Catalysis of phosphoryl transfer from adenosine-5′-triphosphate (ATP) by trinuclear “chelate” complexes

Ge, Ruiguang; Lin, Hai; Xu, Xin-He; Sun, Xuesong; Lin, Huakuan; Zhu, Shou‐Fei; Ji, Baofeng; Li, Fenghua; Wu, Hongxing

doi:10.1016/j.jinorgbio.2004.03.007

Cited by 7 publications

(7 citation statements)

References 16 publications

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“…585 As seen with many of the previously described polyammonium macrocycles, the binding affinities with receptor 537 increased with increasing degree of protonation as inferred from potentiometric titration (pH 2-10.5). This receptor bound ATP > ADP > AMP in accordance with the relative anionic charge of the analytes.…”

Section: Major Phosphate-binding Functionalitiesmentioning

confidence: 60%

Artificial Receptors for the Recognition of Phosphorylated Molecules

et al. 2011

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Section: Major Phosphate-binding Functionalitiesmentioning

confidence: 60%

Artificial Receptors for the Recognition of Phosphorylated Molecules

et al. 2011

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“…11, 12 In recent years, synthetic ligands, from macrocyclic polyammonium to phenanthroline as well as polyoxomolydates, have been developed to elucidate the mechanism of ATP cleavage. [13][14][15][16][17] However, it is surprising to find that our knowledge on the properties of metal ions and amino acids on ATP hydrolysis system is very scarce. Amino acids play central roles as building blocks of protein.…”

Section: Introductionmentioning

confidence: 99%

Differential effects of Mg(ii) and N_α-4-tosyl-l-arginine methyl ester hydrochloride on the recognition and catalysis in ATP hydrolysis

Lü

2008

Dalton Trans.

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The supramolecular interactions of Mg(ii) and N(alpha)-4-tosyl-l-arginine methyl ester hydrochloride (TAME) with ATP have been investigated using (1)H and (31)P NMR spectra. Furthermore, the hydrolysis of ATP catalyzed by Mg(ii) and TAME has been studied at 60 degrees C and pH 7 using (31)P NMR spectra. In the Mg(ii)-ATP-TAME ternary system, the binding interaction of Mg(2+) with ATP involves not only N1 and N7 in the adenine ring but also beta- and gamma-phosphate of ATP. The binding forces are mainly electrostatic interaction and cation (Mg(2+))-pi interaction. The guanidinium group and the aromatic ring of TAME interacts with ATP by beta and gamma phosphate and the adenine ring of ATP. The binding forces are mainly electrostatic interactions and pi-pi stacking. A significant difference between the binary and the ternary system indicates that TAME is essential to the stablization of the intermediate. Kinetic studies show that the hydrolysis rate constant of ATP is 2.16 x 10(-2) h(-1) at pH 7 in the Mg(ii)-TAME-ATP ternary system. The Mg(ii) ion and TAME can accelerate the ATP hydrolysis process. A possible mechanism has been proposed that the hydrolysis occurs through an addition-elimination, in which the phosphoramidate intermediate was observed at 3.21 ppm in the (31)P NMR of the ternary system. These results provide further information concerning the effect of the key amino acid residue and metal ions as cofactors of ATPase on ATP synthesis/hydrolysis at the molecular level.

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“…5 In addition, ATP hydrolysis via highly efficient metalloenzymatic ATPases also plays a central role in a variety of processes including photosynthesis phosphorylation, oxidative phosphorylation, and muscle action. 6 Uncatalyzed ATP hydrolysis in aqueous solution is a slow process with a half-life between 10 and 100 days in the pH range 1−12 at room temperature. 7 However, the rate of ATP hydrolysis is increased by a factor of 10 11 via enzymatic catalysis and a factor of 10−100 in the presence of metal ions.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Moreover, ATP consumption may promote the release of the polypeptide product from the enzyme and, alternatively, ATP hydrolysis may permit the translocation of the enzyme along the substrate to the next cleavage site . In addition, ATP hydrolysis via highly efficient metalloenzymatic ATPases also plays a central role in a variety of processes including photosynthesis phosphorylation, oxidative phosphorylation, and muscle action …”

Section: Introductionmentioning

confidence: 99%

Detailed Mechanism of Phosphoanhydride Bond Hydrolysis Promoted by a Binuclear Zr^IV-Substituted Keggin Polyoxometalate Elucidated by a Combination of ³¹P, ³¹P DOSY, and ³¹P EXSY NMR Spectroscopy

et al. 2016

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A detailed reaction mechanism is proposed for the hydrolysis of the phosphoanhydride bonds in adenosine triphosphate (ATP) in the presence of the binuclear Zr(IV)-substituted Keggin type polyoxometalate (Et2NH2)8[{α-PW11O39Zr(μ-OH)(H2O)}2]·7H2O (ZrK 2:2). The full reaction mechanism of ATP hydrolysis in the presence of ZrK 2:2 at pD 6.4 was elucidated by a combination of (31)P, (31)P DOSY, and (31)P EXSY NMR spectroscopy, demonstrating the potential of these techniques for the analysis of complex reaction mixtures involving polyoxometalates (POMs). Two possible parallel reaction pathways were proposed on the basis of the observed reaction intermediates and final products. The 1D (31)P and (31)P DOSY spectra of a mixture of 20.0 mM ATP and 3.0 mM ZrK 2:2 at pD 6.4, measured immediately after sample preparation, evidenced the formation of two types of complexes, I1A and I1B, representing different binding modes between ATP and the Zr(IV)-substituted Keggin type polyoxometalate (ZrK). Analysis of the NMR data shows that at pD 6.4 and 50 °C ATP hydrolysis in the presence of ZrK proceeds in a stepwise fashion. During the course of the hydrolytic reaction various products, including adenosine diphosphate (ADP), adenosine monophosphate (AMP), pyrophosphate (PP), and phosphate (P), were detected. In addition, intermediate species representing the complexes ADP/ZrK (I2) and PP/ZrK (I5) were identified and the potential formation of two other intermediates, AMP/ZrK (I3) and P/ZrK (I4), was demonstrated. (31)P EXSY NMR spectra evidenced slow exchange between ATP and I1A, ADP and I2, and PP and I5, thus confirming the proposed reaction pathways.

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Catalysis of phosphoryl transfer from adenosine-5′-triphosphate (ATP) by trinuclear “chelate” complexes

Cited by 7 publications

References 16 publications

Artificial Receptors for the Recognition of Phosphorylated Molecules

Artificial Receptors for the Recognition of Phosphorylated Molecules

Differential effects of Mg(ii) and N_α-4-tosyl-l-arginine methyl ester hydrochloride on the recognition and catalysis in ATP hydrolysis

Detailed Mechanism of Phosphoanhydride Bond Hydrolysis Promoted by a Binuclear Zr^IV-Substituted Keggin Polyoxometalate Elucidated by a Combination of ³¹P, ³¹P DOSY, and ³¹P EXSY NMR Spectroscopy

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Catalysis of phosphoryl transfer from adenosine-5′-triphosphate (ATP) by trinuclear “chelate” complexes

Cited by 7 publications

References 16 publications

Artificial Receptors for the Recognition of Phosphorylated Molecules

Artificial Receptors for the Recognition of Phosphorylated Molecules

Differential effects of Mg(ii) and Nα-4-tosyl-l-arginine methyl ester hydrochloride on the recognition and catalysis in ATP hydrolysis

Detailed Mechanism of Phosphoanhydride Bond Hydrolysis Promoted by a Binuclear ZrIV-Substituted Keggin Polyoxometalate Elucidated by a Combination of 31P, 31P DOSY, and 31P EXSY NMR Spectroscopy

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Differential effects of Mg(ii) and N_α-4-tosyl-l-arginine methyl ester hydrochloride on the recognition and catalysis in ATP hydrolysis

Detailed Mechanism of Phosphoanhydride Bond Hydrolysis Promoted by a Binuclear Zr^IV-Substituted Keggin Polyoxometalate Elucidated by a Combination of ³¹P, ³¹P DOSY, and ³¹P EXSY NMR Spectroscopy