Isothermal diffusion coefficients of sodium chloride-magnesium chloride-water at 25.degree.C. 5. Solute concentration ratio of 1:1 and some Rayleigh results

Miller, Donald G.; Albright, John G.; Mathew, Roy; Lee, Catherine M.; Rard, Joseph A.; Eppstein, Lee B.

doi:10.1021/j100117a040

Cited by 40 publications

(110 citation statements)

References 17 publications

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“…At low salt concentrations, long-range electrostatic effects can account for the salt-specific differences in their dependence on salt concentration. Our thermodynamic analysis demonstrates that the concentration dependence of (D 21 We suggest how the cross-diffusion coefficients may play a role in crystallization kinetics, with salt-ion insertion into the crystalline phase being enhanced during crystal growth due the magnitude and sign of (D 21 ) V . The other cross-coefficient, (D 21 ) V , might be important in initial clustering of lysozyme cations during nucleation.…”

Section: Discussionmentioning

confidence: 77%

“…To determine the number of fitting parameters sufficient for regression, we first retained only a 12 and a 21 in eqs 8a and 8b, respectively, and then included the higher-order parameters b 12 and b 21 for comparison. For KCl, this inclusion led to a significantly improved regression of eqs 8a and 8b and, consequently, better accuracy of z p , as previously found for NaCl 7 but not for NH 4 Cl.…”

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confidence: 99%

“…Examination of (D 21 ) V . Values of (D 21 ) V for NaCl, NH 4 Cl, and KCl at pH 4.5 are shown in Figure 1c.…”

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confidence: 99%

“…Indeed, the intercept can be directly obtained using relations for D 21 and D 22 shown in eq 10. We also observe that V h 1 is responsible for more than 80% of ω + V h 1 , the slope of (D 21 ) 0 /(D 22 ) 0 . This is again due to the large volume of the …”

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confidence: 99%

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The Effect of Salt on Protein Chemical Potential Determined by Ternary Diffusion in Aqueous Solutions

et al. 2005

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We use accurate thermodynamic derivatives extracted from high-precision measurements of the four volumefixed diffusion coefficients in ternary solutions of lysozyme chloride in aqueous NaCl, NH 4 Cl, and KCl at pH 4.5 and 25°C to (a) assess the relative contributions of the common-ion and nonideality effects to the protein chemical potential as a function of salt concentration, (b) compare the behavior of the protein chemical potential for the three salts, which we found to be consistent with the Hofmeister series, and (c) discuss our thermodynamic data in relation to the dependence of the protein solubility on salt concentration. The four diffusion coefficients are reported at 0.6 mM lysozyme chloride and 0.25, 0.5, 0.9, 1.2, and 1.5 M KCl and extend into the protein-supersaturated region. The chemical potential cross-derivatives are extracted from diffusion data using the Onsager reciprocal relation and the equality of molal cross-derivatives of solute chemical potentials. They are compared to those calculated previously from diffusion data for lysozyme in aqueous NaCl and NH 4 Cl. We estimate the effective charge on the diffusing lysozyme cation at the experimental concentrations. Our diffusion measurements on the three salts allowed us to analyze and interpret the four diffusion coefficients for charged proteins in the presence of 1:1 electrolytes. Our results may provide guidance to the understanding of protein crystallization.

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Section: Discussionmentioning

confidence: 77%

mentioning

confidence: 99%

“…Examination of (D 21 ) V . Values of (D 21 ) V for NaCl, NH 4 Cl, and KCl at pH 4.5 are shown in Figure 1c.…”

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confidence: 99%

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confidence: 99%

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The Effect of Salt on Protein Chemical Potential Determined by Ternary Diffusion in Aqueous Solutions

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“…Very careful investigation of cross-diffusion coefficients has been carried out in aqueous solutions of NaCl (c 1 ) and MgCl 2 (c 2 ), as well as in solutions of NaCl (c 1 ) and Na 2 SO 4 (c 2 ). 40,[106][107][108][109] For the NaCl-MgCl 2 system, at molar ratios c 1 /c 2 4 1 (e.g., c 1 /c 2 = 3), 40 In that work, the diffusion of charged macromolecules in the presence of an electrolyte solution was discussed in terms of two models: (a) the Nernst-Hartley equations, 96 applicable to an ideal dilute ternary solution with two ionic components, and; (b) the Stokes-Einstein equation, 110 which describes the tracer diffusion coefficient (or mobility) of macromolecules in the limit of c 1 -0. For both models, the diffusion coefficients are independent of the reference frame, because they apply at infinite dilution.…”

Section: Cross-diffusion Without Reactionmentioning

confidence: 99%

Cross-diffusion and pattern formation in reaction–diffusion systems

Vanag

Epstein

2009

Phys. Chem. Chem. Phys.

254

199

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Cross-diffusion, the phenomenon in which a gradient in the concentration of one species induces a flux of another chemical species, has generally been neglected in the study of reaction-diffusion systems.We summarize experiments that demonstrate that cross-diffusion coefficients can be quite significant, even exceeding ''normal,'' diagonal diffusion coefficients in magnitude in systems that involve ions, micelles, complex formation, excluded volume effects (e.g., surface or polymer reactions) and other phenomena commonly encountered in situations of interest to chemists. We then demonstrate with a series of model calculations that cross-diffusion can lead to spatial and spatiotemporal pattern formation, even in relatively simple systems. We also show that, in the absence of cross-diffusion among the reacting species, introduction of a nonreactive species that induces appropriate cross-diffusive fluxes with reactive species can lead to pattern formation.

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Ternary diffusivities by model‐based analysis of Raman spectroscopy measurements

et al. 2006

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in Wiley InterScience (www.interscience.wiley.com).Even though multicomponent mixtures are ubiquitous in mass transfer processes, mutual diffusion data in these systems are scarce. This is due to the fact that established diffusion measurements are laborious. In particular, several experiments are required to determine multicomponent diffusion coefficients at a single composition. In order to overcome these deficiencies, a diffusion experiment employing one-dimensional Raman spectroscopy is presented. Concentrations of the individual species are resolved with high spatial and temporal resolution during the diffusion process. In this work, it is shown that these data allow determining the ternary Fick diffusion matrix from a single isothermal diffusion experiment. The experimental procedure is further optimized using model-based experimental design techniques, where general design guidelines for diffusion experiments are derived. Thereby, precision of the diffusion measurements can be improved by an order of magnitude. The theoretical calculations are validated by experimental results for the system n-propanol þ 1-chlorobutane þ n-heptane.

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Isothermal diffusion coefficients of sodium chloride-magnesium chloride-water at 25.degree.C. 5. Solute concentration ratio of 1:1 and some Rayleigh results

Cited by 40 publications

References 17 publications

The Effect of Salt on Protein Chemical Potential Determined by Ternary Diffusion in Aqueous Solutions

The Effect of Salt on Protein Chemical Potential Determined by Ternary Diffusion in Aqueous Solutions

Cross-diffusion and pattern formation in reaction–diffusion systems

Ternary diffusivities by model‐based analysis of Raman spectroscopy measurements

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