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A combined QM/MM study of ligand substitution enthalpies in the L2Fe(CO)3, RuCpL2Cl, and RuCp*L2Cl systems

A combined density functional and molecular mechanics approach (QM/MM) has been validated in a study of the substitution reactions: (i) (PH3)2Fe(CO)3 + 2ER3 mutually implies (ER3)2Fe(CO)3 + 2PH3 (ER3 = PMe3, PEt3, PMePh2, PPh3, PCyPh2, P(i)Pr3, PBz3, PCy3, AsEt3, AsPh3); and (ii) Cp’Ru(PH3)2Cl + 2ER3 mutually implies Cp’Ru(ER3)2Cl + 2PH3 (Cp’ = C5H5, C5(CH3)5; ER3 = PMe3, PEt3 P(n)Bu3, PMe2Ph, PMePh2, PPh3, AsEt3, P(OMe)3, P(OPh)3, P(OCH2)3CEt). The steric influence of the R substituents on the substitution enthalpies correlates well with experimental data. The combined QM/MM approach is also able to afford molecular structures in good accord with experimental estimates.

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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Synthesis and transition metal complexes of 1,1?-bis(diphenylethynylphosphino)ferrocene

The new ferrocene based bisphosphine [Fe{C5H4P(C[tbnd]CPh)2}2] (1) was synthesized in 82% yield by the treatment of bis(dichlorophosphino)ferrocene [Fe(C5H4PCl2)2] with four equivalents of lithium phenylacetylide. The reactions of 1 with aq. H2O2, elemental sulfur or selenium afforded bis(chalcogenide) derivatives, [Fe{C5H4P(E)(C[tbnd]CPh)2}2] (2 E = O, 3 E = S, 4 E = Se). The reaction of 1 with [M(NC5H11)2(CO)4] (M = Mo, W), [RuCp(PPh3)2Cl] and [M(COD)Cl2] (M = Pd, Pt) resulted in the formation of the respective chelate complexes, [Fe{C5H4P(C[tbnd]CPh)2}2{M(CO)4}] (5 M = Mo, 6 M = W), [Fe{C5H4P(C[tbnd]CPh)2}2{RuCp(Cl)}] (8) and [Fe{C5H4P(C[tbnd]CPh)2}2{MCl2}] (9 M = Pd, 10 M = Pt), whereas the reaction of 1 with [Ru(eta6-p-cymene)Cl2]2 and [AuCl(SMe2)] yielded the corresponding bimetallic complexes [Fe{C5H4P(C[tbnd]CPh)2}2{RuCl2(eta6-p-cymene)}2] (7) and [Fe{C5H4P(C[tbnd]CPh)2}2{AuCl}2] (15). The reactions between 1 and CuX in equimolar ratios also yielded binuclear complexes, [Fe{C5H4P(C[tbnd]CPh)2}2{CuX}2] (11 X = Cl, 12 X = Br, 13 X = I), whereas [Cu(CH3CN)4]BF4 yielded the cationic complex [(Fe{C5H4P(C[tbnd]CPh)2}2)2Cu]BF4 (14). All the compounds were characterized by spectroscopic methods and the structures of complexes 1, 5, 6, 8, 10, 13 and 14 were confirmed by single crystal X-ray diffraction studies.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Valence tautomerism in titanium enolates: Catalytic radical haloalkylation and application in the total synthesis of neodysidenin

(Chemical Equation Presented) A direct ruthenium-catalyzed radical chloroalkylation of N-acyl oxazolidinones capitalizing on valence tautomerism of titanium enolates has been developed. The chloroalkylation method served as the centerpiece in the enantioselective total synthesis of trichloroleucine-derived marine natural product neodysidenin.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Complexes of the Platinum Metals. Part 29. Pyridine-2-thiolate Derivatives of Ruthenium and Osmium: X-Ray Crystal Structures of and

Ruthenium and osmium precursors , , , , , and react with pyridine-2-thiol (pySH) or dipyridyl-2,2′-disulphide (pySSpy) in boiling benzene or toluene to afford a range of pyridin-2-thiolate complexes including , (2 isomers), , , and in which the pyridin-2-thiolate ligands are bound in monodentate (S-bonded) or bidentate (N,S-chelated) mode.Similar products are obtained from and in the presence of triethylamine and pyridine-2-thiol.The new complexes have been characterised by i.r. and n.m.r. (31P-<1H> and 1H) spectroscopy; reaction pathways are discussed.The X-ray crystal structures of and have been determined.The dicarbonyl , which undergoes facile conversion to , displays structural evidence of incipent attack by the non-co-ordinated N atom of the monodentate pyridine-2-thiolate ligand on a carbonyl group .Crystals of are monoclinic, space group P21/c, with a = 11.307(2), b = 11.083(3), c = 24.090(5) Angstroem, beta = 109.47(2) deg, and Z = 4.The structure, which has been refined to R = 0.045 for 4375 observed reflections, consists of highly distorted octahedral ruthenium(II) molecules with monodentate (S-bonded) and bidentate (N,S-bonded) pyridine-2-thiolate ligands, a cis pair of carbonyl groups, and a triphenylphosphine ligand trans to the S-bonded pyridin-2-thiolate.Crystals of are triclinic, space group P1, with a = 10.317(3), b = 11.749(3), c = 12.517(3) Angstroem, alpha = 67.65(2), beta = 70.55(2), gamma = 86.43(2) deg, and Z = 2.The structure, which has been refined to R = 0.040 for 12196 observed reflections consists of highly distorted octahedral ruthenium(II) molecules with a cis pair of bidentate (N,S-bonded) pyridine-2-thiolate ligands (trans S atoms), a carbonyl group, and a triphenylphosphine ligand.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Cyclopentadienyl-ruthenium and -osmium complexes VII. Formation and properties of ion-pairs containing the dihydride (eta-cyclopentadienyl)bis(triphenylphosphine)-ruthenium(IV) cation

The + cation in the simple and fast reaction of CpRuH(PPh3)2 with organic sulphonic acids in polar solvents (methanol, acetone) has been obtained in the form of ion-pairs.The reaction runs for several minutes, with practically quantitative yields.The dihydride complex cation obtained may be isolated from polar solutions as a sparingly soluble ion-pair with the tetraphenylborate anion.In the ion-pairs a reduction-elimination process slowly proceeds with the formation of non-ionic compounds of the CpRu(sulphonate)(PPh3)2 type.Also, the effect of methyl substituents in the Cp-ring on shifts in the 31P NMR signals and MS(FD) investigations of the new compounds obtained have been described.Explanation of the new group signals in the MS(FD) spectra as originating from the fragments formed, containing two ruthenium atoms ?-bonded to the phenyl ring of BPh4, i.e. +, were proposed.In the case of compounds containing the PPh3 molecule, a similar phenomenon occurs.For fragments obtained in the MS(FD) spectra, the formula + was ascribed.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

32993-05-8, Name is Chlorocyclopentadienylbis(triphenylphosphine)ruthenium(II), molecular formula is C41H35ClP2Ru, belongs to ruthenium-catalysts compound, is a common compound. In a patnet, once mentioned the new application about 32993-05-8, Recommanded Product: 32993-05-8

Easy hydrolysis of white phosphorus coordinated to ruthenium

The P4 molecule bound to ruthenium as an eta1- ligand in [CpRu(PPh3)2(eta1-P4)]Y (Y = PF6, CF3SO3) undergoes an easy reaction with water in exceedingly mild conditions to yield PH3, which remains coordinated to the [CpRu(PPh3)2] fragment, and oxygenated derivatives. The Royal Society of Chemistry 2005.

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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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DIASTEREOMERIC CHIRAL DIPHOSPHINE CHLORO(eta5-CYCLOPENTADIENYL)-RUTHENIUM(II) COMPLEXES AND THE CRYSTAL STRUCTURE OF <(S)RuCl(eta5-C5H5)<(R)Ph2PCH(Me)CH2PPh2>>

Diastereomeric > chelate complexes (where R=CH3, cyclo-C6H11, or C6H5) from in nearly equimolar amounts in the displacement reaction of triphenylphosphine form .The diastereomers were separated by fractional crystallization.Diastereomeric composition at the equilibrium showed a low asymmetric induction (28-41percent) by the optically active diphosphine ligand on the chiral ruthenium atom.The absolute configuration at the ruthenium atom has little influence on the chiroptical properties of the complexes, which appear to be dominated, at least in the visible region, by the chiral conformation of the chelate ligand.The crystal structure of the title diastereomer, <(S)RuCl(eta5-C5H5)-<(R)Ph2PCH(Me)CH2PPh2>>, has been investigated.It is monoclinic, space group P21, with a=9.688(3), b=15.037(4), c=10.556(2) Angstroem, beta=113.54(2)deg, and Z=2.The structure was solved by Patterson and Fourier methods, and refined by least squares on the basis of 2 000 significant counter data, to a final R value of 0.042.The complex shows a distored lambda conformation of the diphosphine ligand in the chelate five-membered ring, in the solid state.The Ru-Cl and Ru-P interactions are 2.444(2) and 2.277 Angstroem (mean value), respectively.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

The reaction rate of a catalyzed reaction is faster than the reaction rate of the uncatalyzed reaction at the same temperature.14564-35-3, Name is Dichlorodicarbonylbis(triphenylphosphine)ruthenium(II), molecular formula is C38H34Cl2O2P2Ru. In a Article£¬once mentioned of 14564-35-3, Recommanded Product: 14564-35-3

RuCl2(PPh3)3 catalyzed liquid phase hydroformylation of propene under mild pressure conditions in alcoholic media: Isolation and characterization of species separated out during the reaction

Dichlorotris(triphenylphosphine)ruthenium(II), RuCl2(PPh3)3, catalyzed liquid phase hydroformylation of propene was carried out in ethanol. Mixture of two complexes, which get separated, were observed to form along with hydroformylation products under mild pressure of 9 bar at 175 C. These two complexes were identified as dicarbonylchlorohydridobis(triphenylphosphine)ruthenium(II), HRuCl(CO)2(PPh3)2 and dicarbonyldichlorobis(triphenylphosphine)ruthenium(II), RuCl2(CO)2(PPh3)2 which have been isolated and characterized. The crystal structure of one of the intermediates as determined by single crystal X-ray diffraction established this as cis form of RuCl2(CO)2(PPh3)2. The isolated complexes were found to be inactive towards hydroformylation of propene. A possible mechanism for the formation of these intermediate species and lower conversion for hydroformylation products is discussed.

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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Organometallic complexes for nonlinear optics: Part 19. Syntheses and molecular quadratic hyperpolarizabilities of indoanilino-alkynyl-ruthenium complexes

The terminal alkyne 4-HCCC6H4N=CCH=CtBuC(O)CtBu=CH (1) and ruthenium complex derivatives trans-[Ru(CC-4-C6H4N=CCH=CtBuC(O)C tBu=CH}Cl(dppm)2] (2) and [Ru{CC-4-C6H4N=CCH=CtBuC(O)C tBu=CH}(PPh3)2(eta-C5H 5)] (3) have been synthesized. An X-ray structural study of 3 reveals the expected equivalent C-C bond lengths of the phenyl and alternating C-C and C=C bond lengths of the quinonal ring in the indoanilino-alkynyl ligand; there is a dihedral angle of 47.59 between the phenyl and quinonal rings, probably a result of ortho-hydrogen repulsion. Metal-centred oxidation potentials of 2 and 3 are similar to those of ‘extended chain’ 4-nitroaryl-alkynyl complex analogues. Irreversible quinonal ring-centred reductions occur at significantly more negative potentials than the quasi-reversible reductions in their nitro-containing analogues. Quadratic optical nonlinearities by hyper-Rayleigh scattering at 1064 nm for 2 (417¡Á10-30 esu) and 3 (658¡Á10-30 esu) are both large, but resonance enhanced. Two-level-corrected nonlinearities for these complexes (124¡Á10-30, 159¡Á10-30 esu, respectively) are also large, despite the presence of electron-donating tert-butyl groups reducing the efficiency of the (formally) electron-accepting quinonal ring in these donor-bridge-acceptor complexes.

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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI

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Ruthenium-Catalyzed Heck-Type Alkenylation of Alkyl Bromides

The complex [CpRuCl(PPh3)2] displays a high catalytic activity for the Heck-type alkenylation of alkyl bromides in the first example using this metal under thermal conditions. The coupling reaction proceeds efficiently with a variety of functionalized tertiary, secondary, and primary alkyl bromides. The presence of Huenig’s base has been revealed to be crucial for this transformation. Preliminary mechanistic studies support the participation of alkyl radicals in the reaction.

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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI