The distinction between valence electrons and essentially inactive core electrons is the basis of many classifying concepts in chemistry. However, it has recently been recognized that this is an oversimplification and should, at least in some areas of chemistry, be modified. Many cases are known where cations with closed d10 configurations are subject to homoatomic interactions that influence structure and properties. A characteristic and surprisingly uniform structural feature (e.g., of a number of compounds containing monovalent coinage metals) is a clusterlike assembly of d10 cations that corresponds in geometry and bond lengths to fragments of the metal structures themselves. Further evidence for a special type of bonding in such compounds is provided by their physical properties; for example, the absorption in the UV/VIS region shows a drastic redshift and the compounds are often conductors or semiconductors. The d electrons in such cases have obviously lost their pure “core” nature. All bonding models so far proposed for such systems involve mixing of higher orbitals.

Homoatomic d10–d10 Interactions: Their Effects on Structure and Chemical and Physical Properties

Chemists today are increasingly fascinated by gold’s unique position in the family of elements. In this review, the author looks at important new results emerging from recent research in gold chemistry.

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The fascinating implications of new results in gold chemistry

Transition metals can assemble to form multinuclear complexes by engaging in direct metal-to-metal interactions. Metal–metal covalent bonds provide a large perturbation in electronic structure, relative to mononuclear metal ions, and the unique properties of these dinuclear fragments can be harnessed in a broad range of applications—for example, as chromophores in photochemical processes, redox centers in molecular electronics, or structural elements in metal–organic materials. There is a growing body of evidence that metal–metal bonds may also be formed under conditions relevant to catalysis and play a key role in transformations that were previously assumed to only involve mononuclear species. These findings have stimulated interest in characterizing multinuclear reaction pathways and developing well-defined multinuclear platforms as catalytic active sites. In this Perspective, we present case studies in this emerging area of catalysis research, emphasizing the impact of metal–metal bonding in either en...

Metal–Metal Bonds in Catalysis

In 2009, we reported C−halogen reductive elimination reactions from dinuclear Pd(III) complexes and implicated dinuclear intermediates in Pd(OAc)2-catalyzed C−H oxidation chemistry. Herein, we report results of a thorough experimental and theoretical investigation of the mechanism of reductive elimination from such dinuclear Pd(III) complexes, which establish the role of each metal during reductive elimination. Our results implicate reductive elimination from a complex in which the dinuclear core is intact and suggest that redox synergy between the two metals is responsible for the facile reductive elimination reactions observed.

/pdf/bimetallic-reductive-elimination-from-dinuclear-pd-iii-1ntelrt2bk.pdf

Bimetallic Reductive Elimination from Dinuclear Pd(III) Complexes

Phosphorus ylides are not only classical reagents in organic chemistry, but also play an increasingly important role as novel components in organometallic compounds. These metallic “ylide complexes” are either synthesized from “preformed ylides” and coordination compounds by addition or substitution, on the building block principle, or they are formed, in sometimes complicated reactions, from phosphanes, metal complexes, and C1 substrates in the coordination sphere of the metals. The resulting metal-carbon bonds are greatly modified in their properties by the immediate presence of the phosphonium center and often belong to the most stable of M-C structural units. The metal can come from any group of the periodic table, including the lanthanoids and actinoids. Numerous preparative and structural studies are gradually enabling us to gain an overall picture of the scope of this area of research.

Phosphorus Ylides in the Coordination Sphere of Transition Metals: An Inventory

Nonclassical Coordination Compounds

Ring opening of the [Au(CH2)2PPh2]2X4 (X = halogen) metallacycle. Cleavage of gold(III)-CH2 bonds

Experimental and Theoretical Studies of Dinuclear Gold(I) and Gold(II) Phosphorus Ylide Complexes.

Catalytic halogen exchange mediated by the dinuclear gold(I) complex [Au(CH2)2PPh2]2

Oxidative addition of methyl iodide to a dinuclear gold(I) complex. The x-ray crystal structure of bis[.mu.-(dimethyldimethylenephosphoranyl-C,C)]-iodomethyldigold(II)(Au-Au), Au2[(CH2)2P(CH3)2]2(CH3)I

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