By Maria B. Ezhova, Brian R. James (auth.), László I. Simándi (eds.)
The topic of dioxygen activation and homogeneous catalytic oxidation by way of steel complexes has been within the concentration of awareness over the past two decades. The common curiosity is illustrated by way of its habitual presence one of the classes and topic parts of vital overseas meetings on a variety of facets of bioinorganic and coordination chemistry in addition to catalysis. the main famous examples are ICCC, ICBIC, EUROBIC, ISHC, and naturally the ADHOC sequence of conferences concentrating on the topic itself. equally, the variety of unique and assessment papers dedicated to quite a few features of dioxygen activation are at the upward push. This pattern is due evidently to the relevance of catalytic oxidation to organic strategies corresponding to dioxygen shipping, and the motion of oxygenase and oxidase enzymes concerning metabolism. The structural and practical modeling of metalloenzymes, quite of these containing iron and copper, via low-molecular complexes of iron, copper, ruthenium, cobalt, manganese, etc., have supplied a wealth of oblique info assisting to appreciate how the lively facilities of metalloenzymes may perhaps function. the information won from the examine of metalloenzyme versions is usually acceptable within the layout of transition steel complexes as catalytsts for particular reactions. This procedure has become referred to as biomimetic or bioinspired catalysis and remains to be a fruitful and increasing quarter of research.
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Extra resources for Advances in Catalytic Activation of Dioxygen by Metal Complexes
10) has been reported by Che’s group163. , led to the corresponding alcohols (27-48% yield) and ketones (24-34% yield), with ee values of 9-58% (S) for the alcohols. 2 at 25°C. A dual-parameter Hammett correlation with data for 4-substituted ethylbenzenes was considered consistent with a ratelimiting step involving C-H bond cleavage (Fig. 21). Preferential formation of the S-isomer was explained by preferential collapse of the benzylic radical 44 Maria B. Ezhova and Brian R. James on the pro-S face versus pro-R face during an O-atom rebound step, resulting from the fit of the substrate in the chiral cavity (see Fig.
The species is thermally unreactive toward cyclooctane at 1 atm at 70°C, but some O-atom insertion into saturated C-H bonds has been achieved under photolytic conditions and with the electrochemically generated species40; few details are available, but the latter system showed for adamantane oxidation the usual radical selectivity (tertiary > secondary carbon). Work in this laboratory has shown also that the complexes (porp = TMP, TDCPP, and are “practically” inactive for thermal of saturated hydrocarbons65.
In pyridine solution, a reaction similar to 29 generates and two equivalents of epoxide. In EtOH, the monooxo species is thought to be stabilized as Ru(OEP)O(EtOH) and a very slow catalytic epoxidation, observed at 1 atm was attributed to slow of Ru(IV)=O to Ru(VI)-dioxo species67; whether disproportionation of the Ru(IV)=O occurs under these conditions (eq. 16) is unclear. As noted for the thioether oxidations, introduction of halogen substituents into the porphyrin, especially in positions to prevent sterically formation of Ru species, can increase and/or prolong catalytic activity.