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This account presents an overview of our achievements in structural and chemical understanding of endohedral metallofullerenes (EMFs), a new class of metal-carbon hybrid materials formed by encapsulation of metals inside fullerene cavities. Structural determination of EMFs is of fundamental importance for understanding their intrinsic properties and the formation mechanism, and for broadening their applications. We have developed an effective method for determining the structures of paramagnetic EMFs, and also succeeded in observing the motion of cluster in a di-metal EMF for the first time. Recently, we unambiguously established the structures of some carbide EMFs which had been wrongly assumed as conventional EMFs previously. More importantly, we have obtained some insoluble EMF species which had never been explored or even expected before. Meanwhile, the chemical properties of various EMFs with different cage structures or different metallic cores have been systematically investigated by means of both covalent and supramolecular considerations, yielding many fascinating results relating to the dictating effect of internal metals. It is noteworthy that all these achievements are based on unambiguous X-ray results of pristine or functionalized EMFs. DOI 10.1002/tcr.201100038Endohedral metallofullerenes (EMFs) are a new class of metal-carbon hybrid materials formed by encapsulation of metals inside fullerene cavities. Structural determination of EMFs is of fundamental importance for understanding their intrinsic properties and the formation mechanism, and broadening their applications. An overview of the structure and chemistry of EMFs is presented with emphasis on: the determination of structures of paramagnetic EMFs, the first observation of the motion of cluster in a di-metal EMF, unambiguously established structures of carbide EMFs, recently obtained insoluble EMF species, and the chemical properties of various EMFs in terms of both covalent and supramolecular considerations as well as the dictating effect of internal metals.
The first reaction between hydrogen and a main-group compound under ambient conditions was reported in 2005. This unexpected result has been followed by numerous others which show that such reactivity is widespread in unsaturated and multiple bonded main-group species. These may react spontaneously not only with hydrogen, but also with ethylene, ammonia and related molecules. This account focuses on results from the author's laboratory but also on parallel work by other groups. The link between HOMO-LUMO separations, symmetry considerations and reactivity of the main-group species is emphasized as is their similarity in reactivity to transition-metal organometallic compounds.DOI 10.1002/tcr.201100016The reaction between hydrogen and a main-group compound under ambient conditions was first reported in 2005, and this unexpected result has been followed by numerous others which show that such reactivity is widespread in unsaturated and multiple bonded main-group species. These may react spontaneously not only with hydrogen, but also with ethylene, ammonia and related molecules. Illustrated here is the mechanism of the initial step of the activation of dihydrogen under ambient conditions by a main-group molecule (a digermyne).
Development of highly active catalysts has been an important research area in synthetic chemistry, especially from a practical point of view. Herein, we focus on the homogeneous catalytic hydrogenation using well-defined molecular catalysts and discuss recent advances in the field with regard to the turnover number for these catalysts. DOI 10.1002/tcr.201100019High, higher, highest! Homogeneous catalytic hydrogenation reactions using well-defined molecular catalysts with extremely high turnover numbers (on the order of millions) are concisely reviewed.
Posted on 12 December 2011 | 12:13 pm
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