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Nanoconfinement facilitates reactions of carbon dioxide in supercritical water.

ABSTRACT: The reactions of CO₂ in water under extreme pressure-temperature conditions are of great importance to the carbon storage and transport below Earth's surface, which substantially affect the carbon budget in the atmosphere. Previous studies focus on the CO₂(aq) solutions in the bulk phase, but underground aqueous solutions are often confined to the nanoscale, and nanoconfinement and solid-liquid interfaces may substantially affect chemical speciation and reaction mechanisms, which are poorly known on the molecular scale. Here, we apply extensive ab initio molecular dynamics simulations to study aqueous carbon solutions nanoconfined by graphene and stishovite (SiO₂) at 10 GPa and 1000 ~ 1400 K. We find that CO₂(aq) reacts more in nanoconfinement than in bulk. The stishovite-water interface makes the solutions more acidic, which shifts the chemical equilibria, and the interface chemistry also significantly affects the reaction mechanisms. Our findings suggest that CO₂(aq) in deep Earth is more active than previously thought, and confining CO₂ and water in nanopores may enhance the efficiency of mineral carbonation.

SUBMITTER: Stolte N

PROVIDER: S-EPMC9547913 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

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Nanoconfinement facilitates reactions of carbon dioxide in supercritical water.

Stolte Nore N Hou Rui R Pan Ding D

Nature communications 20221008 1

The reactions of CO<sub>2</sub> in water under extreme pressure-temperature conditions are of great importance to the carbon storage and transport below Earth's surface, which substantially affect the carbon budget in the atmosphere. Previous studies focus on the CO<sub>2</sub>(aq) solutions in the bulk phase, but underground aqueous solutions are often confined to the nanoscale, and nanoconfinement and solid-liquid interfaces may substantially affect chemical speciation and reaction mechanisms, ...[more]

PMID: 36209274

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Project description:Mutual diffusion of six hydrocarbons (methane, ethane, isobutane, benzene, toluene or naphthalene) diluted in supercritical carbon dioxide ([Formula: see text]) is studied by molecular dynamics simulation near the Widom line, i.e., in the temperature range from 290 to 345 K along the isobar 9 MPa. The [Formula: see text] + aromatics mixtures are additionally sampled at 10 and 12 MPa and an experimental database with Fick diffusion coefficient data for those systems is provided. Taylor dispersion experiments of [Formula: see text] with benzene, toluene, n-dodecane and 1,2,3,4-tetrahydronaphthalene are conducted along the [Formula: see text] 10 MPa isobar. Maxwell-Stefan and Fick diffusion coefficients are analyzed, together with the thermodynamic factor that relates them. It is found that the peculiar behavior of the Fick diffusion coefficient of some [Formula: see text] mixtures in the extended critical region is a consequence of the thermodynamic factor minimum due to pronounced clustering on the molecular scale. Further, the strong dependence of the Fick diffusion coefficient on the molecular mass of the solute as well as the breakdown of the Stokes-Einstein relation near the Widom line are confirmed. Eleven correlations for the prediction of the Fick diffusion coefficient of [Formula: see text] mixtures are assessed. An alternative two-step approach for the prediction of the infinite dilution Fick diffusion coefficient of supercritical [Formula: see text] mixtures is proposed. It requires only the state point in terms of temperature and pressure (or density) as well as the molecular solute mass as input parameters. First, entropy scaling is applied to estimate the self-diffusion coefficient of [Formula: see text]. Subsequently, this coefficient is used to determine the infinite dilution Fick diffusion coefficient of the mixture, based on the finding that these two diffusion coefficients exhibit a linear relationship, where the slope depends only on the molecular solute mass.

Dataset Information

Nanoconfinement facilitates reactions of carbon dioxide in supercritical water.

Publications

Nanoconfinement facilitates reactions of carbon dioxide in supercritical water.

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