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Cheng-Yong Su

Publications and source records attributed to Cheng-Yong Su.

At least 19 recordsLinked to original sources

An effective metallohydrolase model with a supramolecular environment: structures, properties, and activities.

A supramolecular inclusion complex, [Zn(L1)(H2O)2(beta-CD)](ClO4)2.9.5 H2O (1) was synthesized and characterized structurally and its first-order active species for hydrolysis of esters, [Zn(L1)(H2O)(OH)(beta-CD)](ClO4) (2), was isolated (L1=4-(4'-tert-butylbenzyl)diethylenetriamine; beta-CD=beta-cyclodextrin). The apparent inclusion stability constant of the host and the guest measured in aqueous solution was (5.91+/-0.03)x10(3) for 1. The measured values of the first- and second-order pK(a) values of coordinated water molecules were 8.20+/-0.08 and 10.44+/-0.08, respectively, and were assigned to water molecules occupying the plane and remaining axial positions in a distorted trigonal bipyramid of the [Zn(L1)(H2O)2(beta-CD)]2+ sphere according to the structural analysis of [Zn(L2)(H2O)}2(mu-OH)](ClO4)3 (3) (L2=4-benzyldiethylenetriamine). p-Nitrophenyl acetate (pNA) hydrolysis catalyzed by 1 at pH 7.5-9.1 and 25.0+/-0.1 degrees C exhibited a first-order reaction with various concentrations of pNA and 1, but the pH profile did not indicate saturated kinetic behavior. Second-order rate constants of 0.59 and 24.0 M(-1) s(-1) were calculated for [Zn(L1)(H2O)(OH)(beta-CD)]+ and [Zn(L1)(OH)2(beta-CD)], respectively; the latter exhibited a potent catalytic activity relative to the reported mononuclear and polynuclear Zn(II) species.

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A new 2-carboxylate-substituted 4,4'-bipyridine ligand: coordination chemistry of 4,4'-bipyridine-2-carboxylic acid and its synthetic intermediate 2-methyl-4,4'-bipyridine.

The first monocarboxylate-substituted 4,4'-bipyridine ligand, 4,4'-bipyridine-2-carboxylic acid (4-(pyridin-4-yl)pyridine-2-carboxylic acid (PPCAH)), has been successfully synthesized from 4,4'-bipyridine. Reactions with transition metals zinc and manganese were used to establish the coordination characteristics of the product, 4,4'-bipyridine-2-carboxylic acid, and of the synthetic intermediate, 2-methyl-4,4'-bipyridine, by single-crystal X-ray diffraction. The ligand PPCAH is useful for the formation of metal-containing building blocks that can be used in the assembly of mixed-metal framework materials. The synthesis and structure of one such mixed-metal coordination polymer, Cu(PPCA)(2)HgI(2), is also presented.

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Non-interpenetrated square-grid coordination polymers synthesized using an extremely long N,N'-type ligand.

Four new, non-interpenetrated square-grid coordination polymers, namely [Mn(L)2(NO3)2]infinity (1), [[Cd(L)2(NO3)2].solvate]infinity (2), [Cd(L)2(NO3)2]infinity (3), and [[Zn(L)2](BF4)2.(C6H6)2.564.(DMF)1.576.(MeOH, H2O)3.454]infinity (4), were synthesized using the new, extremely long N,N'-type ligand: 2,5-bis(4'-(imidazol-1-yl)benzyl)-3,4-diaza-2,4-hexadiene (L). The reaction of Cd(NO3)2 with L leads to two novel structures sharing the same framework composition, [Cd(L)2(NO3)2]infinity, which have different arrangements of L around the metal centers. Both the channel-containing structure and the nonporous structure can be formed by choice of the appropriate solvent system. Moreover, the less stable, channel-containing form readily converts into the more stable, condensed structure upon removal of the guest molecules from the channels.

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Disilver(I) rectangular-shaped metallacycles: X-ray crystal structure and dynamic behavior in solution.

Reaction of the ditopic semirigid ligand 1,2-bis(imidazolylmethyl)benzene (1,2-bImb) or the flexible ligand 1,4-bis(2-benzimidazolyl)butane (C4BIm) with AgX (X = ClO4-, BF4-, CF3CO2-) afforded five new complexes, namely, [Ag2(1,2-bImb)2](ClO4)2 (1), [Ag2(1,2-bImb)2](BF4)2 (2), [Ag2(1,2-bImb)2](CF3CO2)2.2CH3OH (3.2CH3OH), [Ag2(C4BIm)2](ClO4)2.2DMF (4.2DMF), and [Ag2(C4BIm)2](CF3CO2)2.2H2O (5.2H2O), all of which contain a centrosymmetric, rectangular-shaped cationic disilver(I) metallacycle [Ag2(L)2]2+. In 1-3, a pair of 1,2-bImb ligands takes on the syn conformation to connect two Ag(I) ions to give a compressed rectangle with a transannular Ag...Ag separation of 3.27-3.36 angstroms, whereas in 4 and 5, the pair of planar C4BIm ligands acts in the cis conformation to connect two Ag(I) ions to yield a normal rectangle with a transannular Ag...Ag separation of 7.67-7.91 angstroms. The anions form Ag...O or Ag...F weak interactions in 1-3 and O-H...O or N-H...O hydrogen bonds in 4 and 5 in crystal packing but exhibit no significant influence on the formation of the disilver(I) macrocycles. The solution structure and dynamic behavior of the complexes studied by electrospray ionization mass spectrometry, 1H NMR, and variable-temperature NMR indicated that the dynamic equilibrium between the [Ag2(L)2]2+ cation and the open-ring oligomers or other potential species occurs via solvent-assisted dissociative exchange. The metal-ligand exchange barrier was estimated to be 54.5 kJ mol(-1).

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2,2'-(iminodimethylene)bis(1H-benzimidazolium)1+ chloride.

The title compound, C(16)H(16)N(5)(+).Cl(-) (nbbH(+).Cl(-)), displays N-H...N, N-H...Cl and pi-pi interactions in the crystal packing. The Cl(-) anion is chelated by the nbbH(+) cation via two N-H...Cl hydrogen bonds. Inter-ion N-H...N and N-H...Cl hydrogen bonds link ions related by 2(1) screw axes into chains along the c axis. These chains are further linked by glide-plane operations to generate a three-dimensional network, which is additionally stabilized by interchain pi-pi interactions.

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Spontaneously resolved chiral three-fold interpenetrating diamondoidlike Cu(II) coordination polymers with temperature-driven crystal-to-crystal transformation.

The chiral 3-fold interpenetrating diamondoidlike Cu(II)-containing coordination polymer [Cu(2,5-bis(4-pyridyl)-1,3,4-oxadiazole)2(H2O)](ClO4)2]n (1a) is reported. It undergoes a temperature-driven reversible single-crystal-to-single-crystal structural transformation between room- (293 K, 1a) and low-temperature (150 K, 1b) forms.

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Tris(1H-benzimidazol-2-ylmethyl)amine-solvent adducts.

The tris(1H-benzimidazol-2-ylmethyl)amine (ntb) molecule crystallizes in different solvent systems, resulting in two kinds of adduct, namely the monohydrate, C24H21N7.H2O or ntb.H2O, (I), and the acetonitrile-methanol-water (1/0.5/1.5) solvate, C24H21N7.C2H3N.0.5CH4O.1.5H2O or ntb.1.5H2O.0.5MeOH.MeCN, (II). In both cases, ntb adopts a tripodal mode to form hydrogen bonds with a solvent water molecule via two N-H...O and one O-H...N hydrogen bond. In (I), the ntb.H2O adduct is further assembled into a two-dimensional network by N-H...N and O-H...N hydrogen bonds, while in (II), a double-stranded one-dimensional chain structure is assembled via N-H...O and O-H...O hydrogen bonds, with the acetonitrile molecules located inside the cavities of the chain structure.

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3D coordination polymers with nitrilotriacetic and 4,4'-bipyridyl mixed ligands: structural variation based on dinuclear or tetranuclear subunits assisted by Na-O and/or O-H...O interactions.

The reactions of Cu(II) with the mixed nitrilotriacetic acid (H3NTA) and 4,4'-bipyridyl (4,4'-bpy) ligands in different metal-to-ligand ratios in the presence of NaOH and NaClO4 afforded two complexes, Na3[Cu2(NTA)2(4,4'-bpy)]ClO4 x 5H2O (1) and [Cu2(NTA) (4,4'-bpy)2]ClO4 x 4H2O (2). The two complexes have been characterized by elemental analysis, IR, XRD, and single-crystal X-ray diffraction. 1 contains a basic doubly negatively charged [Cu2(NTA)2(4,4'-bpy)]2- dinuclear unit which was further assembled via multiple Na-O and O-H...O interactions into a three-dimensional (3D) pillared-layer structure. 2 features a two-dimensional (2D) undulated brick-wall architecture containing a basic doubly positively charged [Cu4(NTA)2(4,4'-bpy)2]2+ tetranuclear unit. The 2D network possesses large cavities hosting guest molecules and was further assembled via O-H...O hydrogen bonds into a 3D structure with several channels running in different directions.

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A noninterpenetrated 1D molecular ladder and 2D butterfly network: effect of positional isomerism of semirigid bis(pyridylmethyl)pyromellitic diimide ligands on the architecture of their metal(II) complexes.

Three new complexes [Cd(4-pmpmd)1.5 (NO3)2] x CHCl3 (1), [Cd(3-pmpmd)1.5 (NO3)2] x EtOH (2), and [Zn(3-pmpmd)1.5 (NO3)2] x MeOH (3) (3- or 4-pmpmd = N,N'-bis(3- or 4-pyridylmethyl)pyromellitic diimide) containing T-shaped building blocks have been obtained from reactions between the long semirigid ligands 3- or 4-pmpmd and either cadmium or zinc nitrate. 1 forms noninterpenetrated 1D molecular ladders that are linked via multiple, complementary intermolecular C-H...O hydrogen bonds that effect the 3D alignment. 2 and 3 are isostructural and feature a noninterpenetrated 2D butterfly-shaped network with (6,3) topology. Multiple intermolecular C-H...O hydrogen bonds exist between the 2D layers and generate the 3D framework. The structural differences between 1 and 2 or 3 are attributed to the different conformations adopted by the ligands, which illustrate the influence of positional isomerism on the resultant supramolecular architectures of metal complexes.

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A three-dimensional, noninterpenetrating metal--organic framework with the moganite topology: a simple (4(2)x6(2)x8(2))(4x6(4)x8)(2) net containing two kinds of topologically nonequivalent points.

Self assembly of Cu(2+) with the multifunctional ligand 2-(4-pyridyl)thiazole-4-carboxylic acid (Pytac) affords the neutral 3D coordination polymer [Cu(3)(Pytac)(6)](H(2)O)(14) (hereafter, SZL-1), which has the rare moganite topology. The mineral moganite has a topology that is closely related to the well-known quartz topology, but the two topologies are differentiated by the number of topologically inequivalent nodes. Whereas only one kind of node is present in quartz, two types of topologically inequivalent nodes are present in moganite. The title compound, which has three vertices in its repeat unit, has two types of topologically inequivalent nodes with the overall vertex symbol (4(2)x6(2)x8(2))(4x6(4)x8)(2) corresponding to the moganite net. Prior to this report, few metal-organic framework materials (MOFs) have been found to contain more than one type of node, and SZL-1 is the first MOF with the moganite topology.

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Assembly of large simple 1D and rare polycatenated 3D molecular ladders from T-shaped building blocks containing a new, long N,N'-bidentate ligand.

Molecular ladders [Co(2)(nbpy4)(3)(NO(3))(4)]*solvents and [Cd(2)(nbpy4)(3)(NO(3))(4)](nbpy4 =N,N'-bis-(4-pyridinylmethylene)-1,5-naphthalenediamine) were synthesized via self-assembly; the former is a large, simple, noninterpenetrated 1D ladder that contains guest solvent molecules between the rungs, while the latter exists as 1D ladders in a rare four-fold interlocked 3D structure.

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Exceptionally stable, hollow tubular metal-organic architectures: synthesis, characterization, and solid-state transformation study.

An effective solvothermal procedure has been developed to synthesize the new three-dimensional metal-organic framework, [ZnF(AmTAZ)].solvents, using either 3-amino-1,2,4-triazole (AmTAZ) or 3-amino-1,2,4-triazole-5-carboxylic acid (AmTAZAc) and a choice of several Zn(II) salts as starting materials. The three-dimensional structure displays open-ended, hollow nanotubular channels that are formed by hexanuclear metallamacrocyclic Zn(6)F(6)(AmTAZ)(6) rings. The framework integrity is maintained to 350 degrees C, at which point most of the guest solvent molecules have been removed, as evidenced by single-crystal X-ray analyses, (1)H solid-state NMR, and TGA measurements. At higher temperatures, the framework is converted either to zinc oxide (ZnO) when heated in air or to zinc cyanamide (ZnCN(2)) when heated in an inert atmosphere. In both cases, the as-grown, rodlike crystal shape is maintained during the solid-state transformation, suggesting a possible route for preparing one-dimensional crystalline nanomaterials.

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Formation of dinuclear, macrocyclic, and chain structures from HgI(2) and a semirigid benzimidazole-based bridging ligand: an example of ring-opening supramolecular isomerism.

The reactions of HgI(2) with the semirigid ditopic ligand 1,3-bis(benzimidazol-1-ylmethyl)-2,4,6-trimethylbenzene (bbimms) afforded three new complexes, [Hg(2)(mu-I)(2)I(2)(bbimms)] (1), [Hg(2)I(4)(bbimms)(2)] (2), and catena-poly[HgI(2)(bbimms)] (3). The ligand and all complexes have been structurally characterized by single-crystal X-ray diffraction. 1 is a triply bridged dinuclear complex comprised of two Hg(II) ions, one bridging ligand, two bridging I(-) anions, and two terminal I(-) anions. 2 is a dinuclear metallamacrocycle comprised of two Hg(II) ions, two bridging ligands, and four terminal I(-) anions, while 3 is a helical chain with the repeating unit of HgI(2)(bbimms). 2 and 3 can be classified as supramolecular isomers, and both are related to the triply bridged precursor 1 via the addition of one more ligand in a ring-opening process.

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Ligand-directed molecular architectures: self-assembly of two-dimensional rectangular metallacycles and three-dimensional trigonal or tetragonal prisms.

Three angular ditopic ligands (1,3-bis(benzimidazol-1-ylmethyl)-4,6-dimethylbenzene L(1), 1,3-bis(benzimidazol-1-ylmethyl)-2,4,6-trimethylbenzene L(2), and 1,4-bis(benzimidazol-1-ylmethyl)-2,3,5,6-tetramethylbenzene L(3)) and one tripodal ligand 1,3,5-tris(benzimidazol-1-ylmethyl)-2,4,6-trimethylbenzene L(4) have been prepared. Reaction of these shape-specific designed ligands with different metal salts affords a series of discrete molecular architectures: [Ag(2)L(1)(2)](BF(4))(2) 1, [Ag(2)L(2)(2)](CF(3)SO(3))(2) 2, [CF(3)SO(3)(-) subset Ag(2)L(3)(2)]CF(3)SO(3) 3, [CF(3)SO(3)(-) subset Ag(2)L(3)(3)]CF(3)SO(3) 4, [ClO(4)(-) subset Cu(2)L(2)(4)](ClO(4))(3) 5, [4H(2)O subset Ni(2)L(2)(4)Cl(4)].6H(2)O 6, [BF(4)(-) subset Ag(3)L(4)(2)](BF(4))(2) 7, [ClO(4)(-) subset Ag(3)L(4)(2)](ClO(4))(2) 8, and [CuI(3)(2-) subset Cu(3)L(4)(2)](2)[Cu(2)I(4)] 9. The compounds were characterized by elemental analysis, ESI-MS, IR, and NMR spectroscopy, and X-ray crystallography. 1 is a dinuclear metallacycle with 2-fold rotational symmetry in which two syn-conformational L(1) ligands are connected by two linearly coordinated Ag(+) ions. 2 and 3 are structurally related, consisting of rectangular structures assembled from two linearly coordinated Ag(+) ions and two L(2) or L(3) ligands. The structure of 4 is a trigonal prismatic box consisting of two Ag(+) ions in trigonal planar coordination linked by three L(3) ligands, while the structures of 5 and 6 are tetragonal prismatic cages constructed by two square planar Cu(2+) or Ni(2+) ions linked by four L(2) ligands. The topologies of 7-9 are similar to that of 4; however, these three structures are assembled from three linearly coordinated Ag(+) or Cu(+) ions and two tripodal ligands, representing an alternative strategy to assembling a trigonal prism. (1)H NMR and ESI-MS were utilized to elucidate the solution structures of these macrocycles.

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Multidimensional frameworks assembled from silver(I) coordination polymers containing flexible bis(thioquinolyl) ligands: role of the intra- and intermolecular aromatic stacking interactions.

The two flexible multidentate ligands 1,3-bis(8-thioquinolyl)propane (C3TQ) and 1,4-bis(8-thioquinolyl)butane (C4TQ) were reacted with AgX (X = CF(3)SO(3)(-) or ClO(4)(-)) to give four new complexes: ([Ag(C3TQ)](ClO(4)))(n)() 1, ([Ag(C3TQ)](CF(3)SO(3)))(n)() 2, ([Ag(2)(C4TQ)(CF(3)SO(3))(CH(3)CN)](CF(3)SO(3)))(n)() 3, and ([Ag(C4TQ)](ClO(4)))(n)() 4. All complexes have been characterized by elemental analysis, IR, and (1)H NMR spectroscopy. Single-crystal X-ray analysis showed that chain structures form for all complexes in which the quinoline rings interact via various intra- (1) or intermolecular (2, 3, and 4) pi-pi aromatic stacking interactions, which in the latter cases results in multidimensional structures. Additional weak interactions, such as Ag.O and Ag.S contacts and C-H.O hydrogen bonding, are also present and help form stable, crystalline materials. It was found that the (CH(2))(n) spacers (n = 3 or 4) affect the orientation of the two terminal quinolyl rings, thereby significantly influencing the specific framework structure that forms. If the same ligand is used, on the other hand, then the different counteranions have the greatest effect on the final structure.

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