Kinetics of stepwise hydrolysis of ferrioxamine B and of formation of diferrioxamine B in acid perchlorate solution

Biruš, Mladen; Bradić, Zdravko; Krznaric, G.; Kujundžić, Nikola; Pribanic, Marijan; Wilkins, Patricia C.; Wilkins, Ralph G.

doi:10.1021/ic00254a009

Cited by 42 publications

(41 citation statements)

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“…One should expect that binding atoms to Ni(II) in 1:1:0 complex are probably the oxygen atoms of the hydroxamate moiety and the oxygen atom of the carboxylate group. The involvement of the hydroxamate moiety in metal complex formation was reported before for several metal complexes of acetohydroxamic acid [24][25][26][27][28][29]. The log β for the 1:1:0 complex of Cu(II)-, Ni(II)-, and Zn(II)-with acetohydroxamic acid are 7.89, 5.37, and 5.32, respectively [29].…”

Section: Equilibrium Studysupporting

confidence: 58%

The reactivity of Ni(II) toward aspartic and glutamic monohydroxamates

Al-Sogair

Marafie

Shuaib

et al. 2006

Int J of Chemical Kinetics

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The formation of complexes of Ni(II) with aspartic and glutamic acid hydroxamates was determined by potentiometric methods at I = 0.15 M NaCl and T = 25 • C. The equilibrium study of Ni(II) with ASX or GLX revealed that the predominant species formed in solution were (M:L:H + ): (1:1:0), (1:1:1), (2:1:0), and (2:1:1) in the whole pH range (∼3-11). The formation of polymeric species was not observed. The octahedral structures were predicted in which the ligands act as tridentate ligands. The kinetics of complex formation between Ni(II) with ASX system as well as Ni(II) with GLX were also studied in a wide pH range. The observed rate constants for the Ni(II)-hydroxamates were found to be dependent on the total concentration of hydroxamates at a given pH through the following relations:The trans effect of the hydroxyl group present in the reacting species of Ni(OH) + as well as a ring closure resulted from ligand chelation are introduced as explanations for the rate constants obtained for the reactions of Ni(II) with ASX or GLX. C 2006

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Section: Equilibrium Studysupporting

confidence: 58%

The reactivity of Ni(II) toward aspartic and glutamic monohydroxamates

Al-Sogair

Marafie

Shuaib

et al. 2006

Int J of Chemical Kinetics

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“…1), which could prevent easy access of the proton to a site of Fe 3ϩ coordination (Biruš et al, 1987). Another possible cause of the difference in complex stability between the siderophore and the simple hydroxamate ligand is the difference in substituent on the N atom in the coordinating hydroxamate (i.e., an alkyl group vs. a proton), which places additional electron density on the carbonyl O in the case of the siderophore (Crumbliss, 1991).…”

Section: Discussionmentioning

confidence: 99%

“…b Conditional equilibrium constant and kinetics data at 298 K and 2 M ionic strength, from Biruš et al (1987). Units of k f are M Ϫ1 s Ϫ1 (row 5) or s Ϫ1 (rows 6 and 7).…”

Section: Discussionmentioning

confidence: 99%

Temperature dependence of goethite dissolution promoted by trihydroxamate siderophores

Cocozza

Tsao

Cheah

et al. 2002

Geochimica et Cosmochimica Acta

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Abstract-This article reports an investigation of the temperature dependence of goethite dissolution kinetics in the presence of desferrioxamine B (DFO-B), a trihydroxamate siderophore, and its acetyl derivative, desferrioxamine D1 (DFO-D1). At 25 and 40°C, DFO-D1 dissolved goethite at twice the rate of DFO-B, whereas at 55°C, the behavior of the two ligands was almost the same. Increasing the temperature from 25 to 55°C caused little or no significant change in DFO-B or DFO-D1 adsorption by goethite. A pseudo-first-order rate coefficient for dissolution, calculated as the ratio of the mass-normalized dissolution rate coefficient to the surface excess of siderophore, was approximately the same at 25 and 40°C for both siderophores. At 55°C, however, this rate coefficient for DFO-D1 was about half that for DFO-B. Analysis of the temperature dependence of the mass-normalized dissolution rate coefficient via the Arrhenius equation led to an apparent activation energy that was larger for DFO-B than for DFO-D1, but much smaller than that reported for the proton-promoted dissolution of goethite. A compensation law was found to relate the pre-exponential factor to the apparent activation energy in the Arrhenius equation, in agreement with what has been noted for the proton-promoted dissolution of oxide minerals and for the complexation of Fe 3ϩ by DFO-B and simple hydroxamate ligands in aqueous solution. Analysis of these results suggested that the siderophores adsorb on goethite with a only single hydroxamate group in bidentate ligation with an Fe(III) center.

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“…b Conditional formation constant from Biruš et al (1987), corrected to zero ionic strength with the Davies equation.…”

Section: Goethite Dissolution Kineticsmentioning

confidence: 99%

Steady-state dissolution kinetics of goethite in the presence of desferrioxamine B and oxalate ligands: implications for the microbial acquisition of iron

et al. 2003

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This paper reports an investigation of the effects of a trihydroxamate siderophore, desferrioxamine B (DFO-B), and a common biological ligand, oxalate, on the steady-state dissolution of goethite at pH 5 and 25 jC. The main goal of our study was to quantify the adsorption of the ligands and the dissolution of goethite they promote in a two-ligand system. In systems with one ligand only, the adsorption of oxalate and DFO-B each followed an L-type isotherm. The surface excess of oxalate was approximately 40 mmol kg À 1 at solution concentrations above 80 AM, whereas the surface excess of DFO-B was only 1.2 mmol kg À 1 at 80 AM solution concentration. In the two-ligand systems, oxalate decreased DFO-B adsorption quite significantly, but not vice versa. For example, in solutions containing 40 AM DFO-B and 40 AM oxalate, 30% of the DFO-B adsorbed in the absence of oxalate was displaced. The mass-normalized dissolution rate of goethite in the presence of DFO-B alone increased as the surface excess of the ligand increased, suggesting a ligand-promoted dissolution mechanism. In systems containing oxalate only, mass-normalized goethite dissolution rates were very low at concentrations below 200 AM, despite maximal adsorption of the ligand. At higher oxalate concentrations (up to 8 mM), the steady-state dissolution rate continued to increase, even though the surface excess of adsorbed ligand was essentially constant. Chemical affinity calculations and dissolution experiments with variation of the reactor flow rate showed that far-from-equilibrium conditions did not obtain in systems containing oxalate at concentrations below 5 mM. The dissolution rate in the presence of DFO-B at solution concentrations between 1 and 80 AM was approximately doubled when oxalate was also present at 40 AM solution concentration. The dissolution rate in the presence of oxalate at solution concentrations between 0 and 200 AM was increased by more than an order of magnitude when DFO-B was also present at 40 AM solution concentration. Chemical affinity calculations showed that, in systems containing DFO-B, goethite dissolution was always under far-from-equilibrium conditions, irrespective of the presence of oxalate. These results were described quantitatively by a model rate law containing a term proportional to the surface excess of DFO-B and a term proportional to that of oxalate, with both surface excesses being determined in the twoligand system. The pseudo first-order rate coefficient in the DFO-B term has the same value as measured for goethite dissolution in the presence of DFO-B only, while the rate coefficient in the oxalate term must be measured in the two-ligand system, since it is only in this system that far-from-equilibrium conditions obtain. These latter conditions do not exist in the system containing oxalate only, but they do exist in the DFO-B/oxalate system because the siderophore is able to remove Fe(III) from all Fe -oxalate complexes rapidly, leaving the uncomplexed oxalate ligand in solution free to react again wit...

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Kinetics of stepwise hydrolysis of ferrioxamine B and of formation of diferrioxamine B in acid perchlorate solution

Cited by 42 publications

References 0 publications

The reactivity of Ni(II) toward aspartic and glutamic monohydroxamates

The reactivity of Ni(II) toward aspartic and glutamic monohydroxamates

Temperature dependence of goethite dissolution promoted by trihydroxamate siderophores

Steady-state dissolution kinetics of goethite in the presence of desferrioxamine B and oxalate ligands: implications for the microbial acquisition of iron

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