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Wei-Zhong Chen

Publications and source records attributed to Wei-Zhong Chen.

12 recordsLinked to original sources

Symmetric and unsymmetric "dumbbells" of Ru2-alkynyl units via C-C bond formation reactions.

Oxidative homocoupling (Glaser) reaction of Ru2 compounds bearing peripheral ethyne resulted in symmetric dimers. Cross-coupling (Sonogashira) reaction between Ru2 compounds bearing peripheral iodo and ethyne groups yielded an unsymmetric dimer. Voltammetric data indicated that Ru2 units in the symmetric dimers are noninteracting, and the unsymmetric dimer is best described as a weakly coupled push-pull compound.

Journal Article↗

Preparation and characterization of a family of Ru2 compounds bearing iodo/ethynyl substituents on the periphery.

A high-yield synthesis of mixed-bridging-ligand Ru2 compounds, Ru2(D(3,5-Cl2Ph)F)(4-n)(OAc)nCl [n = 1 (1) and 2 (2)] was developed, where D(3,5-Cl2Ph)F is bis(3,5-dichlorophenyl)formamidinate. The acetate ligands in 1 and 2 can be quantitatively displaced with DMBA-I to yield Ru2(D(3,5-Cl2Ph)F)3(DMBA-I)Cl (3) and Ru2(D(3,5-Cl2Ph)F)2(DMBA-I)2Cl (4), respectively, where DMBA-I is N,N'-dimethyl-4-iodobenzamidinate. When compound 2 was treated with 1 equiv of HDMBA-I, a unique Ru2 compound containing three different types of bidentate bridging ligands, cis-Ru2(D(3,5-Cl2Ph)F)2(DMBA-I)(OAc)Cl (5), was obtained. Subsequent reactions between 3/4 and (trimethylsilyl)acetylene under Sonogashira coupling conditions resulted in Ru2(D(3,5-Cl2Ph)F)(4-n)(DMBA-C[triple bond]CSiMe3)nCl [n = 1 (6) and 2 (8)] in excellent yields, which were converted to the corresponding bis(phenylacetylide) compounds Ru2(D(3,5-Cl2Ph)F)(4-n)(DMBA-C[triple bond]CSiMe3)n(C[triple bond]CPh)2 [n = 1 (7) and 2 (9)]. Structural studies of several compounds provided insights about the change in Ru2 coordination geometry upon the displacement of bridging and axial ligands. Voltammetric studies of these compounds revealed rich redox characteristics in all Ru2 compounds reported and a minimal electronic perturbation upon the peripheral Sonogashira modification.

Journal Article↗

Cu2{[18]ane-N6} complexes: structures, magnetism, and phosphate monoester binding.

A novel Cu(II)2 complex of the [18]ane-N6 macrocycle ([18]ane-N6 = 1,4,7,10,13,16-hexaazacyclooctadecane) was prepared from the reaction between [18]ane-N6 and Cu(II) salts such as Cu(NO3)2 and Cu(OAc)2. A structural study of the complex derived from Cu(OAc)2 (1) revealed a Cu(II)2 core encircled by a [18]ane-N6 ligand and two mu-O-OAc ligands. The facile replacement of mu-O-OAc by a phosphate monoester [PO3(OR)2-] yielded a number of bis(phosphate monoester)dicopper complexes with ROPO3(2-) as hydrogen phosphate (HPO4(2-), 3a), phenyl phosphate [PO3(OPh)2-, 3b], glycerol 2-phosphate [PO3(OCH(CH2OH)2)2-, 3c], alpha-d-gluocose phosphate [PO3(C6H11O6)2-, 3d], and dl-alpha-glycerol phosphate [PO3(OCH2CHOHCH2OH)2-, 3e]. Structural studies of compounds 3a-d confirmed both the retention of the Cu2{[18]ane-N6} core and a mu-O-PO3(OR) coordination mode. Displacement of acetate by a phosphate monoester in an aqueous solution was accompanied by a significant change in the visible absorption, which enables the establishment of relative association constants of PO3(OR)2- on the order of 10(4) in the unbuffered solution and 10(3) in the buffered solution (HEPES). Measurement of the magnetic susceptibility of compound 3a over the temperature range of 5-300 K and subsequent modeling revealed a weak antiferromagnetic coupling (J = -1.1 cm(-1)) between two Cu(II) centers.

Carbon↗

Structural insights into the coordination and extraction of Pb(II) by disulfonamide ligands derived from o-phenylenediamine.

The o-phenylenediamine-derived disulfonamide ligands 1 and 2 complex and efficiently extract Pb(II) from water into 1,2-dichloroethane via ion-exchange, in combination with 2,2'-bipyridine (97.5% and 95.0%, respectively, for 1:1 ligand-to-Pb ratios). The corresponding Pb(II)-sulfonamido binary complexes of ligands 1 and 2 (3 and 4, respectively), and ternary complexes with 2,2'-bipyridine (5 and 6, respectively), were isolated and characterized. (1)H NMR spectra of the organic phases after extraction show the formation of ternary Pb-sulfonamido-bipy complexes. X-ray characterization of 3, 4, and the ternary complex 5 consistently demonstrates four primary coordination sites and a stereochemically active lone pair on Pb. The X-ray structure of 3 shows a pseudo trigonal bipyramidal configuration on Pb, with the lone pair occupying one of the equatorial sites, and the formation of an unusual "hemidirected" coordination polymer via axial S=O-Pb coordination. The same axial S=O-Pb coordination pattern with two DMSO molecules is observed in the structure of 4.[2(CH(3))(2)SO)], thus rationalizing the high solubility of the binary complexes in strongly coordinating solvents. In contrast, the X-ray structure of the ternary complex 5 reveals a distorted four-coordinate configuration with only weak S=O-Pb coordination leading to dimer formation, thus explaining its higher solubility in weakly coordinating solvents. FT-IR spectroscopy confirms the X-ray data, since the ligand nu(S)(=)(O) stretching frequencies shift to lower values in the binary Pb(II)-sulfonamido complexes and are again altered upon formation of the ternary Pb(II)-sulfonamido-bipy complexes, as would be expected for 2,2'-bipy complexation and hindered S=O-Pb coordination.

Lead↗

Proof of large positive zero-field splitting in a Ru2 5+ paddlewheel.

We present the synthesis, as well as the structural and magnetic characterization, of [Ru2(D(3,5-Cl2Ph)F)4Cl(0.5H2O)].C6H14 (D(3,5-Cl2Ph)F = N,N'-di(3,5-dichlorophenyl)formamidinate), a Ru2(5+) compound having a 4B(2u) ground state derived from a sigma2pi4delta2pi2delta electron configuration. The persistence of this configuration from 27 to 300 K is shown by the invariance of the Ru-Ru distance. Orientation-dependent magnetic susceptibility (chiT) and magnetization (M(H)) data are in accord with a spin quartet ground state with large magnetocrystalline anisotropy associated with a large axial zero-field splitting (D) parameter. Theoretical fits to chiT and M(H) plots yielded D/kB = +114 K, implying an S = +/-1/2 Kramers doublet ground state at low temperature. Single-crystal and powder EPR data are consistent with this result, as the only observed transition is between the M(s) = +/1/2 Zeeman levels. The g values are g(perpendicular) = 2.182, g(parallel) = 1.970, and D = 79.8 cm(-1). The totality of the results demands D >> 0.

Crystallography, X-Ray↗

Diosmium(III) compounds supported by 2-anilinopyridinate and novel alkynyl derivatives.

The reaction between Os(2)(OAc)(4)Cl(2) and Hap (Hap is 2-anilinopyridine) under prolonged refluxing conditions resulted in an Os(III)(2) compound, Os(2)(ap)(4)Cl(2) (1), that can be crystallized as either the cis-(2,2) isomer from a CH(3)OH-CH(2)Cl(2) solution or the (3,1) isomer from a hexanes-CH(2)Cl(2) solution. Compound 1 undergoes facile reactions with LiC(2)Y to yield a series of Os(2)(ap)(4)(C(2)Y)(2) compounds with Y as Ph (2), ferrocenyl (3), SiMe(3) (4), and C(2)SiMe(3) (5). X-ray diffraction study of compound 2 reveals solvent-dependent isomerism similar to that of the parent compound 1. Compound 1 has Os-Os distances of 2.3937(8) and 2.3913(8) Angstroms for the cis-(2,2) and (3,1) isomers, respectively, and is paramagnetic (S = 1). Both the ethynyl derivatives 2-4 and butadiynyl derivative 5 are diamagnetic and have Os-Os distances of 2.456(1), 2.471(1), and 2.481(1) Angstroms for the cis-(2,2) and (3,1) isomers of 2 and (3,1) isomer of 4, respectively. Compounds 1-5 exhibit multiple one-electron redox couples in their cyclic voltammograms, including a reversible Os(2)(8+/7+) couple for 2. Resonance Raman spectra of both compounds 1 and 2 are reported.

Journal Article↗

Fluorescent sensing and selective Pb(II) extraction by a dansylamide ion-exchanger.

The (bis)dansylated sulfonamide 1,2-C6H4(NHSO2C10H6-5-N(CH3)2)2 (1) extracted Pb(II) selectively from water into 1,2-dichloroethane via an ion-exchange mechanism and showed fluorescence quenching upon Pb(II) extraction. The distribution ratios for metal extraction (determined by ICP-MS) for Pb(II) were 133-1410 times higher than those for other metal cations [Co(II), Ni(II), Cu(II), Zn(II), and Cd(II)] under identical conditions. Fluorescence quenching was observed upon Pb(II) extraction, which was dependent on Pb(II) concentration. The monodansylated control, C6H5NHSO2C10H6-5-N(CH3)2 (2), showed neither extraction nor quenching, indicating that the fluorescence effects are a direct result of Pb coordination to 1. The observed selectivity for Pb(II) is ascribed to the formation of a low-coordinate binary Pb(II)-Sulfonamido complex in the organic phase.

Cations, Divalent↗

Treatment of experimental hepatic fibrosis by combinational delivery of urokinase-type plasminogen activator and hepatocyte growth factor genes.

PURPOSE: To investigate the effect of combinational delivery of urokinase-type plasminogen activator (uPA) and hepatocyte growth factor (HGF) genes on hepatic fibrosis. METHODS: Replication-deficient adenoviral vectors expressing either human HGF (AdHGF) or uPA (AduPA) were generated. HGF gene was transferred into primary cultured hepatocytes and uPA gene to hepatic stellate cell (HSC) to investigate the effect on the biological character of cells. Combinational adenoviruses were infused into hepatic fibrosis rats. Serum markers as well as histological and immunohistochemical examination were carried out to test the reversal of hepatic fibrosis. RESULTS: Transfection of exogenous HGF gene induced expression of c-met/HGF receptor and stimulated hepatocyte proliferation. uPA gene delivered into HSC decreased the amount of collagen types I and III accompanied with the increased expression of matrix metalloproteinase-2. In vivo, the area of extracellular matrix in the fibrotic liver decreased to 72% in AdHGF-treated rats (P<0.01), 64% in the AduPA-treated group (P<0.01), and 51% in bi-genes transfection (P<0.01), compared with that of the controls. Moreover, immunohistochemical staining of collagen types I and III revealed that combinational genes delivery exerted more effect on reversal of hepatic fibrosis than mono-gene transfection. CONCLUSIONS: Our study indicated that simultaneous delivery of two antifibrotic genes could confer synergistic effect on hepatic fibrosis.

Adenoviridae↗

[The value of antimitochondrial antibody and its subtypes in the diagnosis of primary biliary cirrhosis].

OBJECTIVE: A study on the value of antimitochondrial antibody (AMA) and its subtypes anti-M2, anti-M4, and anti-M9 in diagnosing primary biliary cirrhosis (PBC). METHODS: Antimitochondrial antibody was detected by indirect immunofluorescence and anti-M2, anti-M4 and anti-M9 by Western blotting. AMA and anti-M2 of 78 PBC patients, of 35 non-PBC hepato-biliary disease patients and 20 healthy controls were studied and anti-M2, anti-M4 and anti-M9 were studied in 30 of the 78 PBC patients. RESULTS: 96.2% (75/78) of PBC patients were AMA positive and 94.9% (74/78) of PBC patients were anti-M2 positive. Only three among the 35 non-PBC patients were positive for AMA (one with very low titre). None of the 35 non-PBC patients was anti-M2 positive. AMA and anti-M2 were negative in all the healthy controls. Among the 30 anti-M2 positive patients, 16 patients were anti-M4 positive (16/30, 53.3%) and 4 patients were anti-M9 positive (4/30, 13.3%). CONCLUSION: AMA and its subtypes (special anti-M2) are important sero-immunological markers for the diagnosis of PBC.

Autoantibodies↗

[Role of bcl-2 and bax expression in apoptosis of hypoxic pulmonary artery smooth muscle cells of rats induced by Na+/H+ exchanger isoform-1 inhibition in vitro].

OBJECTIVE: To investigate the role of bcl-2 and bax expression in apoptosis of hypoxic pulmonary artery smooth muscle cells (PASMCs) of rats induced by Na+/H+ exchanger isoform-1 (NHE-1) inhibition in vitro. METHODS: Cultured rat PASMCs transfected with NHE-1 ribozyme gene (PRZ cell), cultured rat PASMCs transfected only with pLXSN vector (PX cell) and non-transfected rat PASMCs (PA cell) were obtained in our previous studies. The cells were cultured under low oxygen tension (<1% O2) for 0, 2, 6, 12, 24 and 48 hours respectively. Then cell apoptosis was examined with terminal deoxynucleotidyl transferase-mediated dUTP nick end labeling (TUNEL). Intracellular Ca2+([Ca2+]i) of cells was measured using fluorescence dye Fura-2/AM. The changes in mRNA expression of bcl-2 and bax in cells were assessed by semi quantitative reverse transcription-polymerase chain reaction (sqRT-PCR). The expression of Bcl-2 protein and Bax protein of cells was detected immunohistochemically. RESULTS: In contrast to normal PASMCs and cells transfected with pLXSN, the apoptosis rates in recombinant vectors transfected cells increased significantly and continuously. [Ca2+]i values were also increased in these cells, but the increase extent was remarkably lower than in the normal PASMCs (all P<0.01). The expression of bax mRNA and protein of cells transfected with recombinant vectors was increased significantly compared with cells of other two groups. Meanwhile, the expression of bcl-2 mRNA and protein of these cells were decreased significantly. CONCLUSION: The NHE-1 specific hammerhead ribozymes induce apoptosis of PASMCs under low oxygen tension by inhibiting the increase in intracellular Ca2+ concentration, increasing bax expression and decreasing bcl-2 expression.

Animals↗

Synthesis and characterization of Ru2(DMBA)4X2 (X = CN, N3, N(CN)2, I): controlling structural, redox, and magnetic properties with axial ligands.

Metathesis reactions between Ru(2)(DMBA)(4)Cl(2) (DMBA = N,N'-dimethylbenzamidinate) and MX (M = Na and K) yielded bis-adduct derivatives Ru(2)(DMBA)(4)X(2) (X = CN (1), N(3) (2), N(CN)(2) (3)). Metathesis reactions between Ru(2)(DMBA)(4)(NO(3))(2) and KI resulted in Ru(2)(DMBA)(4)I(2) (4). Compound 1 is diamagnetic, while compounds 2-4 are paramagnetic (S = 1). Both compounds 1 and 2 undergo two reversible one-electron processes, an oxidation and a reduction, while compound 3 features a quasireversible reduction. Single-crystal X-ray diffraction studies revealed that the Ru-Ru bond lengths are 2.4508(9), 2.3166(7), 2.304[1], and 2.328(1) A for compounds 1-4, respectively. Structural and electrochemical data clearly indicate that the axial ligands impart a significant influence on the electronic structures of diruthenium species.

Journal Article↗

Cyanide adducts on the diruthenium core of [Ru2(L)4](+) (L = ap, CH3ap, Fap, or F3ap). Electronic properties and binding modes of the bridging ligand.

The products of the reaction between CN(-) and four different diruthenium complexes of the type Ru(2)(L)(4)Cl where L = 2-CH(3)ap (2-(2-methylanilino)pyridinate anion), ap (2-anilinopyridinate anion), 2-Fap (2-(2-fluoroanilino)pyridinate anion), or 2,4,6-F(3)ap (2-(2,4,6-trifluoroanilino)pyridinate anion) are reported. Mono- and/or dicyano adducts of the type Ru(2)(L)(4)(CN) and Ru(2)(L)(4)(CN)(2) are found exclusively as reaction products when either the 2-CH(3)ap or the ap derivative is reacted with CN(-), but diruthenium complexes with formulations of the type Ru(2)(F(x)ap)(3)[mu-(o-NC)F(x-1)ap](mu-CN) or Ru(2)(F(x)ap)(4)(mu-CN)(2) (x = 1 or 3) are also generated when Ru(2)(Fap)(4)Cl or Ru(2)(F(3)ap)(4)Cl is reacted with CN(-). More specifically, four products formulated as Ru(2)(Fap)(4)(CN), Ru(2)(Fap)(4)(CN)(2), Ru(2)(Fap)(3)[mu-(o-NC)ap](mu-CN), and Ru(2)(Fap)(4)(mu-CN)(2) can be isolated from a reaction of CN(-) with the Fap derivative, but the exact type and yield of these compounds depend on the temperature at which the experiment is carried out. In the case of the F(3)ap derivative, the only diruthenium complex isolated from the reaction mixture has the formulation Ru(2)(F(3)ap)(3)[mu-(o-NC)F(2)ap](mu-CN) and this compound has structural, electrochemical, and spectroscopic properties quite similar to that of previously characterized Ru(2)(F(5)ap)[mu-(o-NC)F(4)ap](mu-CN). Both the mono- and dicyano derivatives synthesized in this study possess the isomer type of their parent chloro complexes. The Ru-Ru bond lengths of Ru(2)(ap)(4)(CN) and Ru(2)(2-CH(3)ap)(4)(CN) are longer than those of Ru(2)(ap)(4)Cl and Ru(2)(CH(3)ap)(4)Cl, respectively, and this is accounted for by the strong sigma-donor properties of the CN(-) ligand as compared to Cl(-). The Ru-C bonds in Ru(2)(ap)(4)(CN)(2) are significantly shorter than those in Ru(2)(ap)(4)(CN), thus revealing a greatly enhanced Ru-CN interaction in the dicyano adduct, a result which is also indicated by the fact that nu(CN) in Ru(2)(ap)(4)(CN)(2) is 50 cm(-1) higher than nu(CN) in Ru(2)(ap)(4)(CN). Although both (4,0) Ru(2)(ap)(4)(CN)(2) and (3,1) Ru(2)(Fap)(4)(CN)(2) possess the same formulation, there are clear structural differences between the two complexes and this can be explained by the fact that the two cyano derivatives possess a different binding symmetry of the bridging ligands. Each mono- and dicyano adduct was electrochemically investigated in CH(2)Cl(2) containing TBAP as supporting electrolyte. Ru(2)(ap)(4)(CN), Ru(2)(CH(3)ap)(4)(CN), and Ru(2)(Fap)(4)(CN) undergo one reduction and two oxidations. The two dicyano adducts of the ap and Fap derivatives are characterized by two reductions and one oxidation. The potentials of these processes are all negatively shifted in potential by 400-720 mV with respect to half-wave potentials for the same redox couples of the monocyano derivatives, with the exact value depending upon the specific redox reaction.

Journal Article↗