Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging

Weber, James H.; Bracco, Jacquelyn N.; Poplawsky, Jonathan D.; Ievlev, Anton V.; More, Karren L.; Lorenz, Matthias; Bertagni, Angela L.; Jindra, Sarah A.; Starchenko, Vitalii; Stack, Andrew G.

doi:10.1021/acs.cgd.8b00839

Cited by 24 publications

(37 citation statements)

References 73 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In addition, studies on the removal of Sr by barite precipitation have shown that the effect of ionic strength and competitive ions (Ca 2+ and Mg 2+ ) can be neglected at higher supersaturation [39]. Recent studies on crystal growth of barite in the presence of Sr aq at low supersaturation indicate important implications of the Sr/Ba-ratio in solution on barite growth [40][41][42]. These studies described the inhibiting effect of strontium on barite growth observed in our study.…”

Section: Effect Of Sr In Solution: Kinetics Of Ra-uptake and Approachsupporting

confidence: 63%

“…These studies described the inhibiting effect of strontium on barite growth observed in our study. At elevated temperatures of 108 • C, Weber et al (2018) [41] observed that at low Sr/Ba ratios (<5.5) in the solution Sr aq is inhibiting barite crystal growth. In contrast, at higher aqueous Sr/Ba ratios the inhibiting effect of strontium on barite growth is overcome by a shift in the growth mechanism from typical barite growth to celestine growth.…”

Section: Effect Of Sr In Solution: Kinetics Of Ra-uptake and Approachmentioning

confidence: 99%

See 1 more Smart Citation

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

Brandt¹,

Klinkenberg²,

Poonoosamy³

et al. 2018

Minerals

Self Cite

View full text Add to dashboard Cite

Recrystallization and solid-solution formation with barite is considered as relevant retention mechanism for 226Ra in long-term scenarios of nuclear waste management. Here, we studied the effect of ionic strength and the presence of Sr in solution upon the Ra-uptake kinetics and final Ra concentrations in solution by recrystallizing barite in solution with varying Sr and NaCl concentration and temperature for up to 1000 days. Final Ra-concentrations were interpreted based on thermodynamic modelling. Our results indicate a slight decrease of the retention potential of barite for Ra but little effect on the uptake kinetics due to the increase of ionic strength from. 0.1 mol/kg to 1.0 mol/kg of NaCl. The final concentrations at solid/liquid ratio of 0.5 g/kg are well described based on available thermodynamic models whereas at 5 g/kg additional Ra uptake probably due to kinetic effects was observed. On the contrary, the presence of Sr in solution can have a significant inhibiting kinetic effect on the uptake kinetics and lower the final Ra-uptake. In some cases, with low solid/liquid ratio or at ambient conditions, Sr completely inhibits barite recrystallization. In all other cases, Ra, Ba and Sr were taken up as thermodynamically predicted at the end of the experiments.

show abstract

Section: Effect Of Sr In Solution: Kinetics Of Ra-uptake and Approachsupporting

confidence: 63%

Section: Effect Of Sr In Solution: Kinetics Of Ra-uptake and Approachmentioning

confidence: 99%

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

Brandt¹,

Klinkenberg²,

Poonoosamy³

et al. 2018

Minerals

Self Cite

View full text Add to dashboard Cite

show abstract

“…Inductively coupled plasma atomic emission 134 spectroscopy (ICP-AES -Thermo ICAP 6000) was used for the analyses of Ba 2+ and Na + , and ion chromatography (ICS-5000 Thermofisher Dionex) was used for the analyses of SO4 2and Cl -. Because foreign cations such as Sr can impact barite growth rates 17 , all input solutions were analyzed for major (Na, K, Ca, Mg, Fe, Si, Al) and minor (Sr, Ni, Mn, Ti, Co, Cr, Zn, Cu) cations prior to the immersion of the barite samples. The concentration of all of these elements was systematically below the detection limit (≤ 5 ppb), except for Cu, for which concentrations up to 20 ppb (8×10 -8 M) were occasionally 140 detected.…”

Section: Growth Experiments and Analytical Proceduresmentioning

confidence: 99%

Barite Growth Rates as a Function of Crystallographic Orientation, Temperature, And Solution Saturation State

Vital

Daval

Morvan

et al. 2020

Crystal Growth & Design

View full text Add to dashboard Cite

Barite growth kinetics was investigated as a function of crystallographic orientation for temperatures between 10 and °C, and initial saturation indices (SI) of 1.1 and 2.1. The growth rates were estimated for (001), ( 210), and (101) faces using vertical scanning interferometry. Overall, face-specific barite growth rates ( ( ) ) can be successfully described by the following rate law:where ( ) and() represent the face-specific Arrhenius pre-exponential factor and activation 24 energy, respectively, R is the gas constant, and T refers to the absolute temperature. In addition, because of the modest growth anisotropy of the various investigated faces, the following isotropic rate law can be used to satisfactorily account for the measured rate data: ( ) = . exp(− ⁄ ). (10 − 1)with average values of A = exp(13.59) nm.h -1 and Ea = 35.0 ± 2.5 kJ.mol -1 . Over the range of conditions investigated in the present study, our results suggest that barite growth kinetics is surface-controlled, while possibly verifying the principle of detailed balancing and micro-reversibility. These results imply that previous modeling exercises of steady-state barite growth based on isotropic rate laws may remain valid, at least over the range of conditions investigated in the present study.

show abstract

“…Studies on the thermodynamics of (Ba x , Sr 1−x )SO 4 solid solutions are still under active development (37), and one of the uncertainties is the interaction parameter of Ba-Sr ions in (Ba x , Sr 1−x )SO 4 solid solutions, which determines the ideality (SI Appendix, section 1.3) and the free energy of mixing (SI Appendix, section 1.4) of the solid solution (35)(36)(37)(38)(39). Using the interaction parameters developed by different models (35,36), the calculated compositions (i.e., x) varied to some extent but were all in general consistent with the measured compositions of (Ba x , Sr 1−x )SO 4 .…”

Section: Sr Enrichment In Heterogeneous (Ba X Sr 1−x )So 4 Precipitmentioning

confidence: 99%

Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba _x , Sr _{1−
x} )SO ₄ from undersaturated solution

Deng

Stack

Weber

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

Self Cite

View full text Add to dashboard Cite

Sr-bearing marine barite [(Ba x , Sr 1−x )SO 4 ] cycling has been widely used to reconstruct geochemical evolutions of paleoenvironments. However, an understanding of barite precipitation in the ocean, which is globally undersaturated with respect to barite, is missing. Moreover, the reason for the occurrence of higher Sr content in marine barites than expected for classical crystal growth processes remains unknown. Field data analyses suggested that organic molecules may regulate the formation and composition of marine barites; however, the specific organic-mineral interactions are unclear. Using in situ grazing incidence small-angle X-ray scattering (GISAXS), size and total volume evolutions of barite precipitates on organic films were characterized. The results show that barite forms on organic films from undersaturated solutions. Moreover, from a single supersaturated solution with respect to barite, Sr-rich barite nanoparticles formed on organics, while micrometer-size Sr-poor barites formed in bulk solutions. Ion adsorption experiments showed that organic films can enrich cation concentrations in the adjacent solution, thus increasing the local supersaturation and promoting barite nucleation on organic films, even when the bulk solution was undersaturated. The Sr enrichment in barites formed on organic films was found to be controlled by solid-solution nucleation rates; instead, the Sr-poor barite formation in bulk solution was found to be controlled by solid-solution growth rates. This study provides a mechanistic explanation for Sr-rich marine barite formation and offers insights for understanding and controlling the compositions of solid solutions by separately tuning their nucleation and growth rates via the unique chemistry of solution-organic interfaces.Sr-rich marine barite | organic-mineral interactions | solid solution | nucleation and growth | paleoenvironments S r-bearing barite [(Ba x , Sr 1−x )SO 4 ] is an important marine authigenic mineral present in the seawater column and marine sediments (1-5). Marine barite formation, essential to the global cycles of organic carbon, sulfate, and oxygen, can be used to reconstruct the changes in geochemical cycles and paleoproductivity, and Sr incorporation may reflect the oceanographic conditions (2, 5-7). Despite the geochemical importance of marine (Ba x , Sr 1−x )SO 4 formation, two paradoxes still exist. First, the global oceans are undersaturated with respect to barite, while barite is extensively present in seawater column and marine sediments (5,7,8). Second, Sr-rich marine barite (>50 mol% strontium) formation (7, 9) is not thermodynamically favorable (7, 10), as the solubility of SrSO 4 (K sp,SrSO4 = 10 −6.63 ) is three orders of magnitude higher than BaSO 4 (K sp,BaSO4 = 10 −9.98 ) (3, 10). Field and laboratory studies provide evidence for the association of organics with both paradoxes (7, 11); however, the specific roles of organics in these thermodynamically unfavorable mineralization processes are not clear (7,11,12).Organic-mineral interac...

show abstract

Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging

Cited by 24 publications

References 73 publications

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

Barite Growth Rates as a Function of Crystallographic Orientation, Temperature, And Solution Saturation State

Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba _x , Sr _{1−
x} )SO ₄ from undersaturated solution

Contact Info

Product

Resources

About

Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging

Cited by 24 publications

References 73 publications

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

The Effect of Ionic Strength and Sraq upon the Uptake of Ra during the Recrystallization of Barite

Barite Growth Rates as a Function of Crystallographic Orientation, Temperature, And Solution Saturation State

Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba x , Sr 1− x )SO 4 from undersaturated solution

Contact Info

Product

Resources

About

Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba _x , Sr _{1−
x} )SO ₄ from undersaturated solution