Calculation of mass transfer in geochemical processes involving aqueous solutions

Helgeson, Harold C.; Brown, Thomas H.; Nigrini, Andrew; Jones, Thomas A.

doi:10.1016/0016-7037(70)90017-7

Cited by 227 publications

(76 citation statements)

References 6 publications

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“…The EQ3/6 geochemical software package is a set of computer codes and supporting thermodynamic and kinetic databases that calculates the solubilities of minerals and other solids and the speciation of solutes in aqueous solutions (EQ3NR), and predicts chemical reactions between these solutions and solids, gases, or other aqueous solutions (EQ6). Wolery [1978] first developed EQ3/6 to model basalt-seawater reactions in hydrothermal systems at mid-ocean ridges; he patterned EQ3/6 after the PATHI code developed by Helgeson [1968] and Helgeson et al [1970]. Subsequently, Wolery and his colleagues at LLNL have continued the development of EQ3/6, mainly for application to various radioactive-waste repositories.…”

Section: Geochemical Modeling Methodologymentioning

confidence: 99%

Compliance Assessment Document for the Transuranic Wastes in the Greater Confinement Disposal Boreholes at the Nevada Test Site, Volume 2: Performance Assessment

Cochran¹,

Beyeler²,

Brosseau³

et al. 2001

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Intermediate depth disposal operations were conducted by the U.S. Department of Energy (DOE) at the DOE's Nevada Test Site (NTS) from 1984 through 1989. These operations emplaced highspecific activity low-level wastes (LLW) and limited quantities of classified, "special case" transuranic (TRU) wastes in 37 m (120-ft) deep, 3 m (10 ft) diameter Greater Confinement Disposal (GCD) boreholes.Four boreholes contain about 60,000 kg (132,000 lb.) of classified TRU waste packages, containing less than 330 curies of Plutonium-239. All of the TRU wastes emplaced in the GCD boreholes are classified for national security reasons and cannot be disposed of in the DOE's Waste Isolation Pilot Plant.The U.S. Environmental Protection Agency's (EPA's) 40 CFR 191 defines the requirements for protection of human health from disposed TRU wastes. This EPA standard sets a number of requirements, including probabilistic limits on the cumulative releases of radionuclides to the accessible environment for 10,000 years. This report presents the performance assessment (PA) that has been conducted to determine if disposal of TRU waste in the GCD boreholes complies with the EPA's 40 CFR 191 requirements.Sandia National Laboratories completed this PA using all available information and an Iterative PA Methodology, which focused work on uncertainty reduction in a cost-effective fashion that does not overestimate system performance and assured defensibility. The simplicity of the conceptual models of the GCD disposal system allowed them to be implemented in Microsoft ® Visual Basic™ macros in an Access™ database. This PA model is built from a mathematical expression for mass conservation that includes the operation of a number of transport processes, including dissolution, precipitation, reversible chemical sorption onto soil, advection, diffusion, dispersion, radioactive decay and ingrowth, plant uptake, and bioturbation. The mathematical model and implementing code was used to calculate a complementary cumulative distribution function of integrated normalized release to the accessible environment for 10,000 years and probability distributions of dose based on two exposure conditions for the 1,000 year individual protection requirements.The primary conclusions of this PA are that the disposal of TRU wastes in the GCD boreholes will, at most, result in minuscule doses to individuals, and that the GCD disposal system easily meets the EPA's 1985, 40 CFR 191 requirements for disposal of TRU waste. Further, there is a strong, reasonable expectation that actual system performance will be better than what is simulated in this PA.vi ACKNOWLEDGMENTS

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Section: Geochemical Modeling Methodologymentioning

confidence: 99%

Compliance Assessment Document for the Transuranic Wastes in the Greater Confinement Disposal Boreholes at the Nevada Test Site, Volume 2: Performance Assessment

Cochran¹,

Beyeler²,

Brosseau³

et al. 2001

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“…Essentially, for a geochemical system that has n species, the following ordinary differential equations completely define the geochemical reaction network in a well-mixed reactor (Helgeson et al, 1970),…”

Section: Conceptual Models and Assumptionsmentioning

confidence: 99%

Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems: 4. Numerical modeling of kinetic reaction paths

Zhu

Lü

Zheng

et al. 2010

Geochimica et Cosmochimica Acta

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This paper explores how dissolution and precipitation reactions are coupled in batch reactor experimental systems at elevated temperatures. This is the fourth paper in our series of "Coupled Alkali Feldspar Dissolution and Secondary Mineral Precipitation in Batch Systems". In our third paper, we demonstrated via speciation-solubility modeling that partial equilibrium between secondary minerals and aqueous solutions was not attained in feldspar hydrolysis batch reactors at 90-300°C and that a strong coupling between dissolution and precipitation reactions follows as a consequence of the slower precipitation of secondary minerals ). Here, we develop this concept further by using numerical reaction path models to elucidate how the dissolution and precipitation reactions are coupled. Modeling results show that a quasi-steady state was reached. At the quasi-steady state, dissolution reactions proceeded at rates that are orders of magnitude slower than the rates measured at far from equilibrium. The quasi-steady state is determined by the relative rate constants, and strongly influenced by the function of Gibbs free energy of reaction (DG r ) in the rate laws.To explore the potential effects of fluid flow rates on the coupling of reactions, we extrapolate a batch system (Ganor et al., 2007) to open systems and simulated one-dimensional reactive mass transport for oligoclase dissolution and kaolinite precipitation in homogeneous porous media. Different steady states were achieved at different locations along the one-dimensional domain. The time-space distribution and saturation indices (SI) at the steady states were a function of flow rates for a given kinetic model. Regardless of the differences in SI, the ratio between oligoclase dissolution rates and kaolinite precipitation rates remained 1.626, as in the batch system case (Ganor et al., 2007). Therefore, our simulation results demonstrated coupling among dissolution, precipitation, and flow rates.Results reported in this communication lend support to our hypothesis that slow secondary mineral precipitation explains part of the well-known apparent discrepancy between lab measured and field estimated feldspar dissolution rates (Zhu et al., 2004). Here we show how the slow secondary mineral precipitation provides a regulator to explain why the systems are held close to equilibrium and show how the most often-quoted "near equilibrium" explanation for an apparent field-lab discrepancy can work quantitatively. The substantiated hypothesis now offers the promise of reconciling part of the apparent fieldlab discrepancy.

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“…Recognition of evaporite involvement in the Lavicky magmatic system has implications for economic mineralization in the region, as evaporites typically contain large quantities of anions that are necessary for mobilizing and transporting metals (e.g., Helgeson et al, 1970;Barnes, 1979). It is also noteworthy here that many Sn deposits are associated with quartz-tourmaline orbicule-bearing leucogranites, for example at Cornwall, England (Brammall and Harwood, 1925), Malaysia (Hutchison and Leow, 1963), Yukon Territory (Sinclair and Richardson, 1992), and Tasmania (Taylor, 1979).…”

Section: Disscusions On Possible Primary Boron Sources For the Granitementioning

confidence: 99%

Chemical and boron isotopic compositions of tourmaline from the Lavicky leucogranite, Czech Republic

et al. 2003

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Abundant tourmaline occurs in the Lavicky leucogranite, Czech Republic as spherical to ovoid quartztourmaline orbicules, typically 5 to 7 cm in diameter. The tourmalines also occur as fine-grained quartztourmaline veins (<1 cm thick) that cut the orbicule-rich granite. Electron microprobe analyses reveal that tourmaline from the quartz-tourmaline orbicules is Fe-rich schorl with a range of Fe/(Fe+Mg) ratio 0.62 to 0.77 and Na/(Na+Ca) ratio 0.82 to 0.95. In contrast, tourmaline from quartz-tourmaline veins is Mg-rich dravite with a range of Fe/(Fe+Mg) ratio 0.23 to 0.45 and Na/(Na+Ca) ratio 0.67 to 0.90. Very low δ 11 B values of -37.3 to -32.1‰ are found in the tourmalines from the orbicules, whereas tourmalines from the veins display relatively higher δ 11 B values of -28.2 to -21.3‰. The overall large δ 11 B variation is suggested to reflect mixing of different boron sources and boron isotope fractionation during magmatic degassing and magmatic-hydrothermal evolution at late solidus to early subsolidus stages of granite crystallization. Only non-marine evaporites show very negative δ 11 B values (<-20‰) in all natural boron reservoirs, hence, the very low δ 11 B values of the quartz-tourmaline orbicules likely indicate a major contribution of boron from non-marine evaporites that probably exist in the magma source regions or assimilated into the magma during its ascent. Quartz-tourmaline orbicules may have formed during a transition from magmatic to hydrothermal processes, whereas the vein tourmalines formed by mixing of the exsolved magmatic-hydrothermal fluids with an external fluid rich in Ca and Mg and having higher δ 11 B than the exsolved magmatic fluids.

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Calculation of mass transfer in geochemical processes involving aqueous solutions

Cited by 227 publications

References 6 publications

Compliance Assessment Document for the Transuranic Wastes in the Greater Confinement Disposal Boreholes at the Nevada Test Site, Volume 2: Performance Assessment

Compliance Assessment Document for the Transuranic Wastes in the Greater Confinement Disposal Boreholes at the Nevada Test Site, Volume 2: Performance Assessment

Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems: 4. Numerical modeling of kinetic reaction paths

Chemical and boron isotopic compositions of tourmaline from the Lavicky leucogranite, Czech Republic

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