scholarly journals A reactive transport model for evaluating the long-term performance of stainless steels in concrete

Author(s):  
M. Boulfiza
Minerals ◽  
2021 ◽  
Vol 11 (9) ◽  
pp. 1026
Author(s):  
Keith Bateman ◽  
Shota Murayama ◽  
Yuji Hanamachi ◽  
James Wilson ◽  
Takamasa Seta ◽  
...  

The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH > 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid, and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a mudstone, comparing data from sequential flow experiments with the results of reactive transport modelling. The reaction of the mudstone with the cement leachates resulted in small changes in pH with the precipitation of calcium aluminium silicate hydrate (C-(A-)S-H) phases of varying compositions. As the system evolves, secondary C-(A-)S-H phases re-dissolve and are replaced by secondary carbonates. This general sequence was successfully simulated using reactive transport modelling.


2018 ◽  
Vol 8 (12) ◽  
pp. 2597 ◽  
Author(s):  
Yogarajah Elakneswaran ◽  
Eiji Owaki ◽  
Toyoharu Nawa

Cementitious materials are one of the essential components for low- and intermediate-level waste disposal sites. Low-level nuclear waste from power plants consists of highly concentrated (~25 wt %) Na2SO4, and the wastes are solidified with cementitious materials. Degradation of cementitious materials that result from chemical and physical sulphate attack is a major concern in the safety of the waste disposal. In this study, hydration and reactive transport models, developed in previous works by the authors, were applied with Pitzer interactions coefficients to evaluate the long-term performance of Portland cement (PC) solidified with high concentration of Na2SO4. Expansive sulphate-bearing products of ettringite and mirabilite were formed and filled the pores in the hydrating PC with 25% of Na2SO4 by weight, but they were destabilised as temperature increased. Influence of Na2SO4 concentration and temperature on mineralogical changes is discussed. The simulation results from the reactive-transport model showed that the degradation of solidified Na2SO4 waste by cementitious materials exposed to 10% Na2SO4 for 1000 years is due to dissolution of mirabilite and secondary formation of ettringite, but not Na2SO4 crystallisation. The phases and porosity became stable close to exposure surface after 10 years, although the deterioration progressed from the surface to core with exposure time.


2021 ◽  
Vol 11 (19) ◽  
pp. 9314
Author(s):  
Svenja Steding ◽  
Thomas Kempka ◽  
Michael Kühn

Potash seams are a valuable resource containing several economically interesting, but also highly soluble minerals. In the presence of water, uncontrolled leaching can occur, endangering subsurface mining operations. In the present study, the influence of insoluble inclusions and intersecting layers on leaching zone evolution was examined by means of a reactive transport model. For that purpose, a scenario analysis was carried out, considering different rock distributions within a carnallite-bearing potash seam. The results show that reaction-dominated systems are not affected by heterogeneities at all, whereas transport-dominated systems exhibit a faster advance in homogeneous rock compositions. In return, the ratio of permeated rock in vertical direction is higher in heterogeneous systems. Literature data indicate that most natural potash systems are transport-dominated. Accordingly, insoluble inclusions and intersecting layers can usually be seen as beneficial with regard to reducing hazard potential as long as the mechanical stability of leaching zones is maintained. Thereby, the distribution of insoluble areas is of minor impact unless an inclined, intersecting layer occurs that accelerates leaching zone growth in one direction. Moreover, it is found that the saturation dependency of dissolution rates increases the growth rate in the long term, and therefore must be considered in risk assessments.


2021 ◽  
Author(s):  
Ahmed M. S. Elgendy ◽  
Simone Ricci ◽  
Elena I. Cojocariu ◽  
Claudio Geloni

Abstract Dynamic-geochemical model is a powerful instrument to evaluate the geochemical effects on CO2storage capacity, injectivity and long-term containment. The study objective is to apply an integrated multi-step workflow to a carbon capture and storage (CCS) candidate field (offshore), namely hereinafter H field. From experimental analyses, a comprehensive real data-tailored reactive transport model (RTM) has been built to capture the dynamics and the geochemical phenomena (e.g., water vaporization, CO2solubility, mineral alteration) occurring during and after the CO2injection in sedimentary formations. The proposed integrated workflow couples lab activities and numerical simulations and it is developed according to the following steps: Mineralogical-chemical characterization (XRD, XRF and SEM-EDX experimental techniques) of field core samples; Data elaboration and integration to define the conceptual geochemical model; Synthetic brine reconstruction by means of 0D geochemical models; Numerical geochemical modelling at different complexity levels. Field rocks chosen for CO2injection have been experimentally characterized, showing a high content of Fe in clayey, micaceous and carbonate mineralogical phases. New-defined, site-specific minerals have been characterized, starting from real XRD, XRF and SEM-EDX data and by calculation of their thermochemical parameters with a proprietary procedure. They are used to reconstruct synthetic formation water chemical composition (at equilibrium with both rock mineralogy and gas phase), subsequently used in RTM. CO2injection is simulated using 2D radial reactive transport model(s) built in a commercial compositional reservoir simulator. The simulations follow a step-increase in the complexity of the model by adding CO2solubility, water vaporization and geochemical reactions. Geochemical processes impact on CO2storage capacity and injectivity is quantitatively analyzed. The results show that neglecting the CO2solubility in formation water may underestimate the max CO2storage capacity in H field by around 1%, maintaining the same pressure build-up profile. Sensitivities on the impact of formation water salinity on the CO2solubility are presented. In a one thousand years’ time-scale, changes in reservoir porosity due to mineral alteration, triggered by CO2-brine-rock interactions, seem to be minimal in the near wellbore and far field. However, it has been seen that water vaporization with the associated halite precipitation inclusion in the simulation models is recommended, especially at high-level of formation brine salinity, for a reliable evaluation of CO2injectivity related risks. The proposed workflow provides a new perspective in geochemical application for CCS studies, which relies on novel labs techniques (analyses automation), data digitalization, unification and integration with a direct connection to the numerical models. The presented procedure can be followed to assess the geochemical short-and long-term risks in carbon storage projects.


Clay Minerals ◽  
2013 ◽  
Vol 48 (2) ◽  
pp. 185-197 ◽  
Author(s):  
T. Yamaguchi ◽  
M. Kataoka ◽  
T. Sawaguchi ◽  
M. Mukai ◽  
S. Hoshino ◽  
...  

AbstractHighly alkaline environments induced by cement-based materials are likely to cause the physical and/or chemical properties of the bentonite buffer materials in radioactive waste repositories to deteriorate. Assessing long-term alteration of concrete/clay systems requires physicochemical models and a number of input parameters. In order to provide reliability in the assessment of the long-term performance of bentonite buffers under disposal conditions, it is necessary to develop and verify reactive transport codes for concrete/clay systems. In this study, a PHREEQC-based, reactive transport analysis code (MC-CEMENT ver. 2) was developed and was verified by comparing results of the calculations with in situ observations of the mineralogical evolution at the concrete/argillite interface. The calculation reproduced the observations such as the mineralogical changes in the argillite limited to within 1 cm in thickness from the interface, formation of CaCO3 and CSH, dissolution of quartz, decrease of porosity in the argillite and an increase in the concrete. These agreements indicate a possibility that models based on lab-scale (∼1 year) experiments can be applied to longer time scales although confidence in the models is necessary for much longer timescales. The fact that the calculations did not reproduce the dissolution of clays and the formation of gypsum indicates that there is still room for improvement in our model.


Geofluids ◽  
2019 ◽  
Vol 2019 ◽  
pp. 1-16
Author(s):  
Huixing Zhu ◽  
Tianfu Xu ◽  
Hailong Tian ◽  
Guanhong Feng ◽  
Zhijie Yang ◽  
...  

To further understand the interactions of CO2-brine-rock at geological time scales, in this study, a 1D reactive transport model of CO2 intrusion into sandstone of the Longtan Formation (P2l) in the Huangqiao area, China, was constructed based on site-specific data. The simulation time is consistent with the retention time of CO2 in the Longtan sandstone Formation and is set to 20 Ma. The reactive transport model is calibrated and revised using the measured data for sandstone samples from Well X3 (i.e., the natural analogue). By comparing the simulation results with measured data for the natural analogue, the long-term geochemical reactions are investigated. The simulation results indicate that the brine-rock interactions induced by CO2 can be roughly divided into two stages. First, susceptible minerals (e.g., chlorite, ankerite, calcite, and feldspar minerals) dissolve rapidly under acidic conditions formed by the dissolution of CO2. The precipitation of siderite is facilitated by the dissolution of ankerite and chlorite. Smectite-Ca and dawsonite precipitate due to the dissolution of anorthite and albite, respectively. Dawsonite begins to convert into smectite-Na when albite is completely dissolved. As the reactions continue, intermediate products (i.e., illite, smectite-Na, and smectite-Ca) generated in the first stage become the reactants and subsequently react with CO2 and brine. These three clay minerals are not stable under acidic conditions and transform into kaolinite and paragenetic quartz in the later stage of reaction. Comparing the simulation results of the Base Case with the measured data for the natural analogue and inspired by previous studies, the scour of kaolinite is supposed to have occurred in this region and is considered in the revised model by introducing a coefficient of the scour of kaolinite (i.e., Case 2). The simulation results of Case 2 fit well with the measured data on mineral assemblage, and the trend of the sandstone porosity growth caused by the CO2-brine-rock reaction is captured by our simulation results. The combination of numerical simulation and natural analogue study indicates that the joint effects of long-term CO2-brine-rock reactions and scour of kaolinite increase the pore space of the host rock and result in an increase in quartz content in the sandstone.


2008 ◽  
Vol 33 ◽  
pp. S285-S294 ◽  
Author(s):  
T. Yamaguchi ◽  
F. Yamada ◽  
K. Negishi ◽  
S. Hoshino ◽  
M. Mukai ◽  
...  

Author(s):  
Carl Malings ◽  
Rebecca Tanzer ◽  
Aliaksei Hauryliuk ◽  
Provat K. Saha ◽  
Allen L. Robinson ◽  
...  

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