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1.
A series of new manganese(I) and ruthenium(II) monometallic and bimetallic complexes made of 2,2′-bipyridine and 1,10-phenanthroline ligands, [Mn(CO)3(NN)(4,4′-bpy)]+, [{(CO)3(NN)Mn}2(4,4′-bpy)]2+ and [(CO)3(NN)Mn(4,4′-bpy)Ru(NN)2Cl]2+ (NN = 2,2′-bipyridine, 1,10-phenanthroline; 4,4′-bpy = 4,4′-bipyridine) are synthesized and characterized, in addition to already known ruthenium(II) complexes [Ru(NN)2Cl(4,4′-bpy)]+ and [Cl(NN)2Ru(4,4′-bpy)Ru(NN)2Cl]2+. The electrochemical properties show that there is a weak interaction between two metal centers in Mn–Ru heterobimetallic complexes. The photophysical behavior of all the complexes is studied. The Mn(I) monometallic and homobimetallic complexes have no detectable emission. In Mn–Ru heterobimetallic complexes, the attachment of Mn(I) with Ru(II) provides interesting photophysical properties. 相似文献
2.
P. Sudhakar R. Srivijaya B.R. Sreekanth P.K. Jayanthi Peddy Vishweshwar Moses J. Babu K. Vyas Javed Iqbal 《Journal of Molecular Structure》2008,885(1-3):45-49
Robustness of carboxylic acid–pyridine supramolecular heterosynthon was examined in three 1:2 binary co-crystals of 4,4′-bipyridine with monocarboxylic acids, (4,4′-bipyridine)·(dl-hydroxyphenylacetic acid)2, 1; (4,4′-bipyridine)0.5·(4-bromonaphthalene-1-carboxylic acid), 2 and (4,4′-bipyridine)0.5·(4-methylbenzoic acid), 3. All the three co-crystals form “two-component supermolecules” (consisting of one molecule of 4,4′-bipyridine and two molecules of the relevant carboxylic acid) stabilized through carboxylic acid–pyridine heterosynthons. Co-crystals 1 and 2 exhibits the expected carboxylic acid–pyridine dimer (heterodimer I) whereas co-crystal 3 forms a novel carboxylic acid–pyridine catemer (heterocatemer II). 相似文献
3.
Peter A. Jenkins Susan Boland Paul Kavanagh Dnal Leech 《Bioelectrochemistry (Amsterdam, Netherlands)》2009,76(1-2):162
We are interested in investigating the applications of biocatalytic mediated reduction of oxygen by oxygenases in films on electrode surfaces, as such reactions can form the basis for biosensors or biocatalytic fuel cell development. Here we present approaches aimed at improving the stability and signal output of such films. These include selection of oxygen reducing biocatalysts which are active under physiological conditions and development of redox mediators which offer the opportunity to tailor the mediator to each enzyme. It was found that for each enzyme Melanocarpus albomyces laccase (MaL), Trametes hirsutus laccase (ThL) or bilirubin oxidase (MvBOD) it was the biocatalytic films mediated by Os(2,2′-bipyridine)2Cl·PVI that not only generated the highest current densities compared to Os(4,4′-dimethyl-2,2′-bipyridine)2Cl·PVI and Os(4,4′-dichloro-2,2′-bipyridine)2Cl·PVI, but also proved to be the most stable over 48 h. Under physiological conditions electrodes constructed from MvBOD generated the highest initial current densities for each of the osmium redox polymers, however these films proved to be the least stable over 48 h. Stability could be improved using surface pre-treatment. 相似文献
4.
Chun-Feng Yan Fei-Long Jiang Lian Chen Rui Feng Ming Yang Mao-Chun Hong 《Journal of solid state chemistry》2009,182(11):3162-3170
Assembly of 5-sulfosalicylic acid (H3L) and d10 transition metal ions (CdII, AgI) with the neutral N-donor ligands produces five new complexes: [Cd2(HL)2(4,4′-bipy)3]n·2nH2O (1), {[Cd2(μ2-HCO2)2(4,4′-bipy)2(H2O)4][Cd(HL)2(4,4′-bipy)(H2O)2]}n (2), {[Cd(4,4′-bipy)(H2O)4][HL]·H2O}n (3), [Cd(HL)(dpp)2(H2O)]n·4nH2O (4), {[Ag(4,4′-bipy)][Hhbs]}n (5) (4,4′-bipy=4,4′-bipyridine, dpp=1,3-di(pyridin-4-yl)propane, H2hbs=4-hydroxybenzenesulfonic acid, the decarboxylation product of H3L). Complex 1 adopts a 5-connected 3D bilayer topology. Complex 2 has the herring-bone and ladder chain, which are extended to a 3D network via hydrogen bonding. In 3–4 complexes, 3 is a 3D supermolecular structure formed by polymeric chains and 2D network of HL2−, while 4 gives the double-stranded chains. In 5, ladder arrays are stacked with the 2D networks of Hhbs− anions in an –ABAB– sequence. Complexes 1–4 display green luminescences in solid state at room temperature, while emission spectra of 3 and 4 show obvious blue-shifts at low temperature. 相似文献
5.
The combined use of 4,4′-bipyridine (4,4′-bipy) and 2-benzothiazolylthioacetic acid (HBTTAA) as ligands with Mn(II), Cd(II), Co(II) and Cu(II) ions afforded six polymeric complexes, namely {[Mn3(BTTAA)4(4,4′-bipy)4](ClO4)2 · 2H2O}n (1), [Mn(BTTAA)2(4,4′-bipy)2]n (2), [Cd(BTTAA)2(4,4′-bipy)2]n (3), [Cd(BTTAA)(4,4′-bipy)(NO3)(H2O)]n (4), [Co(BTTAA)2(4,4′-bipy)(H2O)2]n (5) and [Cu(BTTAA)2(4,4′-bipy)]n (6). All these complexes have been characterized by a combination of analytical, spectroscopic and crystallographic methods. Complex 1 is a novel 2D network formed by two different 44 grid networks, whereas isomorphous complexes 2 and 3 exhibit a 2Dl coordination architecture formed by the same 44 grid network. In 4–6, extended 1D chains are formed, with the 4,4′-bipy molecules acting as rigid rod-like links between adjacent metal centers. The carboxylato groups of BTTAA in these complexes exhibit four different coordination modes, namely monodentate, chelating, bridging and bridging-chelating modes. The magnetic properties of 1, 2, 5 and 6 were investigated in the temperature range 2.0–300.0 K. Variable temperature magnetic susceptibility measurements show weak antiferromagnetic interactions in these complexes. 相似文献
6.
Matthias Wolf David L. Yang Joseph L. Durant 《Journal of photochemistry and photobiology. A, Chemistry》1994,80(1-3):85-93
Combined experimental and theoretical studies of the reactions
and
were carried out in the present work. The rate constant of reaction (1) was investigated in the temperature range 293 K T612 K using the laser photolysis continuous-wave laser-induced fluorescence technique for the production and detection of NH2. The results are well described by k1(T)=5.43×T−4.02 exp(−1034K/T) cm3 molecule−1 s−1. Stationary points on the potential energy surface were characterized using the gaussian-2 (G2) ab initio method. The surface is complex, with hydrogen-atom transfers and cis—trans isomerization connecting five stable adduct species.The product distribution of reaction (2) was studied at room temperature using the discharge flow technique with mass spectrometric detection of the reaction products. Measured branching fractions for the production of N2O+H(D) were k2a/k2 = 0.84±0.4 for NH+NO and k2a/k2 = 0.87±0.17 for ND+NO. Stationary points on the ground 2A′ surface were calculated using the G2 method. The transition state energy for the dissociation of the cis isomer into H+N2O was found to be lower than the transition state energy for dissociation into OH+N2. Additionally, trans-HNNO was found to isomerize to cis-HNNO before dissociation.For reaction (3), the molecular properties of all relevant intermediates and transition states on the ground state potential energy surface were determined using the G2 method. The results predict the formation of three intermediates, H2NO, trans-HNOH and cis-HNOH, all exothermic relative to the reactants. The transition states separating these intermediates from one another and their products (H2+NO, H+HNO(1A′) or NH+OH) were also characterized, several for the first time. 相似文献
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7.
The reaction of Zn(acac)2 with btaH (1,2,3-benzotriazole) in dmf yielded the pentanuclear complex [Zn5(bta)6(acac)4(dmf)]·dmf (1·dmf). In the presence of pyrazine, the pentanuclear [Zn5(bta)6(acac)4(dmf)]·3.7dmf (2·3.7dmf) and enneanuclear [Zn9(bta)12(acac)6]·6dmf (3·6dmf) complexes were formed, whereas in the presence of 4,4′-bpy the 1D coordination polymer [Zn(acac)2(4,4′-bpy)]n (4) was isolated. The molecular structures of 1·dmf and 2·3.7dmf reveal that the [Zn5] clusters consist of four ZnII ions which span the corners of a tetrahedron and the fifth resides at its centre. The molecular structure of 3·6dmf reveals that the [Zn9] clusters consist of two corner sharing tetrahedra and the structure can be described as the addition of two [Zn5] clusters of 1·dmf and/or 2·3.7dmf followed by the simultaneous abstraction of [Zn(acac)2] and dmf molecules; this alternative was accomplished by recrystallization of 1·dmf from dmf which yielded 3·6dmf. Each of the μ3-κN:κN′:κN′′ benzotriazolate ligands in 1·dmf, 2·3.7dmf and 3·6dmf spans an edge of the tetrahedron. The molecular structure of 4 reveals mononuclear [Zn(acac)2] units bridged via 4,4′-bpy molecules to 1D coordination polymer. Characteristic IR bands of the four complexes are discussed in terms of the coordination modes of the ligands and known structures. 相似文献
8.
Georg Wolfbauer Alan M. Bond Glen B. Deacon Douglas R. MacFarlane Leone Spiccia 《Journal of Electroanalytical Chemistry》2000,490(1-2)
The electrochemical reduction of the black dye photosensitizer [(H3-tctpy)RuII(NCS)3]− (H3-tctpy=2,2′:6′,2′′-terpyridine-4,4′,4′′-tricarboxylic acid) used in photovoltaic cells has been found to be a complex process when studied in dimethylformamide. At low temperatures, fast scan rates and at a glassy carbon electrode, the chemically reversible ligand based one-electron reduction process [(H3-tctpy)Ru(NCS)3]−+e−[(H3-tctpy√−)Ru(NCS)3]2− is detected. This process has a reversible half-wave potential (Er1/2) of −1585±20 mV versus Fc/Fc+ at 25°C. Under other conditions, a deprotonation reaction occurs upon reduction, which produces [(H3−x-tctpyx−)Ru(NCS)3](1+x)− and hydrogen gas. Mechanistic pathways giving rise to the final products are discussed. The Er1/2-value for the ligand based reductions of the deprotonated complex is 0.70 V more negative than for [(H3-tctpy)Ru(NCS)3]−. Consequently, data obtained from molecular orbital calculations are consistent with the reaction [(H3-tctpy)Ru(NCS)3]−+e−→[(H2-tctpy−)Ru(NCS)3]2−+1/2H2 yielding the monodeprotonated complex as the major product obtained after electrochemical reduction of [(H3-tctpy)Ru(NCS)3]−. The Er1/2-values for the metal based RuII/III process differ by 0.30 V when data obtained for the protonated and deprotonated forms of the black dye are compared. Electronic spectra obtained during the course of experiments in an optically transparent thin layer electrolysis configuration are consistent with the overall reaction scheme proposed on the basis of voltammetric measurements and molecular orbital calculations. Reduction studies on the free ligand, H3-tcpy, are consistent with results obtained with [(H3-tctpy)Ru(NCS)3]−. 相似文献
9.
The complex [Pt(5,5′-dmbipy)Cl4] (1) (5,5′-dmbipy is 5,5′-dimethyl-2,2′-bipyridine) was prepared from the reaction of H2PtCl6·6H2O with 5,5′-dimethyl-2,2′-bipyridine in methanol. The same method was employed to make [Pt(6-mbipy)Cl4] (2) (6-mbipy is 6-methyl-2,2′-bipyridine). Both complexes were characterized by elemental analysis, IR, UV–Vis, 1H NMR, 13C NMR and 195Pt NMR spectroscopy. Their solid state structures were determined by the X-ray diffraction method. 相似文献
10.
Rajendra N. Goyal Arshi Rastogi 《Colloids and surfaces. A, Physicochemical and engineering aspects》1999,160(3):832
Linear sweep voltammetric behaviour of 9-β-
-ribofuranosyluric acid 5′-monophosphate (UA-9R-5′-P) has been studied in phosphate buffers of pH 3.0 and 7.0 at the pyrolytic graphite electrode in aqueous and micellar media. At pH 3.0 in the presence of non-ionic and anionic surfactants, UA-9R-5′-P exhibited a single well-defined 2e, 2H+ oxidation peak, whereas in the presence of cationic surfactant (CTAB) the oxidation peak Ia showed a tendency to split into two peaks indicating that the 2e, 2H+ oxidation of UA-9R-5′-P in peak Ia reaction occurs in two 1e steps. The effect of cationic surfactant at pH 3.0 is explained on the basis of hydrophobic penetration of cationic species in cationic micelles. The products of electrode reaction in micellar medium were found as alloxan, urea and ribosyl phosphate at pH 3.0 and ribose, allantoin and 5-hydroxyhydantoin 5-carboxamide at pH 7.0 and were similar to those observed in aqueous media. 相似文献
11.
The reaction of cis-[Pt](CCPh)2 {[Pt]=(bipy)Pt, (bipy′)Pt; BIPY=2,2′-bipyridine, bipy′=4,4′-dimethyl-2,2′-bipyridine} with different copper(I) and silver(I) salts [M′X] (M′=Cu, Ag; X=inorganic or organic ligand) produces alkynyl-bridged (hetero)bi-, tri-, tetra- or pentametallic transition metal complexes. The structural aspects and reaction chemistry of such species and the preference for one coordination mode over another is discussed. The interconversion and mechanistical aspects in the formation of the latter complexes is also reported. 相似文献
12.
Yu-Hui Wu Qing-Jiang Pan Xin Zhou Bao-Hui Xia Tao Liu Hong-Xing Zhang 《Journal of Molecular Structure》2008,860(1-3):111-118
The ground- and excited-state structures for a series of Os(II) diimine complexes [Os(NN)(CO)2I2] (NN = 2,2′-bipyridine (bpy) (1), 4,4′-di-tert-butyl-2,2′-bipyridine (dbubpy) (2), and 4,4′-dichlorine-2,2′-bipyridine (dclbpy) (3)) were optimized by the MP2 and CIS methods, respectively. The spectroscopic properties in dichloromethane solution were predicted at the time-dependent density functional theory (TD-DFT, B3LYP) level associated with the PCM solvent effect model. It was shown that the lowest-energy absorptions at 488, 469 and 539 nm for 1–3, respectively, were attributed to the admixture of the [dxy (Os) → π*(bpy)] (metal-to-ligand charge transfer, MLCT) and [p(I) → π*(bpy)] (interligand charge transfer, LLCT) transitions; their lowest-energy phosphorescent emissions at 610, 537 and 687 nm also have the 3MLCT/3LLCT transition characters. These results agree well with the experimental reports. The present investigation revealed that the variation of the substituents from H → t-Bu → Cl on the bipyridine ligand changes the emission energies by altering the energy level of HOMO and LUMO but does not change the transition natures. 相似文献
13.
Kenichi Maruyama Yuji Mishima Keiji Minagawa Junko Motonaka 《Journal of Electroanalytical Chemistry》2001,510(1-2)
A transition metal complex as an electrochemical probe of a DNA sensor must have an applicable redox potential, high binding affinity and chemical stability. Some complexes with the dipyrido[3,2-a:2′,3′-c]phenazine (DPPZ) ligand have been reported to have high binding affinity for DNA. However, it was difficult to detect the targeted DNA electrochemically using these complexes because of the relatively high redox potential. In this work, a combination of bipyridine ligands with functional groups (---NH2, ---CH3 and ---COOH) and the DPPZ ligand were studied. The introduction of electron-donating groups was effective for controlling the redox potential of the DPPZ-type osmium complex. The [Os(DA-bpy)2DPPZ]2+ complex (DA-bpy; 4,4′-diamino-2,2′-bipyridine) had a lower half-wave potential (E1/2) of 147 mV (vs. Ag AgCl) and higher binding affinity with DNA {binding constant, K=3.1×107 M−1 in 10 mmol dm−3 Tris–HCl buffer with 50 mmol dm−3 NaCl (pH 7.76)} than those of other complexes. With the single stranded DNA (ssDNA) modified gold electrode, the hybridization signal (ΔI) of the [Os(DA-bpy)2DPPZ]2+ complex was linear in the concentration range of 1.0 pg ml−1–0.12 μg ml−1 for the targeted DNA with a regression coefficient of 0.999. The detection limit was 0.1 pg ml−1. 相似文献
14.
H. Ratajczak J. Barycki A. Pietraszko J. Baran S. Debrus M. May J. Venturini 《Journal of Molecular Structure》2000,526(1-3)
-Histidinium dihydrogenarsenate orthoarsenic acid (LHA) crystal ;
belongs to P21 space group of the monoclinic system, Z=2, a=9.264(2) Å, b=8.929(2) Å, c=8.874(2) Å, β=108.61(3)°. The crystal is isomorphous to
(LHP) crystal. The H2AsO4− anions and H3AsO4 molecules are joined into layers parallel to the (100) crystallographic planes by the O–HO type hydrogen bonds. The histidinium cations occupy the space between the layers. The histidinium cation posses the carboxylic COO− group. The positive charges appear in the ring (the proton is attached to the =N(3)– nitrogen) and in the ammonium group. The differential scanning calorimetric (DSC) diagram does not show any phase transition till 100 K. The infrared spectrum fully confirms the X-ray crystal structure. The LHA crystal is a good second harmonic generator (0.46 relative to KDP) 相似文献
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15.
N-bromosuccinimide (NBS) oxidation of some substituted benzhydrols (4-Cl-, 4-Me-, 4-OMe-, 4-NO2−, 4,4′-dimethyl-, 4,4′-dichloro-, 4,4′-dimethoxy-, and 4-methyl-2-nitro-) yields corresponding benzophenones in the presence of Hg(OAc)2. The reaction is first-order in [NBS], [substrate], and [H+]. A study on the primary kinetic hydrogen isotope effect and solvent isotope effect suggest that C-H and O-H stretching frequencies are affected in the transition state. Activation parameters for the rate-determining step have been evaluated. The results are in accord with the linear free energy relationship (LFER). The linear plot of log(k
obs/k
0) vs. σ+ (ρ = −0.69)and Bunnett plots support the existence of proton-transfer in the rate-determining step. Rate behavior in different solvent compositions suggests dipolar-dipolar interaction in the absence of acid and ion-dipolar interaction in the presence of acid. Two different mechanisms have been suggested: cyclic transition state with unprotonated N-bromosuccinimide (NBS) in the absence of acid and noncyclic transition state with protonated NBS in the presence of acid.__________From Kinetika i Kataliz, Vol. 46, No. 3, 2005, pp. 360–365.Original English Text Copyright © 2005 by Hiran, Malkani, Rathore.This article was submitted by the authors in English. 相似文献
16.
Time-dependent density functional theory with quadratic response methodology is used in order to calculate and compare spin–orbit coupling effects and the main mechanism of phosphorescence of the neutral Ir(ppy)3 and cationic [Ir(bpy)3]3+ tris-iridium compounds, [Ir(ppy)2(bpy)]+ and [Ir(2-phenylpyridine)2(4,4′-tert-butyl-2,2′-bipyridine]+ complexes, including also the recently synthesised [Ir(2-phenylpyridine)2(4,4′-dimethylamino-2,2′-bipyridine]+ and [Ir(2,4-difluorophenylpyridine)2(4,4′-dimethylamino-2,2′-bipyridine]+ dyes, where ppy = 2-phenylpyridine and bpy = 2,2′-bipyridine ligands. Comparison with the symmetric, lighter and more studied [Ru(bpy)3]2+ and [Rh(bpy)3]3+ complexes is also presented. Variations in phosphorescence lifetimes for Ir(ppy)3 and [Ir(bpy)3]3+ dyes as well as for the mixed cationic complexes are well reproduced by the quadratic response method. All the ortho-metalated iridium compounds exhibit strong phosphorescence, which is used in organic light-emitting diodes (OLEDs) to overcome the efficiency limit imposed by the formation of triplet excitons. The results from the first principle theoretical analysis of phosphorescence have helped to clarify the connections between the main features of electronic structure and the photo-physical properties of the studied heavy organometallic OLED materials. 相似文献
17.
《Polyhedron》1995,14(23-24)
New complexes of bivalent nickel with isopropylxanthates and nitrogen-donor ligands of composition [Ni(Prixa)2(L)], [Ni(Prixa)2(L1)2], [Ni(L2)2](Prixa)2, and [Ni(L3)3] (Prixa)2 have been synthesized, where Prixa = i-C3H7OCS2−, L = 1,2-diaminopropane (1,2-pn), N,N,N′,N′=tetramethylethylenediamine (tmen) or 4,4′-bipyridine (4,4′-bipy), L1 = pyridine (py), L2 = diethylenetriamine (dien) and L3 = ethylenediamine (en), 1,2-diaminopropane or 1,10-phenanthroline (phen). The compounds have been characterized by elemental analysis, IR and UV-vis spectroscopy, magnetochemical measurements, molar conductivity and thermal analysis. The compounds containing the complex cation have been one-electron irreversibly oxidized using cyclic voltammetry. The crystal and molecular structures of [Ni(Prixa)2(tmen)] and [Ni(phen)3](Prixa)2 have been elucidated. 相似文献
18.
J. Kelber A. H. Reis Jr. A. T. Aldred M. H. Mueller O. MassenetG. DePasqualiG. Stucky 《Journal of solid state chemistry》1979,30(3)
BaVSe3 has been synthesized and its crystal structure determined at 293(2)°K. The structure was solved in the hexagonal space group P63/mmc (D46h), with a = 6.9990(11) and c = 5.8621(13) Å. Scans (2 Θ) of a polycrystalline sample revealed that BaVSe3 undergoes a transition to an orthorhombic unit cell (b′ 31/2 a, a′ a, c′ c) at 303(5)°K. Magnetic susceptibility measurements between 4 and 300°K indicate that BaVSe3 is paramagnetic down to 41(1)°K, where magnetic ordering occurs, with a magnetic moment in the ordered phase of 0.2 μB per vanadium atom. The orthorhombic lattice distortion may be caused by the “freezing in” of “soft” vibrational modes. 相似文献
19.
Murugan Indrani Ramasamy Ramasubramanian Sudalaiandi Kumaresan Sung Kwon Kang Min Chen Miao Du 《Polyhedron》2008,27(18):3593-3600
Two new coordination complexes, viz. [Co(tmb)2(4,4′-bpy)2(H2O)2](Htmb)2 (1) and {[Ni(tmb)2(μ-4,4′-bpy)2(H2O)2](4,4′-bpy)}n (2), have been hydrothermally synthesized by reaction of the corresponding metal acetate with 2,4,6-trimethylbenzoic acid (Htmb) and 4,4′-bipyridyl (4,4′-bpy). X-ray single-crystal diffraction suggests that complex 1 represents a discrete mononuclear species in which the central metal ion is coordinated by the terminal carboxylate moiety and the 4,4′-bipyridyl ligand. The crystal structure of complex 2 reveals a 1D chain coordination polymer in which the Ni(II) ions are connected by the bridging 4,4′-bipyridyl ligands. In both cases, the coordination arrays are further extended via hydrogen bonding interactions to generate 3D supramolecular networks. Complexes 1 and 2 have also been characterized by spectroscopic (IR and UV/Vis), thermal (TGA) and magnetic susceptibility measurements. In addition, both complexes exhibit antimicrobial activity. 相似文献
20.
Shu-Hua Zhang Yan-Ling Zhou Xiao-Jun Sun Lian-Qiang Wei Ming-Hua Zeng Hong Liang 《Journal of solid state chemistry》2009,182(11):2991-2996
Solvothermal reaction assisted with microwave leads to the formation of two unique heterometallic cubic clusters [Ni3M′(L)3(OH)(CH3CN)3]2·CH3CN (M′=K for 1 and M′=Na for 2, where L is an anion of 2-[(2-hydroxy-3-methoxy-benzylidene)-amino]-ethanesulfonate) with higher efficiency, yields and purity than those without it. The 6-metallacrown-3 [Ni3(OH)(L)3]− groups exhibit interesting ion trapping and self-assembly of size-different Na+ and K+ through form recognition and coordination activity in 1 and 2. The magnetic studies for 1 and 2 suggest that the {Ni3M′O4} (M′=K and Na) cores both display dominant ferromagnetic interactions from the nature of the binding modes of μ3-O (oxidophenyl) and μ3-OH. 相似文献