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Zhou Z Sarova GH Zhang S Ou Z Tat FT Kadish KM Echegoyen L Guldi DM Schuster DI Wilson SR 《Chemistry (Weinheim an der Bergstrasse, Germany)》2006,12(16):4241-4248
Fullerene coordination ligands bearing one bipyridine or terpyridine unit were synthesized, and their coordination to ruthenium(II) formed linear rod-like donor-acceptor systems. Steady-state fluorescence of [Ru(bpy)(2)(bpy-C(60))](2+) showed a rapid solvent-dependent, intramolecular quenching of the ruthenium(II) MLCT excited state. Time-resolved flash photolysis in CH(3)CN revealed characteristic transient absorption changes that have been ascribed to the formation of the C(60) triplet state, suggesting that photoexcitation of [Ru(bpy)(2)(bpy-C(60))](2+) results in a rapid intramolecular transduction of triplet excited state energy. The electrochemical studies on both [Ru(bpy)(2)(bpy-C(60))](2+) and [Ru(tpy)(tpy-C(60))](2+) indicated electronic coupling between the metal center and the fullerene core. 相似文献
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Glöckner A Bannenberg T Büschel S Daniliuc CG Jones PG Tamm M 《Chemistry (Weinheim an der Bergstrasse, Germany)》2011,17(22):6118-6128
The transmetalation reaction between [(η(7) -C(7) H(7) )ZrCl(tmeda)] (1; tmeda=N,N,N',N'-tetramethylethylenediamine) and various phospholide anions leads to a new class of mixed sandwich complexes: [(η(7)-C(7)H(7))Zr(η(5)-C(4)PMe(4))] (2), [(η(7)-C(7)H(7))Zr(η(5)-C(4)PH(2)Me(2))] (3) and [(η(7)-C(7)H(7))Zr(η(5)-C(4)PPhHMe(2))] (4). The presence of Lewis basic phosphorus atoms and Lewis acidic zirconium atoms allows ambiphilic behaviour to be observed, and X-ray diffraction analysis reveals dimeric arrangements for 2 and 3 with long intermolecular Zr-P bonds, whereas 4 remains monomeric in the solid state. DFT calculations indicate that the metal-phosphorus interaction is weak, and accordingly, complexes 2-4 act as monodentate ligands upon reaction with [W(CO)(5)(thf)]. The resulting complexes [W(CO)(5)(L)] 5-7 (L=2-4) were studied by IR spectroscopy and compared with the [W(CO)(5) ] complex 9, containing the phosphane-functionalised trozircene [(η(7)-C(7)H(7))Zr(η(5)-C(5)H(4)PPh(2))] (8). They all show a close resemblance to simple phosphanes, such as PMe(3) , although molecular orbital analysis of 2 reveals that the free electron pair in the phosphatrozircenes is not the HOMO. Four equivalents of 2 can replace 1,4-cyclooctadiene (COD) in [Ni(cod)(2)] to form the homoleptic, distorted tetrahedral complex [Ni{2}(4)] (10). 相似文献
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Azomacrocyclic derivatives of imidazole: synthesis, structure, and metal ion complexation properties
New azocrown ethers comprising imidazoles in the macrocycle have been synthesized. Imidazole, 2-methyl-, 4-methyl-, and 4-phenylimidazole were incorporated to form macrocyclic units by coupling with the appropriate bis-diazonium salts. The syntheses were performed under high dilution conditions. The X-ray structure of a water adduct of the 21-membered crown ether derivative of 4-methylimidazole 8 has been solved. Metal cation binding was investigated with the use of UV-vis spectroscopy in acetonitrile, methanol, and methanol-water mixtures. The obtained chromoionophores were tested as ion-carriers in ion-selective membrane electrodes. 相似文献
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A. R. Kudinov D. A. Loginov S. N. Ashikhmin A. A. Fil'chikov L. s. Shul'pina P. V. Petrovskii 《Russian Chemical Bulletin》2000,49(9):1637-1639
30-Electron triple-decker complexes [(η-C5H5)Fe(μ-η:η-C4Me4P)Fe(η-C5Me5)]PF6 and [(η-C4Me4)Co(μ-η:η-C4Me4P)Fe(η-C5Me5)]PF6 with a central tetramethylphospholyl ligand were synthesized by stacking reactions of cationic fragments [(η-C5H5)Fe]+ and [(η-C4Me4)Co]+ with nonamethylphosphaferrocene (η-C4Me4P)Fe(η-C5Me5).
Published inIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 9, pp. 1647–1649, September, 2000. 相似文献
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Schenk WA Beucke T Burzlaff N Klüglein M Stemmler M 《Chemistry (Weinheim an der Bergstrasse, Germany)》2006,12(18):4821-4834
Ruthenium hydrogensulfido complexes [CpRu(P-P)(SH)] ((P-P)=Ph(2)PCH(2)PPh(2) (dppm), Ph(2)PC(2)H(4)PPh(2) (dppe)) were obtained from the corresponding chloro complexes by Cl/SH exchange. Condensation with a range of cinnamaldehydes gave thiocinnamaldehyde complexes [CpRu(P-P)(S=CH-CR(2)=CHR(1))]PF(6) (R(1)=C(6)H(4)X, R(2)=H, Me, X=H, OMe, NMe(2), Cl, NO(2)) as highly-colored crystalline compounds. The thiocinnamaldehyde complexes undergo [4+2]-cycloaddition reactions with vinyl ethers CH(2)=CHOR(3) (R(3)=Et, Bu) and styrenes H(2)C=CHC(6)H(4)Y (Y=H, Me, OMe, Cl, Br, NO(2)) to give complexes of 2,4,5-trisubstituted 3,4-dihydro-2H-thiopyrans as mixtures of two diastereoisomers. The rate of addition of para-substituted styrenes H(2)C=CHC(6)H(4)Y to [CpRu(dppm)(S=CH-CH=CHPh)]PF(6) increases in the series Y=NO(2), Br, Cl, H, Me, OMe, indicating that the cycloaddition is dominated by the HOMO(dienophile)-LUMO(diene) interaction. The strained dienophiles norbornadiene and norbornene also add, giving ruthenium complexes of 3-thia-tricyclo[6.2.1.0(2,7)]undeca-4,9-dienes and 3-thia-tricyclo[6.2.1.0(2,7)]undec-4-enes, respectively. Addition reactions with acrolein, methacrolein, methyl vinyl ketone, acrylic ester, or ethyl propiolate finally yielded ruthenium complexes of 3,4-disubstituted 3,4-dihydro-2H-thiopyrans and 4H-thiopyrans, respectively. 相似文献
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《Journal of Coordination Chemistry》2012,65(9):1539-1547
New tetranuclear compounds have been obtained by reacting binuclear complexes, [Zn2L n (μ-OH)(H2O)2](ClO4)2, with sodium dicyanamide (HL n are end-off bicompartmental ligands resulting from condensation between 2,6-diformyl-p-cresol with N,N-dimethyl-ethylenediamine or 2-aminomethyl-pyridine). The complexes, [{L1(μ-OH)Zn2}(μ 1,5-dca)2{Zn2(μ-OH)L1}](ClO4)2 (1) and [{Zn2L2(μ 3-OH)(dca)}2](ClO4)2?·?2H2O (2), have been characterized by single-crystal X-ray diffraction. The angular nature of the bridging dicyanamido induces the “M” shape of the tetranuclear cationic unit in 1. The tetranuclear cation, because of its particular shape, acts as a receptor toward one perchlorate ion, which is hydrogen bonded to the hydroxo groups. This tetranuclear unit in 2 has a defective heterocubane structure. The luminescence properties of the new tetranuclear complexes have been investigated. 相似文献
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E. V. Mutseneck D. A. Loginov A. A. Pronin P. V. Petrovskii A. R. Kudinov 《Russian Chemical Bulletin》2007,56(9):1927-1929
Cationic arene complexes [Cb*Co(naphthalene)]+ (2, Cb* = C4Me4) and [Cb*Co(phenanthrene)]+ were synthesized by the reactions of [Cb*Co(MeCN)3]+ with arenes. The [Cb*Co(anthracene)]+ complex was synthesized by the abstraction of the iodide ion from [Cb*CoI]2 by TIBF4 in the presence of anthracene. Complex 2 exchanges the naphthalene ligand for other arenes at room temperature.
Dedicated to Academician G. A. Abakumov on the occasion of his 70th birthday.
Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 9, pp. 1861–1863, September, 2007. 相似文献
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《Journal of Coordination Chemistry》2012,65(6):934-944
The reaction of pyridine-2,6-dicarbaldehyde or 2,6-diacetylpyridine with 1,2-bis(o-aminophenylthio)ethane (1) in acetonitrile in the presence of stoichiometric amounts of iron(II) perchlorate gave the complexes [(pyN3S2)FeII(ClO4)2] (4) and [(pyN3Me2S2)FeII(ClO4)2] (5) of the 15-membered N3S2 macrocyclic ligands, pyN3S2 ?=?{6,7-dihydro-15,19-nitrilobenzo(e,p)(1,4,7,15)dithiadiazacyclo-heptadecine-N,N′,N″,S,S′} and pyN3Me2S2?=?{6,7-dihydro-16,18-dimethyl-15,19-nitrilobenzo(e,p)(1,4,7,15)dithiadiazacyclo-heptadecine-N,N′,N″,S,S′}, respectively. Physical measurements led to the conclusion that these complexes contained seven-coordinate iron(II) and a single-crystal X-ray examination of 4 confirmed this. Coordination of the Fe(II) center in 4 is best described as distorted pentagonal-bipyramidal with the three nitrogen atoms and two sulfur donors of the macrocycle defining the pentagonal plane and the perchlorate ions occupying axial positions. Room temperature (293?K) magnetic moments of 4 and 5 (μ eff?=?4.9 and 4.7 B.M., respectively) are close to the value predicted for high-spin d6 systems. 相似文献
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Long J Wang X Zhang G Dong J Yan T Li Z Fu X 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(28):7890-7899
The reaction of ferrocene with the acidic hydroxy groups in the supercages of zeolite HY dehydrated at 673 K and the reactivity of the resultant surface species towards CO and O(2) were investigated by temperature-programmed decomposition (TPD) and reduction (TPR) and IR, X-ray absorption fine structure analysis (XAFS), and X-ray photoelectron (XP) spectroscopy. In situ FTIR, TPD, TPR, and chemical analysis reveal that the Cp(2)Fe molecule adsorbed on the zeolite surface loses one cyclopentadienyl group under vacuum at 423 K, which leads to the formation of a well-defined mononuclear surface Fe-C(5)H(6) complex grafted to two acidic sites and one ([triple bond]Si-O-Si[triple bond]) unit, as confirmed by the lack of Fe-Fe contributions in the EXAFS spectra. Each iron atom is coordinated, on average, to three oxygen atoms of the zeolite surface with a Fe--O distance of 2.00 A and to five carbon atoms with a Fe--C distance of 2.09 A. IR spectra indicate that the cyclopentadiene-iron species grafted on the surface of the zeolite is quite stable in vacuo or under an inert or hydrogen atmosphere below 423 K, and is also relatively stable under oxygen at room temperature. However, the cyclopentadiene ligand readily reacts with CO to form a compound containing carbonyl at 323 K, and even at room temperature. The single carbonyl band in the IR spectra provides evidence for the nearly uniform formation of a cyclopentadiene-iron species on the surface of the zeolite. 相似文献
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Dubberley SR Friedrich A Willman DA Mountford P Radius U 《Chemistry (Weinheim an der Bergstrasse, Germany)》2003,9(15):3634-3654
New mononuclear titanium and zirconium imido complexes [M(NR)(R'(2)calix)] [M=Ti, R'=Me, R=tBu (1), R=2,6-C(6)H(3)Me(2) (2), R=2,6-C(6)H(3)iPr(2) (3), R=2,4,6-C(6)H(2)Me(3) (4); M=Ti, R'=Bz, R=tBu (5), R=2,6-C(6)H(3)Me(2) (6), R=2,6-C(6)H(3)iPr(2) (7); M=Zr, R'=Me, R=2,6-C(6)H(3)iPr(2) (8)] supported by 1,3-diorganyl ether p-tert-butylcalix[4]arenes (R'(2)calix) were prepared in good yield from the readily available complexes [MCl(2)(Me(2)calix)], [Ti(NR)Cl(2)(py)(3)], and [Ti(NR)Cl(2)(NHMe(2))(2)]. The crystallographically characterised complex [Ti(NtBu)(Me(2)calix)] (1) reacts readily with CO(2), CS(2), and p-tolyl-isocyanate to give the isolated complexes [Ti[N(tBu)C(O)O](Me(2)calix)] (10), [[Ti(mu-O)(Me(2)calix)](2)] (11), [[Ti(mu-S)(Me(2)calix)](2)] (12), and [Ti[N(tBu)C(O)N(-4-C(6)H(4)Me)](Me(2)calix)] (13). In the case of CO(2) and CS(2), the addition of the heterocumulene to the Ti-N multiple bond is followed by a cycloreversion reaction to give the dinuclear complexes 11 and 12. The X-ray structure of 13.4(C(7)H(8)) clearly establishes the N,N'-coordination mode of the ureate ligand in this compound. Complex 1 undergoes tert-butyl/arylamine exchange reactions to form 2, 3, [Ti(N-4-C(6)H(4)Me)(Me(2)calix)] (14), [Ti(N-4-C(6)H(4)Fc)(Me(2)calix)] (15) [Fc=Fe(eta(5)-C(5)H(5))(eta(5)-C(5)H(4))], and [[Ti(Me(2)calix)](2)[mu-(N-4-C(6)H(4))(2)CH(2)]] (16). Reaction of 1 with H(2)O, H(2)S and HCl afforded the compounds [[Ti(mu-O)(Me(2)calix)](2)] (11), [[Ti(mu-S)(Me(2)calix)](2)] (12), and [TiCl(2)(Me(2)calix)] in excellent yields. Furthermore, treatment of 1 with two equivalents of phenols results in the formation of [Ti(O-4-C(6)H(4)R)(2)(Me(2)calix)] (R=Me 17 or tBu 18), [Ti(O-2,6-C(6)H(3)Me(2))(2)(Me(2)calix)] (19) and [Ti(mbmp)(Me(2)calix)] (20; H(2)mbmp=2,2'-methylene-bis(4-methyl-6-tert-butylphenol) or CH(2)([CH(3)][C(4)H(9)]C(6)H(2)-OH)(2)). The bis(phenolate) compounds 17 and 18 with para-substituted phenolate ligands undergo elimination and/or rearrangement reactions in the nonpolar solvents pentane or hexane. The metal-containing products of the elimination reactions are dinuclear complexes [[Ti(O-4-C(6)H(4)R)(Mecalix)](2)] [R=Me (23) or tBu (24)] where Mecalix=monomethyl ether of p-tert-butylcalix[4]arene. The products of the rearrangement reaction are [Ti(O-4-C(6)H(4)Me)(2) (paco-Me(2)calix)] (25) and [Ti(O-4-C(6)H(4)tBu)(2)(paco-Me(2)calix)] (26), in which the metallated calix[4]arene ligand is coordinated in a form reminiscent of the partial cone (paco) conformation of calix[4]arene. In these compounds, one of the methoxy groups is located inside the cavity of the calix[4]arene ligand. The complexes 24, 25 and 26 have been crystallographically characterised. Complexes with sterically more demanding phenolate ligands, namely 19 and 20 and the analogous zirconium complexes [Zr(O-4-C(6)H(4)Me)(2)(Me(2)calix)] (21) and [Zr(O-2,6-C(6)H(3)Me(2))(2)(Me(2)calix)] (22) do not rearrange. Density functional calculations for the model complexes [M(OC(6)H(5))(2)(Me(2)calix)] with the calixarene possessing either cone or partial cone conformations are briefly presented. 相似文献
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《Angewandte Chemie (International ed. in English)》2017,56(6):1671-1675
A synthetic approach to the sandwich complex [Cp′′′Co(η4‐P4)] ( 2 ) containing a cyclo‐P4 ligand as an end‐deck was developed. Complex 2 is the missing homologue in the series of first‐row cyclo‐Pn sandwich complexes, and shows a unique tendency to dimerize in solution to form two isomeric P8 complexes [(Cp′′′Co)2(μ,η4:η2:η1‐P8)] ( 3 and 4 ). Reactivity studies indicate that 2 and 3 react with further [Cp′′′Co] fragments to give [(Cp′′′Co)2(μ,η2:η2‐P2)2] ( 5 ) and [(Cp′′′Co)3P8] ( 6 ), respectively. Furthermore, complexes 2 , 3 , and 4 thermally decompose forming 5 , 6 , and the P12 complex [(Cp′′′Co)3P12] ( 7 ). DFT calculations on the P4 activation process suggest a η3‐P4 Co complex as the key intermediate in the synthesis of 2 as well as in the formation of larger polyphosphorus complexes via a unique oligomerization pathway. 相似文献
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Rosa Fandos Ana Rodríguez Pilar Terreros 《Journal of organometallic chemistry》2004,689(16):2641-2645
The early-late heterometallic complexes [TiCp∗((OCH2)2Py)(μ-O)M(COD)] (M = Rh, Ir) behave as four-electron donor ligands yielding the polynuclear cationic complexes [TiCp∗(OCH2)2 Py(μ-O){M(COD)}2]OTf (M = Rh (1), Ir (2)). The molecular structure of complex 1 has been established through an X-ray diffraction study. 相似文献
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M. A. Golubnichaya A. A. Sidorov I. G. Fomina M. O. Ponina S. M. Deomidov S. E. Nefedov I. L. Ermenko I. I. Moiseev 《Russian Chemical Bulletin》1999,48(9):1751-1756
Extraction of polymer (1), formed in the reaction of CoCl2 with KOOCBut, with boiling hexane gives crystals of hexamer Co6(μ3-OH)2(OOCBu1)10(HOOCBu1)4 (2). According to data of X-ray study, four Co11 atoms in the hexanuclear molecule2 have an octahedral ligand environment and two Co11 atoms have a tetrahedral one. Dissolution of polymer1 in EtOH results in its splitting into Co4(μ3-OH)2(OOCBu1)6(HOEt)6 tetramers (3). In molecule3, two asymmetric dimeric (η2-OOCBut)(EtOH)Co(μ-OOCBut)Co(HOEt)2 fragments are bound by two tridentate bridging OH groups.
Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 9, pp. 1773–1778, September, 1999. 相似文献