Mineral Dissolution Rates Research Articles

Fluid–rock interaction controlled by integrated hydrothermal fluid and fault: Implications for reservoir development

Hydrothermal activity is prevalent in petroliferous basins, particularly in fractured reservoirs. Hydrothermal fluids enter the reservoirs and cause significant fluid–rock interaction, which ultimately controls reservoir development. The Mahu Sag in western China is a hydrocarbon-rich region where hydrothermal fluids and faults control the reservoirs, making it challenging to understand the development mechanism of the shale reservoirs. This study focused on the Fengcheng Formation in the Mahu Sag. Based on a range of previous lithological test results, numerical models of hydrothermal fluid charging were established to explore differences in fluid–rock interactions under varying temperature, fluid, and flow rates. Results revealed that within a specific range, increasing temperature and Mg2+ concentration promoted hydrothermal processes. The hydrothermal flow rate influenced ion accumulation on the fluid-rock contact surface, thus controlling mineral dissolution rates. In a certain range, when the flow rate is increased by 3 times, the growth rate of dolomite content is increased by more than 15 times. Hydrothermal fluid flowing near the fault underwent chemical action more readily than in other areas. The influence of hydrothermal fluid and fault on reservoir development was both constructive and destructive. The decrease and increase of porosity are 30 % and 25 %, respectively. This study could provide a theoretical basis for identifying factors influencing shale reservoir development.

Incorporation of trace metals in Hanford waste boehmite mineral phases and dissolution rate impacts

AbstractData from radioactive Hanford tank waste samples was analyzed to assess whether trace metals present were incorporated into the bulk boehmite matrix or were simply intermingled with the bulk material and subsequent impacts to the boehmite dissolution rate. Results suggest that chromium is primarily blended into the bulk boehmite, with a small fraction present on the surface of the solids. However, increasing the level of chromium incorporation 30‐fold decreased the dissolution rate of boehmite by only 8%, suggesting incorporation of chromium into these samples had a minimal impact on the dissolution rate. Iron was also found to be incorporated in the boehmite solids. Silicon appears to be simply intermingled and not blended into the boehmite crystals.

In-situ wet carbonation of steel slag powder paste made with carbonated water: Interaction mechanism between carbonation and hydration

The utilization of steel slag powder is severely limited by its low activity. This study reveals that in-situ wet carbonation with carbonated water can significantly enhance its hydration activity. The influencing mechanism of carbonation on the hydration process and its kinetics during hydration are explored, and on this basis, the interaction between carbonation and hydration is discussed. It is found that both hydration and carbonation exhibit distinct characteristics before and after the acceleration stage. Before the acceleration stage, the hydration rate is affected by mineral dissolution rate, which is dependent on carbonation reaction, with carbonation rate determined by the CO2 concentration. After entering the acceleration stage, the hydration rate is promoted by the increased nucleation effect (e.g., nano-CaCO3 precipitation). The hydration in this period dominates carbonation by controlling mineral dissolution rate, with carbonation rate dependent on the mineral dissolution rate. As a result, mineral dissolution is shown to act as a bridge between hydration and carbonation interactions. Based on these results, the lack of further increase in hydration activity of steel slag powder with higher concentrations of carbonated water is also explained. This study provides a deep understanding for wet carbonation in steel slag powder paste.

The impact of adsorption–desorption reactions on the chemistry of Himalayan rivers and the quantification of silicate weathering rates

Common environmental adsorbents (clay minerals, metal-oxides, metal-oxyhydroxides and organic matter) can significantly impact the chemistry of aqueous fluids via adsorption–desorption reactions. The dissolved chemistry of rivers have routinely been used to quantify silicate mineral dissolution rates, which is a key process for removing carbon dioxide (▪) from the atmosphere over geological timescales. The sensitivity of silicate weathering rates to climate is disproportionately weighted towards regions with high erosion rates. This study quantifies the impact of adsorption-desorption reactions on the chemistry of three large Himalayan rivers over a period of two years, utilising both the adsorbed and dissolved phases. The concentration of riverine adsorbed cations are found to vary principally as a function of the concentration and cation exchange capacity (CEC) of the suspended sediment. Over the study period, the adsorbed phase is responsible for transporting ∼70% of the mobile (adsorbed and dissolved) barium and ∼10% of the mobile calcium and strontium. The relative partitioning of cations between the adsorbed and dissolved phases follows a systematic order in both the monsoon and the dry-season (preferentially adsorbed: Ba > Sr & Ca > Mg & K > Na). Excess mobile sodium (▪=Na-Cl) to silicon (Si) riverine ratios are found to vary systematically during an annual hydrological cycle due to the mixing of low temperature and geothermal waters. The desorption of sodium from uplifted marine sediments is one key process that may increase the Na*/Si ratios. Accounting for the desorption of sodium reduces silicate weathering rate estimates by up to 83% in the catchments. This study highlights that surficial weathering processes alone are unable to explain the chemistry of the rivers studied due to the influence of hydrothermal reactions, which may play an important role in limiting the efficiency of silicate weathering and hence modulating atmospheric ▪ concentrations over geological time.

Mechanisms controlling albite dissolution/precipitation kinetics as a function of chemical affinity: New insights from experiments in 29Si spiked solutions at 150 and 180 °C

Knowledge of the rates of dissolution of rock-forming minerals close to equilibrium and their dependence on ΔGr, the Gibbs free energy of reaction, is essential for describing the temporal and spatial evolution of many environmental and engineering processes involving solid/fluid interactions. In the present study we used the isotope-doping method to quantify albite forward and net dissolution rates. Batch experiments were performed at 150, 180 °C and pH = 9 at near equilibrium and equilibrium conditions (-25 ≤ ΔGr ≤ + 8.2 kJ/mol) in 29Si spiked solutions which were undersaturated with the secondary Al-Si solid phases likely to precipitate.The forward dissolution rates normalized to the initial BET surface area were found to decrease continuously and monotonically with increasing time and ΔGr, achieving values 1.3 to 2.4 orders of magnitude lower at chemical equilibrium than initial far from equilibrium values, with the highest rate decrease for the highest solid to fluid ratio. These rate drops were accompanied by an increase in BET specific surface areas associated with the formation of widespread dissolution features. A decrease of albite forward dissolution rate together with an increase of its BET surface area was also observed as a function of reaction time at far from equilibrium conditions (ΔGr ≤ − 65 kJ/mol). These observations are consistent with a continuous decrease with time and increasing ΔGr of albite effective surface area linked to the formation of unreactive negative crystal facets, in addition to etch pits stopping nucleating above a critical value of ΔGr. Thus, the observed decrease in albite dissolution rate as equilibrium is approached is not linked primarily to the increase in the contribution of the backward reaction but rather to the decrease of the forward reaction rate in conjunction with the decrease in the density of reactive sites at the mineral surface.The results of this study show that the characterization of the effective surface area and its evolution with reaction time and chemical affinity is crucial to deriving robust dissolution rates of well-crystallized minerals like feldspars. Dissolution experiments in 29Si spiked solutions of samples with different history and well-characterized effective surface area and surface morphology should help to better quantify the rate laws controlling silicate minerals weathering.

Muddy sediments are an important potential source of silicon in coastal and continental margin zones

The dissolution of silicate minerals on the seafloor releases an important amount of dissolved silicon (dSi), which is necessary for maintaining high diatom production in Coastal and Continental Margin Zones (CCMZs). However, the dissolution of silicate minerals along the continental shelves is variable, which hinders our understanding of the marine Si cycle on both a regional and global scale. To understand the discrepancy of silicon (Si) released in different sediment matrices and its potential controlling factors, we investigated surface sediments of typical CCMZs of the Chinese marginal Seas using a continuous alkaline extraction technique, grain size and chemical (carbon and total nitrogen) analysis as well as a qualitative measurement of clay mineral composition by X-ray diffraction. The results showed that the amount of Si and aluminum (Al) leached from muddy sediments were 2 times greater than those released from sandy sediments. High dissolution rates (> 0.20 mg-SiO2 g−1 min−1) of silicate minerals are caused by a large sediment-specific surface area. Further, our data showed that biogenic silica (bSi) with high Al content (Si:Al < 40) has low reactivity and that the source of Al incorporated in bSi is silicate minerals undergoing dissolution. We show that although the dissolution of silicate minerals is less active than that of bSi, it still potentially releases more bio-available Si and Al to seawater due to its dominant presence on the seafloor (70.3% − 99.0%wt). This study highlights silicate minerals as an important potential marine Si source and emphasizes the need for a better understanding of the roles of silicate minerals in the Si cycle of marginal seas in future studies.

Modeling Cosmogenic Nuclides in Transiently Evolving Topography and Chemically Weathering Soils

AbstractTerrestrial cosmogenic nuclides (TCN) are widely employed to infer denudation rates in mountainous landscapes. The calculation of an inferred denudation rate (Dinf) from TCN concentrations is typically performed under the assumptions that denudation rates were steady during TCN accumulation and that soil chemical weathering negligibly impacted soil mineral abundances. In many landscapes, however, denudation rates were not steady and soil composition was significantly impacted by chemical weathering, which complicates interpretation of TCN concentrations. We present a landscape evolution model that computes transient changes in topography, soil thickness, soil mineralogy, and soil TCN concentrations. We used this model to investigate TCN responses in transient landscapes by imposing idealized perturbations in tectonically (rock uplift rate) and climatically sensitive parameters (soil production efficiency, hillslope transport efficiency, and mineral dissolution rate) on initially steady‐state landscapes. These experiments revealed key insights about TCN responses in transient landscapes. (a) Accounting for soil chemical erosion is necessary to accurately calculate Dinf. (b) Responses of Dinf to tectonic perturbations differ from those to climatic perturbations, suggesting that spatial and temporal patterns in Dinf are signatures of perturbation type and magnitude. (c) If soil chemical erosion is accounted for, basin‐averaged Dinf inferred from TCN in stream sediment closely tracks actual basin‐averaged denudation rate, showing that Dinf is a reasonable proxy for actual denudation rate, even in many transient landscapes. (d) Response times of Dinf to perturbations increase with hillslope length, implying that response times should be sensitive to the climatic, biological, and lithologic processes that control hillslope length.

Dolomitisation favoured by Lewis acidic background compounds in saline fluids

Predicting the type and rate of reactions between minerals and fluids is of utmost importance in many applications. Due to the presence of background ions, natural environments are often much more complex than laboratory experimental conditions that are used to derive mineral dissolution or precipitation rates. Dolomitisation is one of the most important diagenetic processes affecting carbonate rocks. Still, its underlying mechanisms are not yet completely unraveled. Here, we test the impact of background ions in saline solutions on the dolomitisation rate. Using batch reactor experiments at 200 °C and mineralogical characterisation, we demonstrate that the presence of background ions influences the fluid starting pH and specific ion effect, both impacting the dolomitisation rate. The results indicate that ions with a stronger hydration enthalpy correlate with a shorter dolomitisation induction time, and that Lewis acid AlCl3 is more effective than Brønsted acid HCl. Importantly, dolomitisation occurred at a slightly acidic pH, and carbon speciation modelling showed that carbonate ions did not dominate in any of the experiments. Hence, dolomitisation in our experiments is faster in saline, slightly acidic rather than alkaline solutions and the rate is influenced by the solution composition, with specific ion effects influencing dolomite surface charge, interfacial tension and the structure of water. These new insights have implications for interpretations on natural environments, such as deep reservoirs with saline, slightly acidic formation water, and predictions related to geological carbon dioxide storage.

Probability distributions of mineral dissolution rates: the role of lattice defects

The correct quantification of mineral dissolution rates is a critical task for macroscopic reactive transport modeling. Previous studies showed a substantial rate variability of about two orders of magnitude, which cannot be explained by variance of external environmental parameters alone. If the rate cannot be predicted as a constant parameter, then the critical question is whether it can be predicted as a stable reproducible probability distribution. Although a large variety of factors may contribute to the overall variance across the scales, the effect of defect density and defect spatial distribution can be considered as one of the key variance sources. Here, we tested the reproducibility of probability distributions for Kossel crystals with a different amount and spatial configurations of lattice dislocations. We ran several tests on systems with the same configurations and calculated the probabilities of material flux. Surprisingly, we discovered that the density of dislocations has minimal impact on the probability distributions. However, the spatial location of dislocations has a substantial influence on the rate distributions reproducibility. In cases where multiple etch pits operate simultaneously, reproducible rate distributions are found regardless of the number of dislocations. In cases where dislocations formed clusters, one large etch pit controlled the entire surface, and sets of reproducible probability distributions were detected. Then, more complex statistical behavior is expected, since the result is path-dependent. These results have serious consequences for the implementation of rate distributions in reactive transport models. Further studies, however, are needed to provide clear guidance on relating surface morphologies, dislocation distributions, and dissolution rate variance. The role of material-specific properties, such as crystallographic structure and bonding, in rate distributions, should be additionally addressed. The role of grain boundaries, crystal size and crystal habit, including nanoparticulate forms, in rate variance, also should be addressed for practical applications.

Chemical Alteration of Riverine Particles in Seawater and Marine Sediments: Effects on Seawater Composition and Atmospheric CO2

Numerous studies have shown that riverine particles react with seawater. Reactions include dissolution of reactive silicate minerals (e.g., feldspars) and formation of authigenic clays and carbonates. Previous studies have either focused on mineral dissolution (marine silicate weathering) or authigenic phase formation (reverse weathering). A comprehensive study that assesses all processes affecting the marine alteration of riverine particle has -to our knowledge- not yet been conducted. Our contribution aims to fill this gap. We first quantify cation exchange between seawater and riverine particles that occurs when particles enter the marine realm and show that significant global cation fluxes are induced by this process (-1.3 Tmol Na yr-1, -0.2 Tmol K yr-1, -0.4 Tmol Mg yr-1, +1.2 Tmol Ca yr-1) where the positive sign indicates cation release into seawater while the negative sign denotes uptake on particles. We then use thermodynamic and kinetic modeling to investigate how much of the suspended particle load dissolves in contact with seawater and estimate corresponding global release rates for dissolved cations and silica assuming congruent dissolution (+0.06 Tmol Na yr-1, +0.15 Tmol Ca yr-1, +2.8 Tmol Si yr-1). Subsequently, we investigate rates of mineral dissolution and authigenic clay and carbonate formation in marine sediments applying reactive transport modeling, porewater data and mass balance calculations. Our best estimates for net fluxes across the sediment/water interface (dissolution–mineral formation) result as +1.5 Tmol Na yr-1, -2.5 Tmol K yr-1, -2.0 Tmol Mg yr-1, +2.5 Tmol Ca yr-1, and +1.9 Tmol Si yr-1 where most of the Na and Ca release is induced by plagioclase dissolution, K is taken up in authigenic clays and Mg is removed from solution by authigenic clay and carbonate formation. We conclude that the alkalinity of seawater is not significantly affected by marine silicate alteration since cation release fluxes (Na, Ca) are as high as cation uptake fluxes (K, Mg) on equivalent basis. Moreover, marine silicate weathering and reverse weathering are closely coupled since Al required for clay formation is mostly provided by feldspar dissolution while Al removal in authigenic clay promotes and maintains feldspar dissolution in marine sediments. Authigenic carbonate formation in anoxic subsurface sediments sequesters significant amounts of carbon (2.5 Tmol C yr-1) according to our estimates where most of the Ca and alkalinity required for carbonate formation are provided by the dissolution of Ca-bearing silicate minerals. This hidden sedimentary cycle provides a sink for dissolved inorganic carbon that may drive a slow draw-down of atmospheric CO2 on geological timescales. Marine silicate alteration has an even stronger effect on the geochemical evolution of seawater by generating large fluxes of dissolved K, Mg, Ca and Si.

Experimental determination of the reactivity of basalts as a function of their degree of alteration

The element release rates from naturally altered basalts were measured in batch experiments at 27 °C, and in mixed-flow experiments at 25 °C in reactive fluids initially consisting of pH 3 or 4 aqueous solutions. The basalts reacted in this study consist of 1) surface weathered basalts ranging in age up to 13 million years, and 2) hydrothermally altered basalts from zeolite to actinolite alteration zones (temperatures of ∼50 to 300 °C). The in situ pH in the batch experiments increased over time with the final pH of the fluids ranging from to 4 to 8. Most experiments exhibited a preferential release of Ca and Mg compared to Si from the dissolving basalts, both initially and over the long-term. This behavior is attributed to the combination of an initial rapid cation-proton exchange reaction and the relatively fast dissolution rates of Ca-bearing minerals. The BET surface area normalized Si release rates for all of the altered basalts are within one order of magnitude of each other, and from one to two orders of magnitude lower than corresponding rates from fresh basaltic glass and fresh crystalline basalts. This is interpreted to stem from 1) the fast removal of reactive basaltic glass and olivine from fresh basalts during the natural alteration of the rocks, 2) the similarity of the dissolution rates of the remaining albitic plagioclase, pyroxenes, epidote, and zeolites, and 3) the high surface areas of some less reactive secondary minerals such as clays. Overall, the results suggest that altered basalts will be effective in consuming CO2 during both natural and engineered processes, though at a somewhat slower rate than unaltered basalts.

A comprehensive and consistent mineral dissolution rate database: Part II: Secondary silicate minerals

This paper describes the creation of a consistent database of the far-from-equilibrium dissolution rates of secondary silicate minerals including clays, zeolites, serpentines, chlorites, prehnite, wollastonite, epidotes, garnets, kyanite, staurolite, cordierite, tourmaline, and feldspathoids. This work, based on the regression of available dissolution rate data normalized to their BET surface area as a function of pH and temperature, was performed using equations described in Heřmanská et al. (2022a) using a least-squares algorithm. The average difference between calculated and measured rates ranged from 0.18 to 0.66 log units depending on the mineral. Where relevant data were lacking, rate parameters are proposed based upon the rate behaviors of minerals with similar structures. All obtained rate equations and parameters have been incorporated into the KINEC.v1.dat database for direct use in geochemical fluid reactive transport software.The far-from-equilibrium dissolution rates of most naturally forming silicate minerals are notably similar to one another at neutral conditions. More than 65% of the silicate minerals considered in this study and that of Heřmanská et al. (2022a) range in value from 10-11.8 to 10-12.5 mol m-2 s-2 at 25 oC and pH 7; this range is within the uncertainties associated with these rates. This similarity in rates is attributed to the likelyhood that breaking Si-O bonds is the rate limiting step of the dissolution of each of these minerals. Faster rates are observed for minerals that can be dissolved without breaking Si-O bonds. Retrieved apparent activation energies for the silicate minerals are found to be similar over all pH conditions and average ∼55 kJ mol-1. This apparent activation energy suggests that rates at 100, 200 and 300 °C will be approximately 86, 3,600 and 42,000 times higher, respectively, than corresponding rates at 25 oC.

Study of the basic laws of dissolution of gold and copper in solutions with an ultra-low concentration of sodium cyanide

The work sets out to study the basic physicochemical dissolution patterns of gold, copper, and natural copper-containing minerals (chalcopyrite, bornite and azurite) in solutions with an ultra-low concentration of sodium cyanide (from 0.102∙10-3 to 4.08∙10-3 mol/L). The influence of various factors on the rate of dissolution of Au and Cu in solutions with ultra-low NaCN concentrations was studied by the rotating disk method; for natural copper minerals, the powder diffraction method was used. The concentration of gold and copper in solutions was determined by atomic absorption analysis. The chemical composition of the studied copper minerals was determined using the X-ray phase method, while the specific surface of the minerals was detected using a laser granulometer. The process of gold dissolution is shown to proceed in both diffusion and kinetic regions. In the diffusion region, the rate constant was 0.334∙10-6 L∙cm-2∙s-1/2∙rad-1/2; in the kinetic region – 0.919∙10-6 L∙cm-2∙s-1/2. The calculated value of the apparent activation energy for the diffusion region was 22.5 kJ/mol; for the kinetic region – 40.1 kJ/mol. The addition of glycine to a solution with an ultra-low concentration of sodium cyanide is shown to increase the specific dissolution rate of gold by 1.2 times: from 0.692∙10-9 to 0.82∙10-9 mol/cm2∙s. The process of copper dissolution is shown to take place in the diffusion r egion. The rate constant was 0.496∙ 10-6 L∙cm-2∙s-1/2∙rad-1/2 at an activation energy of 17.0 kJ/mol. With a fractional supply of sodium cyanide, the dissolution rate of copper minerals is reduced by 10–30% compared to a single load. The calculated apparent activation energy values for chalcopyrite, bornite, and azurite were 22.03, 24.2, and 24.1 kJ/mol, respectively. Thus, the use of ultra-low concentrations of NaCN in the process of cyanidation of gold and copper has a positive effect, which can be used i n the processing of gold-copper raw materials to significantly reduce the consumption of sodium cyanide.

Promotion Mechanism of Atrazine Removal from Soil Microbial Fuel Cells by Semiconductor Minerals

In recent years, soil microbial fuel cells (Soil-MFCs) have attracted attention due to their simultaneous electricity production and contaminant removal functions, but soil electron transfer resistance limits their contaminant removal effectiveness. To overcome the above-mentioned drawbacks, in this study, a dual-chamber Soil-MFC was constructed using atrazine (ATR) as the target contaminant, and the electrochemical performance of Soil-MFC and ATR removal were enhanced by semiconductor mineral addition. Analysis of atrazine was performed in soil using HPLC and GC-MS, and analysis of metallic minerals using XPS. Anodic microorganisms were determined using high-throughput sequencing technology. The results showed that the addition of Fe3O4 increased the maximum output voltage of the device by 2.56 times, and the degradation efficiency of atrazine in the soil to 63.35%, while the addition of MnO2 increased the internal resistance of the device and affected the current output, and these changes were closely related to the ion dissolution rate of the semiconductor minerals. In addition, the addition of both minerals significantly increased the relative abundance of both Proteobacteria and Bacteroidota, and Fe3O4 simultaneously promoted the significant enrichment of Firmicutes, indicating that the semiconductor minerals significantly enhanced the enrichment of electroactive microorganisms near the anode. The structural equation modeling indicated that the semiconductor minerals achieved efficient degradation of ATR in the soil through a synergistic mechanism of metal ion leaching and microbial community structure changes. The detection of ATR and its degradation products in soil revealed that the degradation of ATR mainly included: (1) hydrolysis of atrazine by microorganisms to generate dehydroxylated atrazine (HYA); (2) reduced to diethyl atrazine (DEA) and diisopropyl atrazine (DIA) by extracellular electron reduction and re-dechlorination and hydrolysis to HYA. Semiconductor minerals make an important contribution to promoting microbial activity and extracellular electron reduction processes. The results of this study strengthen the power production and ATR removal efficiency of the Soil-MFC system and provide important theoretical support for the on-site removal of organic pollutants and the sustainable application of converting biomass energy into electricity.

Experimental Investigation on Physicochemical and Wetting Characteristics of Modified Gas Coal: Effects of Multicomponent Acids and Surfactant

Abstract In this study, the effects of the different concentrations of hydrochloric acid, hydrofluoric acid, and acetic acid and a surfactant on the physicochemical characteristics of coal, such as pore diameter distribution, pore fractal dimension, and chemical structures were studied. The wettability performance of the reagent-modified coal was proposed. The results demonstrated that the mineral dissolution rate of HF in the coal sample was much higher than those by HCl and HAC treatment, which increases the surface roughness of coal. With the increase in the concentration of a multicomponent acid solution, the number of micropores decreased and the number of macropores increased. Moreover, both fractal dimensions D1 and D2 of the coal sample treated with the multicomponent acid comprising 6% HCl, 6% HF, and 6% HAC (#3) were the smallest. This shows that compound reagent #3 is available to enhance the pore size distribution with a better effect than the other five ones. Compared with the raw coal (#7), treatment with high concentrations of HCl (#4) significantly decreased the contact angle on coal (#4), whereas treatment with high concentrations of HF or HAC (#6 or #5), significantly increased it.

Experimental Study on Water-Rock Interaction Characteristics of Unconsolidated Sandstone during CO2 Multicomponent Thermal Fluid Injection

According to the reservoir characteristics and the current situation of CO2 utilization during thermal recovery in an unconsolidated sandstone heavy oil reservoir, the mechanism and law of porosity and permeability change in an unconsolidated sandstone heavy oil reservoir during CO2+steam and CO2+steam+ sodium alpha-olefin sulfonate (AOS) injection were studied by combining a static monomineral water-rock reaction and a dynamic polymineral sand pack displacement experiment. In the static water-rock reaction between CO2 and monomineral of reservoir rock, the dissolution degree of monomineral at 200°C is greater than that at 100°C and 300°C, and the order of mineral dissolution is illite, montmorillonite, kaolinite, and quartz. Besides, the dissolution rate of single rock minerals decreased significantly in the system of CO2 with AOS. In the polymineral sand pack displacement experiment, the porosity gradually decreases by CO2 multicomponent thermal fluid, and the permeability first decreases and then increases by CO2 multicomponent thermal fluid, but the permeability change is only about 0.5% by CO2+steam+ AOS, which is mainly attributed to the adsorption of AOS on the rock surface, and it is confirmed in the infrared spectrum of unconsolidated sand after displacement. This also shows that CO2+steam+AOS can stabilize the rock skeleton structure of the reservoir and prevent the deterioration of heterogeneity in the subsequent development of thermal recovery of heavy oil reservoirs; therefore, the CO2 multicomponent thermal fluid with chemical agents can improve the damage of a single CO2 thermal fluid to the reservoir.

Experiments and Simulations to Describe Alkalinity Release from Particle-Containing Oil-in-Water Emulsions and Particle Suspensions

Among the most common amendments added to groundwater during site remediation are compounds used to adjust or maintain the pH. This research describes an approach to encapsulate mineral particles (MgO and CaCO3) within oil droplets suspended within an aqueous phase for the purpose of delivery to the subsurface environment. A series of batch experiments was combined with mathematical modeling to illustrate the encapsulation and understand the influence of particle encapsulation on rates and extents of alkalinity release. The encapsulation of the alkalinity-releasing particles results in slower rates of amendment release as compared to rates obtained using suspensions of bare mineral particles, allowing for the possibility of control as a function of the pH. The results indicate that the alkalinity release from particle suspensions followed a mineral dissolution mechanism that could not explain the rate of the alkalinity release of the encapsulated particles. The reduction in mineral dissolution rates observed with the encapsulated particles was found to result from a mass transfer limitation. This limitation was well described using a linear driving force expression to account for the resistance to mass transfer at the oil–water interface.

Insights into the mechanochemical interfacial interaction between calcite and serpentine: Implications for ambient CO2 capture

Mineral carbonation of readily-available serpentine is a promising solution for massive atmospheric carbon dioxide (CO2) sequestration, in which process the most significant challenge is to overcome slow carbonation kinetics under atmospheric conditions. To enhance the mineral dissolution rate and overall carbonation efficiency, activation of serpentine is required. In this study, for the first time, a facile way to obtain activated serpentine by simply co-milling with calcite was discovered, and the as-prepared materials were applied to direct CO2 capture under atmospheric conditions. A series of analytical techniques were carried out to understand the interaction mechanism between serpentine and calcite during ball-milling process, demonstrating the occurrence of interfacial reaction with the mutual diffusion and replacement of sectional ion constituents. This robust interaction between two mineral phases endowed the minerals with superior reactivity compared to single serpentine phase, and meanwhile generated a certain amount of magnesium carbonate directly. From the confirmed cadmium precipitation as carbonate (otavite phase) from solution, methodologically, with Cd removal as quantitative index, the carbonation efficiency of co-milled materials at the molar ratio of 1:1 was about 4 times as high as that of singly-milled minerals within 2 h, indicating the tremendously enhanced CO2 capture capacity of co-milled materials. These findings about the mechanochemical interfacial reaction between calcite and serpentine may provide a novel concept and an alternative way for the activation of magnesium silicates, which can be potentially applicable to solve some tough environmental issues including CO2 sequestration.

Fracture Intensity Impacts on Reaction Front Propagation and Mineral Weathering in Three‐Dimensional Fractured Media

AbstractStudying reaction front propagation in heterogeneous natural settings is challenging, but numerical simulations can provide insight into the varying spatial and temporal scales of reaction front propagation. Here, the impact of increasing fracture intensity on mineral dissolution rates, and the extent of reaction front propagation is investigated using reactive transport simulations in upscaled discrete fracture network domains with varied fracture intensity. Domain‐averaged dissolution rates vary less than 0.5 log units regardless of the fracture intensity, but the spatial distribution of reactions is controlled by the location and number of dead‐end fractures and the number of connected flowpaths through the domain. Higher fracture intensities lead to more weathering in the domain because of more available mineral for water‐rock interactions. We find that reaction fronts propagate through the primary flowpaths in the first 10,000 years of the simulation for a 10‐m length domain, then propagate into secondary flowpaths and dead‐end fractures between 10,000 and 100,000 years, and finally into the matrix over timescales of hundreds of thousands of years. The domain‐averaged reaction rates decrease through time corresponding to a transition from dissolution in advection‐dominated, fast‐flowing pathways, to dissolution in transport‐limited zones of disconnected fractures and matrix. Matrix dissolution, or dissolution under transport‐limited conditions, is the dominant process at late times in these simulations. The results of these simulations recreate the observed paradox found in nature where highly fractured hillslopes tend to be more weathered but have slower weathering rates, while hillslopes with fewer fractures, are less weathered but have higher dissolution rates.

The circular nutrient economy of terrestrial ecosystems and the consequences for rock weathering

Earth’s biosphere is thought to exert a substantial influence on regolith evolution and chemical weathering rates. However, ecosystems are also highly efficient at retaining and recycling nutrients. Thus, when the ecological demand for rock-derived nutrients (e.g., P, Ca, K) exceeds the rates of regolith supply, ecological retention and recycling strategies can minimize nutrient limitations. To evaluate the balance between nutrient recycling and new nutrient input, we combined a plant model that drives growth according to foliar P levels with a weathering model that includes regolith rejuvenation via erosion and export via chemical weathering according to water flow, regolith thickness, mineral dissolution rates, secondary minerals, and nutrient storage in organic and mineral phases. We find that plant growth is strongly dependent on the total regolith nutrient inventory, resulting in a strong correlation between plant productivity and erosion. Increased water export or decreased regolith thickness diminish the total inventory of nutrient corresponding to lower rates of recycling and lower plant growth. In contrast, purported biogenic drivers of weathering, such as enhanced mineral dissolution, only support higher growth rates at high erosion rates. At erosion rates typical of the global land surface, more rapid mineral dissolution combined with enhanced formation of secondary minerals, depletes the inventory of mineral P, resulting in no benefit for plant growth. We also find that the increased chemical weathering export does not scale directly with plant growth. For example, accelerated mineral weathering does increase chemical weathering export but not potential plant growth. Conversely, thicker regolith is associated with a small increase in weathering export, but a large increase in potential plant growth. Collectively, when plant growth is coupled to regolith weathering our calculations suggest that plant productivity is not directly correlated with silicate weathering fluxes, and that biotic drivers of silicate weathering may only be effective at high erosion rates not typical at the Earth’s surface.