva, Vusala A. ^{[5
]}

Nunes, Ana V. M. ^{[6
]}

Mahmudov, Kamran T. ^{[5
,7
]}

Kozlov, Yuriy N. ^{[8
,9
]}

Pombeiro, Armando J. L. ^{[1
]}

机构：

[1] Russian Acad Sci, AN Nesmeyanov Inst Organoelement Cpds, Moscow 119991, Russia

[2] RUDN Univ, Peoples Friendship Univ Russia, Moscow 117198, Russia

[3] Russian Acad Sci, Zelinsky Inst Organ Chem, Moscow 119991, Russia

[4] Kurchatov Inst, Natl Res Ctr, Moscow 123182, Russia

[5] Univ Lisbon, Inst Mol Sci, Ctr Quim Estrut, Inst Super Tecn, P-1049001 Lisbon, Portugal

[6] Univ Nova Lisboa, Fac Ciencias & Tecnol, Dept Quim, LAQV REQUIMTE, P-2829516 Caparica, Portugal

[7] Baku State Univ, Excellence Ctr, Baku Az 1148, Azerbaijan

[8] Russian Acad Sci, NN Semenov Fed Res Ctr Chem Phys, Moscow 119991, Russia

[9] Plekhanov Russian Univ Econ, Moscow 117997, Russia

来源：

INORGANIC CHEMISTRY | 2024年 / 63卷 / 04期

基金：

俄罗斯科学基金会;

关键词：

POLYHEDRAL OLIGOMERIC SILSESQUIOXANE; EFFICIENT; METALLASILSESQUIOXANES; OXIDATION; BEHAVIOR; MODELS;

D O I：

10.1021/acs.inorgchem.3c03587

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Unprecedented iron-based silsesquioxane/acetylacetonate complexes were synthesized. The intriguing cage-like structure of compounds is alkaline metal-dependent: the Fe2Li2 complex includes condensed Si-6-silsesquioxane and four acetylacetonate ligands; the Fe4Na4 complex exhibits two cyclic Si-4-silsesquioxane and eight acetylacetonate ligands, while the Fe3K3 complex features two cyclic Si-3-silsesquioxane and six acetylacetonate ligands. The latter case is the very first observation of small trimeric silsesquioxane ligands in the composition of cage-like metallasilsesquioxanes. The Fe4Na4-based complex exhibits a record high activity in the oxidation of inert alkanes with peroxides (55% yield of oxygenates in cyclohexane oxidation). It also acts as a catalyst in the cycloaddition of CO2 with epoxides, leading to cyclic carbonates in good yields (58-96%).

引用

页码：1909 / 1918

页数：10

共 72 条

[1]

Abbenhuis HCL, 2000, CHEM-EUR J, V6, P25, DOI 10.1002/(SICI)1521-3765(20000103)6:1<25::AID-CHEM25>3.3.CO

[2]

2-P

[3] An NHC-Stabilized Silicon Analogue of Acylium Ion: Synthesis, Structure, Reactivity, and Theoretical Studies [J].

Ahmad, Syed Usman ;

Szilvasi, Tibor ;

Irran, Elisabeth ;

Inoue, Shigeyoshi .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (17) :5828-5836

[4] Halogen Bonding in the Decoration of Secondary Coordination Sphere of Zinc(II) and Cadmium(II) Complexes: Catalytic Application in Cycloaddition Reaction of CO2 with Epoxides [J].

Aliyeva, Vusala A. ;

Paninho, Ana B. ;

Nunes, Ana V. M. ;

Karmakar, Anirban ;

Gurbanov, Atash V. ;

Rutigliano, Arianna R. ;

Gallo, Emma ;

Mahmudov, Kamran T. ;

Pombeiro, Armando J. L. .

ACS OMEGA, 2023, 8 (45) :42290-42300

[5] Cu(II)-silsesquioxanes as efficient precatalysts for Chan-Evans-Lam coupling [J].

Astakhov, G. S. ;

Levitsky, M. M. ;

Bantreil, X. ;

Lamaty, F. ;

Khrustalev, V. N. ;

Zubavichus, Y. V. ;

Dorovatovskii, P. V. ;

Shubina, E. S. ;

Bilyachenko, A. N. .

JOURNAL OF ORGANOMETALLIC CHEMISTRY, 2020, 906

[6] Cage-like manganesesilsesquioxanes: features of their synthesis, unique structure, and catalytic activity in oxidative amidations [J].

Astakhov, Grigorii S. ;

Khrustalev, Victor N. ;

Dronova, Marina S. ;

Gutsul, Evgenii, I ;

Korlyukov, Alexander A. ;

Gelman, Dmitri ;

Zubavichus, Yan, V ;

Novichkov, Daniil A. ;

Trigub, Alexander L. ;

Shubina, Elena S. ;

Bilyachenko, Alexey N. .

INORGANIC CHEMISTRY FRONTIERS, 2022, 9 (17) :4525-4537

[7] Coordination Affinity of Cu(II)-Based Silsesquioxanes toward N,N-Ligands and Associated Skeletal Rearrangements: Cage and Ionic Products Exhibiting a High Catalytic Activity in Oxidation Reactions [J].

Astakhov, Grigorii S. ;

Bilyachenko, Alexey N. ;

Levitsky, Mikhail M. ;

Shul'pina, Lidia S. ;

Korlyukov, Alexander A. ;

Zubavichus, Yan, V ;

Khrustalev, Victor N. ;

Vologzhanina, Anna V. ;

Shubina, Elena S. ;

Dorovatovskii, Pavel, V ;

Shul'pin, Georgiy B. .

INORGANIC CHEMISTRY, 2020, 59 (07) :4536-4545

[8] A Family of Cagelike Mn-Silsesquioxane/Bathophenanthroline Complexes: Synthesis, Structure, and Catalytic and Antifungal Activity [J].

Bilyachenko, Alexey N. ;

Gutsul, Evgenii I. ;

Khrustalev, Victor N. ;

Chusova, Olga ;

Dorovatovskii, Pavel V. ;

Aliyeva, Vusala A. ;

Paninho, Ana B. ;

Nunes, Ana V. M. ;

Mahmudov, Kamran T. ;

Shubina, Elena S. ;

Pombeiro, Armando J. L. .

INORGANIC CHEMISTRY, 2023, 62 (38) :15537-15549

[9] Cage-like Cu5Cs4-Phenylsilsesquioxanes: Synthesis, Supramolecular Structures, and Catalytic Activity [J].

Bilyachenko, Alexey N. ;

Arteev, Ivan S. ;

Khrustalev, Victor N. ;

Shul'pina, Lidia S. ;

Korlyukov, Alexander A. ;

Ikonnikov, Nikolay S. ;

Shubina, Elena S. ;

Kozlov, Yuriy N. ;

Conceicao, Nuno Reis ;

da Silva, M. Fatima C. Guedes ;

Mahmudov, Kamran T. ;

Pombeiro, Armando J. L. .

INORGANIC CHEMISTRY, 2023, 62 (33) :13573-13586

[10] Acetone Factor in the Design of Cu4-, Cu6-, and Cu9-Based Cage Coppersilsesquioxanes: Synthesis, Structural Features, and Catalytic Functionalization of Alkanes [J].

Bilyachenko, Alexey N. ;

Gutsul, Evgenii I. ;

Khrustalev, Victor N. ;

Astakhov, Grigorii S. ;

Zueva, Anna Y. ;

Zubavichus, Yan V. ;

Kirillova, Marina V. ;

Shulpina, Lidia S. ;

Ikonnikov, Nikolay S. ;

Dorovatovskii, Pavel V. ;

Shubina, Elena S. ;

Kirillov, Alexander M. ;

Shulpin, Georgiy B. .

INORGANIC CHEMISTRY, 2022, 61 (37) :14800-14814

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