Blue Ru (o-cat)(PPh3) 3 (5; o-cat= ortho-catecholate), obtained in 94% yield by reaction of RuCl2... more Blue Ru (o-cat)(PPh3) 3 (5; o-cat= ortho-catecholate), obtained in 94% yield by reaction of RuCl2 (PPh3) 3 (4) with dithallium catecholate, was characterized by NMR, MALDI-MS, IR, and single crystal X-ray analysis, and by a combined electronic spectroscopy and time-...
Nearly monodisperse CdSe nanoclusters, surface-passivated with a layer of trioctylphosphine and t... more Nearly monodisperse CdSe nanoclusters, surface-passivated with a layer of trioctylphosphine and trioctylphosphine oxide, have been sequestered within phosphine-containing domains in a diblock copolymer. A convergent approach to fabrication of these composites was ...
ABSTRACT Keeping Metathesis Simple The cover picture shows a clean, general, and highly efficient... more ABSTRACT Keeping Metathesis Simple The cover picture shows a clean, general, and highly efficient route to the three dominant ruthenium catalysts currently used for olefin metathesis. The Full Paper by D. E. Fogg et al. on p. 2020 ff., describes the synthesis of “second‐generation” Ru metathesis catalysts in ≥95% isolated yield and excellent purity, by reacting the PCy3 parent complexes with isolated free H2IMes, and using an ion‐exchange resin to sequester the liberated phosphine. Workup involves simply filtration and evaporation of the solvent. The speed, efficiency, generality and convenience of this methodology provides an attractive alternative to prior approaches based on in situ deprotonation or deprotection of imidazolinium derivatives.
... 8) Bemi, L.; Clark, HC; Davies, JA; Fyfe, CA; Wasylishen, RE J. Am. Chem. Soc.1982, 104, 438.... more ... 8) Bemi, L.; Clark, HC; Davies, JA; Fyfe, CA; Wasylishen, RE J. Am. Chem. Soc.1982, 104, 438. ... DFT Study. Christopher N. Rowley, Heather M. Foucault, Tom K. Woo and Deryn E. Fogg. Organometallics 2008 27 (8), 1661-1663. ...
Monocarbonyl complexes of ruthenium(II) support a wide range of catalytic processes. A survey of ... more Monocarbonyl complexes of ruthenium(II) support a wide range of catalytic processes. A survey of recent studies involving the well-known hydrido carbonyl catalyst RuHCl(PCy 3 ) 2 (CO), for example, reveals high activity in olefin hydrogenation and isomerization, 1-5 ...
A DFT study of the full catalytic cycle of olefin hydrogenation for the important catalyst system... more A DFT study of the full catalytic cycle of olefin hydrogenation for the important catalyst system RuHCl (L)(PR3) 2 reveals a hitherto unsuspected stabilizing function for bound dihydrogen and the favored operation of a Ru (IV), rather than a Ru (II), intermediate.
The diverse applications of acrylate metathesis range from synthesis of high-value α,β-unsaturate... more The diverse applications of acrylate metathesis range from synthesis of high-value α,β-unsaturated esters to depolymerization of unsaturated polymers. Examined here are unexpected side reactions promoted by the important Grubbs catalyst GII. Evidence is presented for attack of PCy3 on the acrylate olefin to generate a reactive carbanion, which participates in multiple pathways, including further Michael addition, proton abstraction, and catalyst deactivation. Related chemistry may be anticipated whenever labile metal-phosphine complexes are used to catalyze reactions of substrates bearing an electron-deficient olefin.
Introduction. During embryonic development, cells secrete an extracellular matrix (ECM) around th... more Introduction. During embryonic development, cells secrete an extracellular matrix (ECM) around themselves that is turn provides cues to the cells to direct organ development. The same ECM componants would therefore also be likely to direct repair and regeneration of these organs. Our goal, therefore, was to develop biomimetic materials that are ECM analogs, capable of sustaining a native-like ECM environment and interacting with host tissues and stem cells to effect regeneration. The human cornea can be thought of as an avascular, optically clear organ that comprises a stratified outermost epithelial layer and a a single innermost endothelial layer sandwiching a stroma that is comprised primarily of a hydrated ECM containing cells. The ECM is composed on mainly collagen (80%) and proteoglycans. So, specifically for corneal substitutes, we have developed a range of ECM substitutes as scaffolds for reconstruction of the cornea. This project is also very medically relevant as loss of v...
Blue Ru (o-cat)(PPh3) 3 (5; o-cat= ortho-catecholate), obtained in 94% yield by reaction of RuCl2... more Blue Ru (o-cat)(PPh3) 3 (5; o-cat= ortho-catecholate), obtained in 94% yield by reaction of RuCl2 (PPh3) 3 (4) with dithallium catecholate, was characterized by NMR, MALDI-MS, IR, and single crystal X-ray analysis, and by a combined electronic spectroscopy and time-...
Nearly monodisperse CdSe nanoclusters, surface-passivated with a layer of trioctylphosphine and t... more Nearly monodisperse CdSe nanoclusters, surface-passivated with a layer of trioctylphosphine and trioctylphosphine oxide, have been sequestered within phosphine-containing domains in a diblock copolymer. A convergent approach to fabrication of these composites was ...
ABSTRACT Keeping Metathesis Simple The cover picture shows a clean, general, and highly efficient... more ABSTRACT Keeping Metathesis Simple The cover picture shows a clean, general, and highly efficient route to the three dominant ruthenium catalysts currently used for olefin metathesis. The Full Paper by D. E. Fogg et al. on p. 2020 ff., describes the synthesis of “second‐generation” Ru metathesis catalysts in ≥95% isolated yield and excellent purity, by reacting the PCy3 parent complexes with isolated free H2IMes, and using an ion‐exchange resin to sequester the liberated phosphine. Workup involves simply filtration and evaporation of the solvent. The speed, efficiency, generality and convenience of this methodology provides an attractive alternative to prior approaches based on in situ deprotonation or deprotection of imidazolinium derivatives.
... 8) Bemi, L.; Clark, HC; Davies, JA; Fyfe, CA; Wasylishen, RE J. Am. Chem. Soc.1982, 104, 438.... more ... 8) Bemi, L.; Clark, HC; Davies, JA; Fyfe, CA; Wasylishen, RE J. Am. Chem. Soc.1982, 104, 438. ... DFT Study. Christopher N. Rowley, Heather M. Foucault, Tom K. Woo and Deryn E. Fogg. Organometallics 2008 27 (8), 1661-1663. ...
Monocarbonyl complexes of ruthenium(II) support a wide range of catalytic processes. A survey of ... more Monocarbonyl complexes of ruthenium(II) support a wide range of catalytic processes. A survey of recent studies involving the well-known hydrido carbonyl catalyst RuHCl(PCy 3 ) 2 (CO), for example, reveals high activity in olefin hydrogenation and isomerization, 1-5 ...
A DFT study of the full catalytic cycle of olefin hydrogenation for the important catalyst system... more A DFT study of the full catalytic cycle of olefin hydrogenation for the important catalyst system RuHCl (L)(PR3) 2 reveals a hitherto unsuspected stabilizing function for bound dihydrogen and the favored operation of a Ru (IV), rather than a Ru (II), intermediate.
The diverse applications of acrylate metathesis range from synthesis of high-value α,β-unsaturate... more The diverse applications of acrylate metathesis range from synthesis of high-value α,β-unsaturated esters to depolymerization of unsaturated polymers. Examined here are unexpected side reactions promoted by the important Grubbs catalyst GII. Evidence is presented for attack of PCy3 on the acrylate olefin to generate a reactive carbanion, which participates in multiple pathways, including further Michael addition, proton abstraction, and catalyst deactivation. Related chemistry may be anticipated whenever labile metal-phosphine complexes are used to catalyze reactions of substrates bearing an electron-deficient olefin.
Introduction. During embryonic development, cells secrete an extracellular matrix (ECM) around th... more Introduction. During embryonic development, cells secrete an extracellular matrix (ECM) around themselves that is turn provides cues to the cells to direct organ development. The same ECM componants would therefore also be likely to direct repair and regeneration of these organs. Our goal, therefore, was to develop biomimetic materials that are ECM analogs, capable of sustaining a native-like ECM environment and interacting with host tissues and stem cells to effect regeneration. The human cornea can be thought of as an avascular, optically clear organ that comprises a stratified outermost epithelial layer and a a single innermost endothelial layer sandwiching a stroma that is comprised primarily of a hydrated ECM containing cells. The ECM is composed on mainly collagen (80%) and proteoglycans. So, specifically for corneal substitutes, we have developed a range of ECM substitutes as scaffolds for reconstruction of the cornea. This project is also very medically relevant as loss of v...
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