Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions. II. Rate constants, effective surface area, and the hydrolysis of feldspar

Helgeson, Harold C.; Murphy, William M.; Aagaard, Per

doi:10.1016/0016-7037(84)90294-1

Cited by 561 publications

(215 citation statements)

References 59 publications

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“…The ratio of the measured surface area using gas adsorption to the geometric surface area has been defined as surface roughness (Helgeson et al, 1984;Brantley and Mellott, 2000). The BET surface area for the LAW 1123 bed product is over 200 times greater than the geometric, and more than 120 times greater for the SBW 1173 bed product.…”

Section: Surface Areamentioning

confidence: 99%

Single-Pass Flow Through (SPFT) Testing of Fluidized-Bed Steam Reforming (FBSR) Waste Forms

Lorier¹,

Pareizs²,

Jantzen³

2005

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EXECUTIVE SUMMARYTwo samples of fluidized-bed steam reforming (FBSR) mineral waste form product were subjected to single-pass flow-through (SPFT) testing. Sample LAW 1123 resulted from pilot-scale FBSR processing with a Hanford Envelope A low-activity waste (LAW) simulant. Sample SBW 1173 resulted from pilot-scale FBSR processing with an Idaho National Laboratory (INL) simulant commonly referred to as sodium-bearing waste (SBW). The pilot-scale waste forms were made at the Science and Technology Applications Research (STAR) facility in Idaho Falls, Idaho. The durability of the two FBSR waste forms was assessed via the SPFT test in this study. Both samples were multiphase mineral waste forms, so the SPFT test results provide an overall release rate from the multiple mineral species in each sample and are dependent on the amount of each phase present and the mineralogy of the phases present. SPFT testing was performed at temperatures of 25°, 40°, 70°, and 90°C on LAW 1123, while SBW 1173 was only tested at 70° and 90°C. The 70° and 90°C data were compared to each other and the LAW-1123 results were compared to previous testing performed by the Pacific Northwest National Laboratory (PNNL) on a LAW Envelope C (high organic content) waste simulant.The objectives of this study were to obtain forward dissolution rate data for both STAR FBSR bed products (using SPFT tests). Also, a qualitative comparison of the FBSR bed products to a glass waste form (specifically the low-activity reference material (LRM) glass) was performed. For these comparisons, the relative surface areas of the FBSR and glass products had to be measured. Due to the more porous and irregular surface of FBSR bed products, the surface area of the bed products was determined using the Brunauer, Emmett, and Teller (BET) measurement method. The surface area of a glass is much smoother and the calculated geometric surface area is typically used for determining dissolution behavior.Presently there are no specifications or standard release rates that the FBSR tested materials have to meet, e.g. the data from the FBSR testing is normally used during subsequent Performance Assessment (PA) calculations. Since a PA calculation is not part of this study, the LAW and SBW steam reforming samples were compared to each other, to previous LAW FBSR SPFT results, and to the results from the LRM reference glass. The experimental durability data generated from this study suggests that an FBSR mineral waste form product would be an adequate alternative form to borosilicate glass. The tested FBSR mineral waste forms showed normalized release rates for matrix elements such as Si to be more than 200X slower than the LRM glass. However, further durability testing and mineral phase information is recommended to further substantiate these findings.

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Section: Surface Areamentioning

confidence: 99%

Single-Pass Flow Through (SPFT) Testing of Fluidized-Bed Steam Reforming (FBSR) Waste Forms

Lorier¹,

Pareizs²,

Jantzen³

2005

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“…The improvement of the dissolution rate of silicate minerals by microbially produced organic acids is mainly occurring due to the exchange of hydrogen ion for the cation ion the lattice (Fig. 1.4a) (Helgeson et al, 1984;White & Brantley, 1995). Other mechanisms that have been reported to accelerate the leaching rate of cations is adsorption and complexation of organic ligands with reactive sites on the mineral surface ( Fig.…”

Section: Microbial Mediated Co 2 Mineral Carbonationmentioning

confidence: 99%

Mineral CO2 sequestration by environmental biotechnological processes

Salek

Kleerebezem

Jonkers

et al. 2013

Trends in Biotechnology

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“…Recently, Jantzen and Pareizs [7] have proposed an Activated Complex Theory (ACT) model based on the early work of Helgeson [8] and the more recent work of Oelkers [9] on basalt glass dissolution. This approach attempts to define the activated complexes that participate in the irreversible formation of the glass gel layer.…”

Section: Product Constraint: Durabilitymentioning

confidence: 99%

High Level Waste (HLW) Vitrification Experience in the US: Application of Glass Product/Process Control to Other HLW and Hazardous Wastes

Jantzen

Marra

2008

MRS Proc.

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Vitrification is currently the most widely used technology for the treatment of high level radioactive wastes (HLW) throughout the world. At the Savannah River Site (SRS) actual HLW tank waste has successfully been processed to stringent product and process constraints without any rework into a stable borosilicate glass waste since 1996. A unique "feed forward" statistical process control (SPC) has been used rather than statistical quality control (SQC). In SPC, the feed composition to the melter is controlled prior to vitrification. In SQC, the glass product is sampled after it is vitrified. Individual glass property models form the basis for the "feed forward" SPC. The property models transform constraints on the melt and glass properties into constraints on the feed composition. The property models are mechanistic and depend on glass bonding/structure, thermodynamics, quasicrystalline melt species, and/or electron transfers. The mechanistic models have been validated over composition regions well outside of the regions for which they were developed because they are mechanistic. Mechanistic models allow accurate extension to radioactive and hazardous waste melts well outside the composition boundaries for which they were developed.

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Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions. II. Rate constants, effective surface area, and the hydrolysis of feldspar

Cited by 561 publications

References 59 publications

Single-Pass Flow Through (SPFT) Testing of Fluidized-Bed Steam Reforming (FBSR) Waste Forms

Single-Pass Flow Through (SPFT) Testing of Fluidized-Bed Steam Reforming (FBSR) Waste Forms

Mineral CO2 sequestration by environmental biotechnological processes

High Level Waste (HLW) Vitrification Experience in the US: Application of Glass Product/Process Control to Other HLW and Hazardous Wastes

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