Structure and Spectroscopy of Copper−Dioxygen Complexes

Porphyrin-based photosensitizers for use in photodynamic therapy

The role of the lone pair of electrons of Pb(II) in determining the coordination geometry is analyzed from crystallographic studies and ab initio molecular orbital optimizations. Of particular interest are factors that contribute to the disposition of ligands around the lead with geometries that are (1) holodirected, in which the bonds to ligand atoms are distributed throughout the surface of an encompassing globe, and (2) hemidirected, in which the bonds to ligand atoms are directed throughout only part of an encompassing globe, i.e., there is an identifiable void in the distribution of bonds to the ligands. The preferred coordination numbers for lead were found to be 4 for Pb(IV) and 4 and 6 for Pb(II). All Pb(IV) structures in the CSD have a holodirected coordination geometry. Pb(II) compounds are hemidirected for low coordination numbers (2−5) and holodirected for high coordination numbers (9, 10), but for intermediate coordination numbers (6−8), examples of either type of stereochemistry are found. A...

Lone Pair Functionality in Divalent Lead Compounds

Functionalization of polyoxometalates: towards advanced applications in catalysis and materials science

In any artificial photosynthetic system, the oxidation of water to molecular oxygen provides the electrons needed for the reduction of protons or carbon dioxide to a fuel. Understanding how this four-electron reaction works in detail is important for the development of improved robust catalysts made of Earth-abundant materials, like first-row transition-metal oxides. Here, using time-resolved Fourier-transform infrared spectroscopy and under reaction conditions, we identify intermediates of water oxidation catalysed by an abundant metal-oxide catalyst, cobalt oxide (Co3O4). One intermediate is a surface superoxide (three-electron oxidation intermediate absorbing at 1,013 cm(-1)), whereas a second observed intermediate is attributed to an oxo Co(IV) site (one-electron oxidation intermediate absorbing at 840 cm(-1)). The temporal behaviour of the intermediates reveals that they belong to different catalytic sites. Knowledge of the structure and kinetics of surface intermediates will enable the design of improved metal-oxide materials for more efficient water oxidation catalysis.

Time-resolved observations of water oxidation intermediates on a cobalt oxide nanoparticle catalyst

This paper describes the synthesis and characterization of a series of iron octaethyltetraazaporphyrin complexes and a comparison of these substances to related iron porphyrins and phthalocyanines. Experimental evidence provided by magnetic susceptibility measurements, 1 H NMR, EPR, and Mossbauer spectroscopies, cyclic voltammetry, and/or X-ray crystallography indicates the tetraazaporphyrin ligand is a stronger a donor and π acceptor than is a porphyrin ligand

Iron octaethyltetraazaporphyrins: synthesis, characterization, coordination chemistry, and comparisons to related iron porphyrins and phthalocyanines

The complexes [tmtaa]Ti=O and [tmtaa]Ti=S have highly reactive Ti=O and Ti=S linkages and are demonstrated to undergo a number of new addition and cycloaddition reactions, and complex 1 has been found to be involved in a series of acid-base equilibria. Treatment with excess RO 3 SCF 3 (R=H, Me, SiMc 3 ) yields the bis(triflate) complex [tmtaa]Ti(O 3 SCF 3 ) 2 .

Addition and cycloaddition reactions of the nucleophilic oxo and sulfido complexes [tmtaa]Ti=X (X=O, S; tmtaa = dianion of 7,16-dihydro-6,8,15,17-tetramethyldibenzo[b,i][1,4,8,11]tetraazacyclotetradecine)

Homoscorpionate (Tris(pyrazolyl)borate) Ligands Containing Tethered 3-Phenyl Groups

Control of structure in lead(II) complexes using poly(pyrazolyl)borate ligands. Stereochemically inactive lone pair in octahedral [HB(3,5-Me2pz)3]2Pb (pz = pyrazolyl ring)

Poly(methylthiomethyl)borates : a new class of sulfur-rich ligands for metal ions

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