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Key Objectives: Use microfluidics as a tool to investigate coupled dissolution-precipitation processes in fractures that flow; Identify key parameters that control optimal carbonation conditions (spatially and quantitatively) that can help guide larger scale field tests.
Warming temperatures in continuous permafrost zones of the Arctic will alter both hydrological and geochemical soil conditions, which are strongly linked with heterotrophic microbial carbon (C) cycling. Heterogeneous permafrost landscapes are often dominated by polygonal features formed by expanding ice wedges: water accumulates in low centered polygons (LCPs), and water drains outward to surrounding troughs in high centered polygons (HCPs). These geospatial differences in hydrology cause gradients in biogeochemistry, soil C storage potential, and thermal properties. Presently, data quantifying carbon dioxide (CO 2 ) and methane (CH 4 ) release from HCP soils are needed to support modeling and evaluation of warming-induced CO 2 and CH 4 fluxes from tundra soils. This study quantifies the distribution of microbial CO 2 and CH 4 release in HCPs over a range of temperatures and draws comparisons to previous LCP studies. Arctic tundra soils were initially characterized for geochemical and hydraulic properties. Laboratory incubations at −2, +4, and +8°C were used to quantify temporal trends in CO 2 and CH 4 production from homogenized active layer organic and mineral soils in HCP centers and troughs, and methanogen abundance was estimated from mcrA gene measurements. Results showed that soil water availability, organic C, and redox conditions influence temporal dynamics and magnitude of gas production from HCP active layer soils during warming. At early incubation times (2–9 days), higher CO 2 emissions were observed from HCP trough soils than from HCP center soils, but increased CO 2 production occurred in center soils at later times (>20 days). HCP center soils did not support methanogenesis, but CH 4 -producing trough soils did indicate methanogen presence. Consistent with previous LCP studies, HCP organic soils showed increased CO 2 and CH 4 production with elevated water content, but HCP trough mineral soils produced more CH 4 than LCP mineral soils. HCP mineral soils also released substantial CO 2 but did not show a strong trend in CO 2 and CH 4 release with water content. Knowledge of temporal and spatial variability in microbial C mineralization rates of Arctic soils in response to warming are key to constraining uncertainties in predictive climate models.
Increasing CO 2 emission has resulted in pressing climate and environmental issues. While abiotic and biotic processes mediating the fate of CO 2 have been studied separately, their interactions and combined effects have been poorly understood. To explore this knowledge gap, an iron-reducing organism, Orenia metallireducens, was cultured under 18 conditions that systematically varied in headspace CO 2 concentrations, ferric oxide loading, and dolomite (CaMg(CO 3 ) 2 ) availability. The results showed that abiotic and biotic processes interactively mediate CO 2 acidification and sequestration through "chain reactions", with pH being the dominant variable. Specifically, dolomite alleviated CO 2 stress on microbial activity, possibly via pH control that transforms the inhibitory CO 2 to the more benign bicarbonate species. The microbial iron reduction further impacted pH via the competition between proton (H + ) consumption during iron reduction and H + generation from oxidization of the organic substrate. Under Fe(III)-rich conditions, microbial iron reduction increased pH, driving dissolved CO 2 to form bicarbonate. Spectroscopic and microscopic analyses showed enhanced formation of siderite (FeCO 3 ) under elevated CO 2 , supporting its incorporation into solids. In conclusion, the results of these CO 2 -microbe-mineral experiments provide insights into the synergistic abiotic and biotic processes that alleviate CO 2 acidification and favor its sequestration, which can be instructive for practical applications (e.g., acidification remediation, CO 2 sequestration, and modeling of carbon flux).
U-Pb carbonate geochronology can directly constrain the timing and rates of important geological processes. However, the mechanisms and controls on U incorporation, distribution, and retention in carbonate minerals remain unclear, limiting geological interpretations. Here X-ray absorption spectroscopy (µXAS) and in-situ U-Pb carbonate geochronology are combined to temporally track U distribution and redox state in a porphyry-epithermal system. In this setting, multiple generations of carbonate minerals record fluid conditions and processes which control the solubility and deposition of metals, including U. This novel approach provides the first evidence of both oxidized UO 2 2+ and reduced U 4+ species in temporally distinct generations of carbonate within a single sample. Preservation of two different U oxidation states during discrete precipitation events requires U retentivity within older domains, demonstrating that the U-Pb carbonate geochronometer is robust under hydrothermal conditions. Furthermore, crystal zones with abundant fluid/vapour inclusions linked to boiling processes coincide with relatively high levels of U and favourable U/Pb. Targeting carbonate domains with these textures may therefore increase success in U-Pb geochronology. U-Pb carbonate dating combined with µXAS can track the temporal evolution of processes critical for metal deposition in long-lived and multistage hydrothermal-magmatic ore deposit settings.
Abstract not provided
The dynamics and reactivity of nanoconfined fluids play critical roles across a wide range of environmental and technological systems, though reaction mechanisms and kinetics are not well understood. Here, the carbonation kinetics of forsterite (Mg 2 SiO 4 ) exposed to 90 atm supercritical carbon dioxide at 35–65 °C and 85–100% relative humidity (RH) was monitored with in situ X-ray diffraction, and partner molecular dynamics simulations were used to describe the free energy landscape of Mg 2+ adsorption and diffusion on forsterite surfaces covered in water films 3–10 monolayers thick. The collective findings reveal how decreasing the water film thickness by ~1.4 monolayers, from ~0.92 to ~0.64 nm, inhibited reaction rates by up to 97%, promoted anhydrous Mg-carbonate (magnesite, MgCO 3 ) precipitation, and more than doubled the apparent activation energy of carbonation. The transport simulations suggest that four monolayers are required to enable sufficiently facile Mg 2+ diffusion, helping explain previously observed water film thickness-dependent reactivity thresholds.
Goal: Gain a fundamental understanding of how fracture characteristics impact mineralization in a stagnant (dead-end) fracture.
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Explore the source record for details and available documents.
Explore the source record for details and available documents.
For presentation at ACS Fall 2023, San Francisco, CA, August 13-17, 2023.
Abstract This study examines the potential of Midcontinent Rift rocks to facilitate long‐term CO 2 sequestration by providing the necessary Ca and Mg for carbonate mineralization. Surface samples were collected from the Oronto and Bayfield‐Jacobsville Groups around Lake Superior and used for petrography and X‐ray diffraction to determine their mineral composition. Also, X‐ray fluorescence was also used to assess their bulk chemical composition. The samples were then exposed to CO 2 and deionized water in Teflon‐lined vessels at 90°C, and the resulting leachate fluids were analyzed for the cation released during the testing. SEM microscopy was used to examine the samples for potential mineralization of carbonate minerals. The Oronto Group sediments consist primarily of feldspathic to feldspathic lithic arenites with a chlorite‐dominated matrix, and the primary porosity is blocked by calcite and hematite cement. The Bayfield–Jacobsville sequences are porous quartz arenites to feldspathic quartz arenites that do not contain significant accumulation of Ca‐, Mg‐, and Fe‐bearing minerals. The leachate fluids obtained from Oronto Group samples exhibit a maximum Ca release rate (5.2 × 10 −4 mole/cm 2 .day), indicating rapid calcite cement dissolution and increased porosity and permeability. SEM/EDS microanalysis revealed areas where pore‐filling calcite was preferentially dissolved. Longer‐term rock‐water reactions resulted in induced carbonate mineralization, as evidenced by calcite crystals observed in a sample reacted for 102 days. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
Sequestration of CO 2 within stable mineral carbonates (e.g., CaCO 3 ) represents an attractive emission reduction strategy because it offers a leakage-free alternative to geological storage of CO 2 in an environmentally benign form. However, the pH of aqueous streams equilibrated with gaseous streams containing CO 2 (pH < 4) are typically lower than that which is required for carbonate precipitation (pH > 8). Traditionally, alkalinity is provided by a stoichiometric reagent (e.g., NaOH) which renders these processes environmentally hazardous and economically unfeasible. This work investigates the use of regenerable ion-exchange materials to induce alkalinity in CO 2 -saturated aqueous solutions such that the pH shift required for mineralization occurs without the need for stoichiometric reagents. Na + -H + exchange isotherms (at [H + ] = 10 −8 –10 −1 M) and rates were measured for 13X and 4A zeolites and TP-207 and TP-260 organic exchange resins in batch equilibrium and fixed-bed exchange experiments, respectively. At solutions equilibrated with CO 2 at 1.0 atm (pH = 3.9), H + exchange capacities for the materials were similar (1.7–2.4 mmol H + /g material) and resulted in pH increases from 3.9 to greater than 8.0. Multi-component mixtures using Ca 2+ and Mg 2+ cations (at 10 −3 –10 −1 M) in CO 2 -saturated water were used to probe competitive ion exchange. The presence of divalent cations in solution inhibited H + exchange, reducing capacities to as low as 0.2 mmol H + /g for both resins and zeolites. Dynamic H + exchange capacities in fixed-bed ion exchange columns were similar to equilibrium values for resins (∼1.5 mmol/g) and zeolites (∼0.8 mmol/g) using inlet solutions that were equilibrated with gaseous streams of CO 2 at 1.0 atm. However, exchange kinetics were limited by intraparticle diffusion as indicated by the increased rate parameters with increasing inlet flow rates (20–160 cm 3 min −1 ). Experimental calcite precipitation from mixing the alkaline CO 3 2− -rich water solution obtained from the ion-exchange column with a simulated liquid waste stream solution achieved thermodynamic maximum yields. The results from these studies indicate that ion exchange processes can be used as an alternative to the addition of stoichiometric bases to induce alkalinity for the precipitation of CaCO 3 , thereby opening a pathway toward sustainable and economic mineralization processes.
Mafic and ultramafic rocks present an intriguing pathway for CO 2 capture through strategic enhancements to the natural silicate weathering cycle. Simultaneously, these rock types are often hosts to appreciable amounts of metals critical to U.S. energy independence, particularly in the context of alkaline mine tailings from historical metal mining. The research and scientific prerogative, then, is to identify promising mafic and ultramafic feedstocks and conduct exploratory studies to effectively recover these critical minerals while preserving the potential for mineral carbonation. The Keweenaw Peninsula of Michigan hosts the largest native Cu reservoir within basalt in the world and experienced a rich history of Cu production spanning from pre-historic times to the mid-1900s. Today, much of the Cu mining legacy remains as mine waste tailings. In this study, we examined the Cu extractability from Keweenaw Basalt tailings using a sodium glycinate solution, in comparison with acid and sodium hydroxide leaching. Experimental results showed an 85 % Cu extraction rate using sodium glycinate as the extraction solution with negligible release of other cations from the basalt. The kinetic and extraction mechanisms of Cu selective recovery using glycinate solution were discussed using time-resolved experimental data and kinetic geochemical modeling. Theoretical estimation of carbon mineralization potential of all the existing basalt waste tailings (∼500 million tons) can reach 85.5 MMT CO 2 . A total of 0.786 MMT Cu can be recovered with sodium glycinate, with a value of 7.7 billion USD. In conclusion, this novel application of alkaline glycinate for selective Cu recovery from basalt mine tailings demonstrates the viability of selective metal recovery using a non-hazardous chemical while preserving CO 2 capture potential and presents a potential pathway toward reducing energy-related emissions and providing an unconventional domestic source of critical minerals.