Asymmetric Two‐Center Catalysis—Learning from Nature

Steinhagen, Henning; Helmchen, Günter

doi:10.1002/anie.199623391

Cited by 246 publications

(92 citation statements)

References 41 publications

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“…It has been proposed [5][6][7][8] that, the dizinc centers are bridged by carboxylate groups of the amino acid sidechains and function as Lewis acids for the activation of the phosphate group, generate a reactive nucleophile, and stabilize both the penta-coordinate phosphorous transition state and the leaving group. Investigation into the use of multinuclear zinc(II) complexes containing bridged carboxylate as biomimetic compounds would be of a value to be synthesized as structural models and clarify the significance of two closely zinc centers in phosphate ester hydrolysis [9][10][11][12][13][14][15][16][17][18][19][20][21][22].…”

Section: Introductionmentioning

confidence: 99%

A Novel Dinucleating Ligand-Containing Hexabenzimidazoles and Its Dinuclear Zinc Complex Bridged by a Carboxylate Group for the Hydrolysis of 2-Hydroxypropyl-p-nitrophenyl phosphate

Ibrahim

2009

J Inorg Organomet Polym

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Section: Introductionmentioning

confidence: 99%

A Novel Dinucleating Ligand-Containing Hexabenzimidazoles and Its Dinuclear Zinc Complex Bridged by a Carboxylate Group for the Hydrolysis of 2-Hydroxypropyl-p-nitrophenyl phosphate

Ibrahim

2009

J Inorg Organomet Polym

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“…4b), the plot of the (where is the difference between the chemical shift of BNPP in the presence and in absence of the complex) as a function of the [7]/[BNPP] molar ratio (R) gives a straight line for low R values (R < 0.8). Then the slope change almost suddenly to give a straight line parallel to the x axis for R > 1.2 (at this point = 4.2).…”

Section: Binding Of Bnpp By the Dinuclear Zn(ii) Complexesmentioning

confidence: 98%

“…Over the years a great deal of interest has been focused on the role of metal ions in the active centers of hydrolytic metalloenzymes [1][2][3][4][5][6][7][8][9][10][11]. Many hydrolytic enzymes, including those which hydrolyze the phosphate ester bond, contain a couple of Zn(II) ions in their active site, which act cooperatively in the catalytic process.…”

Section: Introductionmentioning

confidence: 99%

Zn(II) Coordination by Open-chain Polyamine Ligands Containing Dipyridine Units. Highly Active Dinuclear Zn(II) Complexes in Phosphate Ester Hydrolysis

Bazzicalupi¹,

Bencini

Danesi³

et al. 2008

TOICJ

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Abstract:The synthesis and characterization of two new open-chain ligands, L1 and L2, containing two 2,2'-dipyridine units connected respectively by a pentaethylenhexamine and a pentapropylenhexamine chain, is reported. Zn(II) complexation has been studied by means of potentiometric and UV-vis spectrophotometric measurements in aqueous solution. Both ligands form stable mono-and dinuclear complexes, the metal ions being coordinated by a single dipyridine unit and by the adjacent amine groups. The ability of the binuclear Zn(II) complexes as nucleophilic agents in hydrolytic processes has been tested by using bis(p-nitrophenyl) phosphate (BNPP) as substrate. Both complexes display high rate enhancements in BNPP cleavage in aqueous solution. The study outlines that different mechanisms are operative in BNPP cleavage in the presence of the L1 and L2 complexes.

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“…The binding interactions employed are typically dynamic in character, such as hydrophobic-hydrophilic interactions. Reviews of such catalysts are available [50][51][52][53].…”

Section: Supramolecular Catalystsmentioning

confidence: 99%

Kinematic molecular manufacturing machines

Boskovic

Balakrishnan

Huang

et al. 2016

Coordination Chemistry Reviews

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The principles of kinematic manufacturing machines of the type widely used since the industrial revolution are reviewed. Consideration is then given to how the principles of kinematics ('the geometry of motion') may manifest in molecular catalysts. Actions of this type involve synchronized, regular, repeated and rapid conformational flexing along geometrically optimum pathways that define a single degree of freedom. The proposition that many of the catalysts of biology, enzymes, may generally exploit a kinematic action is discussed. Thereafter, in the major portion of this work, representative abiological molecular catalysts whose actions display the characteristic features of kinematic manufacturing processes, are reviewed. In accordance with the principles of kinematics, molecular catalytic actions of this type are shown to be capable of transforming unremarkable chemical species into powerful catalysts with high activities, selectivities, and durabilities. Disciplines Engineering | Physical Sciences and Mathematics Engineering, Wenzhou University, Wenzhou 325027, Peoples Republic of ChinaAbstract: The principles of kinematic manufacturing machines of the type widely used since the industrial revolution are reviewed. Consideration is then given to how the principles of kinematics ('the geometry of motion') may manifest in molecular catalysts. Actions of this type involve synchronized, regular, repeated and rapid conformational flexing along geometrically optimum pathways that define a single degree of freedom. The proposition that many of the catalysts of biology, enzymes, may generally exploit a kinematic action is discussed. Thereafter, in the major portion of this work, representative abiological molecular catalysts whose actions display the characteristic features of kinematic manufacturing processes, are reviewed. In accordance with the principles of kinematics, molecular catalytic actions of this type are shown to be capable of transforming unremarkable chemical species into powerful catalysts with high activities, selectivities, and durabilities.

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Asymmetric Two‐Center Catalysis—Learning from Nature

Cited by 246 publications

References 41 publications

A Novel Dinucleating Ligand-Containing Hexabenzimidazoles and Its Dinuclear Zinc Complex Bridged by a Carboxylate Group for the Hydrolysis of 2-Hydroxypropyl-p-nitrophenyl phosphate

A Novel Dinucleating Ligand-Containing Hexabenzimidazoles and Its Dinuclear Zinc Complex Bridged by a Carboxylate Group for the Hydrolysis of 2-Hydroxypropyl-p-nitrophenyl phosphate

Zn(II) Coordination by Open-chain Polyamine Ligands Containing Dipyridine Units. Highly Active Dinuclear Zn(II) Complexes in Phosphate Ester Hydrolysis

Kinematic molecular manufacturing machines

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