NDLI: Pyrazolate-Based Cobalt(II)-Containing Metal–Organic Frameworks in Heterogeneous Catalytic Oxidation Reactions: Elucidating the Role of Entatic States for Biomimetic Oxidation Processes

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The First Total Synthesis of Cytopiloyne, an Anti-Diabetic, Polyacetylenic Glucoside

Pyrazolate-Based Cobalt(II)-Containing Metal–Organic Frameworks in Heterogeneous Catalytic Oxidation Reactions: Elucidating the Role of Entatic States for Biomimetic Oxidation Processes

Preparation, Structure, and Ethylene (Co)Polymerization Behavior of Group IV Metal Complexes with an [OSSO]-Carborane Ligand

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Pyrazolate-Based Cobalt(II)-Containing Metal–Organic Frameworks in Heterogeneous Catalytic Oxidation Reactions: Elucidating the Role of Entatic States for Biomimetic Oxidation Processes

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Mavrandonakis, Andreas Lu, Ying Tonigold, Markus Möllmer, Jens Volkmer, Dirk Staudt, Reiner Puls, Angela Sauer, Joachim
Description	Author Affiliation: Tonigold M ( Universität Augsburg, Institut für Physik, Lehrstuhl für Festkörperchemie, Universitätsstrasse 1, 86159 Augsburg, Germany.)
Abstract	Crystal structures of two metal–organic frameworks (MFU-1 and MFU-2) are presented, both of which contain redox-active $Co^{II}$ centres coordinated by linear 1,4-bis[(3,5-dimethyl)pyrazol-4-yl] ligands. In contrast to many MOFs reported previously, these compounds show excellent stability against hydrolytic decomposition. Catalytic turnover is achieved in oxidation reactions by employing tert-butyl hydroperoxide and the solid catalysts are easily recovered from the reaction mixture. Whereas heterogeneous catalysis is unambiguously demonstrated for MFU-1, MFU-2 shows catalytic activity due to slow metal leaching, emphasising the need for a deeper understanding of structure–reactivity relationships in the future design of redox-active metal–organic frameworks. Mechanistic details for oxidation reactions employing tert-butyl hydroperoxide are studied by UV/Vis and IR spectroscopy and XRPD measurements. The catalytic process accompanying changes of redox states and structural changes were investigated by means of cobalt K-edge X-ray absorption spectroscopy. To probe the putative binding modes of molecular oxygen, the isosteric heats of adsorption of $O_{2}$ were determined and compared with models from DFT calculations. The stabilities of the frameworks in an oxygen atmosphere as a reactive gas were examined by temperature-programmed oxidation (TPO). Solution impregnation of MFU-1 with a co-catalyst (N-hydroxyphthalimide) led to NHPI@MFU-1, which oxidised a range of organic substrates under ambient conditions by employing molecular oxygen from air. The catalytic reaction involved a biomimetic reaction cascade based on free radicals. The concept of an entatic state of the cobalt centres is proposed and its relevance for sustained catalytic activity is briefly discussed.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	31
Volume Number	17
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2011-07-25
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Cobalt Chemistry Models, Molecular Organometallic Compounds Phthalimides Pyrazoles Catalysis Crystallography, X-Ray Molecular Conformation Oxidation-Reduction Spectrophotometry, Infrared Spectrophotometry, Ultraviolet Thermodynamics X-Ray Absorption Spectroscopy Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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