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Publications associées (209)

Copper-Catalyzed Alkylation of Benzoxazoles with Secondary Alkyl Halides

Rosario Scopelliti, Xile Hu, Isuf Salihu, Peng Ren

Copper-catalyzed direct alkylation of benzoxazoles using nonactivated secondary alkyl halides has been developed. The best catalyst is a new copper(I) complex (1), and the reactions are promoted by bis[2-(N,N-dimethylamino)ethyl] ether. ...

American Chemical Society2012

Synthesis, Reactivity, and Catalytic Application of a Nickel Pincer Hydride Complex

Rosario Scopelliti, Xile Hu, Jan Breitenfeld

The nickel(II) hydride complex [(MeN2N)Ni-H] (2) was synthesized by the reaction of [(MeN2N)Ni-OMe] (6) with Ph2SiH2 and was characterized by NMR and IR spectroscopy as well as X-ray crystallography. 2 was unstable in solution, and it decomposed via two re ...

American Chemical Society2012

Synthesis and electronic properties of a pentafluoroethyl-derivatized nickel pincer complex

Oleg Vechorkin, Xile Hu, Peng Ren

The synthesis of a bis(amino)amide nickel pincer complex bearing a perfluoroethyl ligand was effected by reaction of the corresponding nickel chloride complex with cesium fluoride and trimethyl(pentafluoroethyl)silane. Electrochemical experiments revealed ...

Royal Society of Chemistry2012

Fe, Co, and Ni Ions Promote the Catalytic Activity of Amorphous Molybdenum Sulfide Films for Hydrogen Evolution

Stéphane Fierro, Lorenzo Rovelli, Xile Hu, Heron Vrubel, Daniel Andreas Merki

Molybdenum sulfide materials had been shown as promising non-precious catalysts for hydrogen evolution. This paper describes the study of the promotional effect of certain transition metal ions on the activity of amorphous MoS3 films. Ternary metal sulfide ...

2012

A Pyridinol Acyl Cofactor in the Active Site of [Fe]-hydrogenase Evidenced by the Reactivity of Model Complexes

Xile Hu, Dafa Chen, Bowen Hu

The decomposition reaction of a water-soluble complex (see scheme; 1) in H2O confirms the existence of a unique bidentate pyridinol cofactor in [Fe]-hydrogenase. This unique moiety is confirmed for the first time by the decomposition of a well-defined mode ...

Wiley-V C H Verlag Gmbh2012

Hydrogen evolution catalyzed by MoS3 and MoS2 particles

Xile Hu, Heron Vrubel, Daniel Andreas Merki

Amorphous MoS3 particles are prepared using a simple chemical method. Several deposition techniques are developed to fabricate electrodes loaded with MoS3 particles. These electrodes are highly active for hydrogen evolution. The catalytically active specie ...

2012

Reversible protonation of a thiolate ligand in an [Fe]-hydrogenase model complex

Rosario Scopelliti, Xile Hu, Dafa Chen

The thiolate ligand in the five-coordinate model complex 1 of [Fe]-hydrogenase is preferentially and reversibly protonated, even in the presence of an acyl ligand. The results suggest that the Cys176 thiolate ligand in [Fe]-hydrogenase can serve as the int ...

Wiley-VCH Verlag GmbH2012

Amorphous Molybdenum Sulfide Films as Catalysts for Electrochemical Hydrogen Production in Water

Stéphane Fierro, Xile Hu, Heron Vrubel, Daniel Andreas Merki

Amorphous molybdenum sulfide films are efficient hydrogen evolution catalysts in water. The films are prepared via simple electro-polymerization procedures and are characterized by XPS, electron microscopy and electronic absorption spectroscopy. Whereas th ...

2011

Cross coupling of non-activated alkyl halides with alkynyl Grignard reagents catalyzed by a well-defined Ni pincer complex

Rosario Scopelliti, Aurélien Godinat, Oleg Vechorkin, Xile Hu

The nickel pincer complex 1 catalyzes the cross-coupling of the title compounds with remarkable substrate scope and functional group tolerance. A nickel/alkynyl species was isolated and shown to be catalytically competent. THF=tetrahydrofuran, O-TMEDA=bis[ ...

Wiley-VCH Verlag GmbH2011

Pd, Pt, and Ru complexes of a pincer bis(amino)amide ligand

Rosario Scopelliti, Oleg Vechorkin, Xile Hu, Isuf Salihu, Peng Ren

An improved synthesis of pincer ligand bis[(2-dimethylamino)phenyl]amine (MeN2NH) was reported. Reaction of the Li complex of MeN2N with suitable Pd, Pt, and Ru precursors gave the corresponding metal complexes. The structures of the Pd, Pt, and Ru complex ...

Royal Society of Chemistry2011

A Five-Coordinate Iron Center in the Active Site of [Fe]-Hydrogenase: Hints from a Model Study

Rosario Scopelliti, Xile Hu, Dafa Chen

The synthesis, structure, and reactivity of a five-coordinate model complex of [Fe]-hydrogenase are described. The work suggests that the iron center in [Fe]-hydrogenases could be five-coordinate in the resting state. ...

Wiley-VCH Verlag GmbH2011

Recent developments of molybdenum and tungsten sulfides as hydrogen evolution catalysts

Xile Hu, Daniel Andreas Merki

Recent work shows that nanoparticulate and amorphous molybdenum and tungsten sulfide materials are active catalysts for hydrogen evolution in aqueous solution. These materials hold promise for applications in clean hydrogen production technologies. In this ...

Royal Society of Chemistry2011

Amorphous transition metal sulphide films or solids as efficient electrocatalysts for hydrogen production from water or aqueous solutions

Xile Hu, Heron Vrubel, Daniel Andreas Merki

The present invention relates to metal electrocatalysts for hydrogen production from water or aqueous solutions and use thereof in electrodes and electrolysers. ...

2011

Ni-catalyzed cross coupling of non-activated alkyl halides: a mechanistic perspective

Xile Hu

Cross coupling of non-activated alkyl halides is a potentially transformative methodology in organic synthesis. Herein we review the recent development of nickel-catalyzed coupling of non-activated alkyl halides. The current understanding of the mechanism ...

2011

Hydrogen evolution at polarised liquid/liquid interfaces catalyzed by molybdenum disulfide

Hubert Girault, Xile Hu, Imren Hatay, Heron Vrubel, Peiyu Ge

Molybdenum disulfide microparticles in suspension in an aqueous acidic solution adsorb at the interface with an organic electrolyte solution containing the reducing agent, decamethylferrocene, to catalyse hydrogen evolution. This catalytic process has been ...

2011

A Structure-Activity Study of Ni-Catalyzed Alkyl-Alkyl Kumada Coupling. Improved Catalysts for Coupling of Secondary Alkyl Halides

Rosario Scopelliti, Oleg Vechorkin, Xile Hu, Peng Ren, Kim Dimuth Von Allmen

A structure–activity study was carried out for Ni catalyzed alkyl–alkyl Kumada-type cross coupling reactions. A series of new nickel(II) complexes including those with tridentate pincer bis(amino)amide ligands (RN2N) and those with bidentate mixed amino-am ...

2011

Synthesis and Characterization of a Series of Model Complexes of the Active Site of [Fe]-Hydrogenase (Hmd)

Rosario Scopelliti, Xile Hu, Dafa Chen

A series of Fe complexes were synthesized and characterized as small molecule mimics for the active site of [Fe]-hydrogenase (Hmd). The collection includes both structurally new compounds and analogues of previously reported models. These complexes contain ...

2011

Why are (NN2)Ni pincer complexes active for alkyl-alkyl coupling: ß-H elimination is kinetically accessible but thermodynamically uphill

Rosario Scopelliti, Anne-Clémence Corminboeuf, Oleg Vechorkin, Xile Hu, Jan Breitenfeld

Isomerization and olefin exchange experiments show that β-H elimination is kinetically viable but thermodynamically unfavorable in [(MeNN2)Ni-alkyl] complexes. The intermediacy of Ni-hydride species was corroborated by a trapping experiment. The alkyl comp ...

American Chemical Society2010

Synthesis and Reactivity of Iron Acyl Complexes Modeling the Active Site of [Fe]-Hydrogenase

Rosario Scopelliti, Xile Hu, Dafa Chen

A [FeIIFeII] dithiolate complex containing acyl and carbonyl ligands was synthesized. The diiron complex reacted with phosphine, cyanide, isocyanide, and CO to give monomeric FeII complexes reproducing the first coordination sphere of the active site of [F ...

2010

[Fe]-Hydrogenase Models Featuring Acylmethylpyridinyl Ligands

Rosario Scopelliti, Xile Hu, Dafa Chen

The synthesis, structure, and reactivity of small-molecule models of [Fe]-hydrogenase are described. These models feature the intriguing acylmethylpyridinyl ligands found exclusively in the enzyme. ...

Wiley-VCH Verlag GmbH2010

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