Structure and dynamics of water on the forsterite surface

Liu, Tingting; Gautam, Siddharth; Wang, Hsiu-Wen; Anovitz, Lawrence M.; Mamontov, Eugene; Allard, Lawrence F.; Cole, David R.

doi:10.1039/c8cp05075a

Cited by 12 publications

(14 citation statements)

References 30 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Transmission and scanning electron microscopy images (TEM and SEM) of the synthetic nano-forsterite are provided in Section I of the Supporting Information. This material is consistent with that used in our previous work . As shown by Liu et al, the XRD pattern suggests that the dominant crystal face for this nano-forsterite is (010) due to the preferred orientation of the nanoparticles, coupled with the flaky shape of the particles observed in the SEM and TEM images (Figures S1 and S2 in the Supporting Information).…”

Section: Methodssupporting

confidence: 90%

“…14,50,51 As will be shown below, this approach provided a reasonable match between the simulation and experimental results, as was obtained in our previous study on water dynamics on the forsterite (010) surface between MD simulation and QENS experiments. 18 The simulation box in this study was composed of a forsterite (Pbnm space group, a = 4.753 Å, b = 10.199 Å, c = 5.981 Å, based on the experimental unit cell determined by ref 58) slab with the unit cell replicated 6 × 1.5 × 6 times. The length of the simulation box was 100 Å.…”

Section: ■ MD Simulationsmentioning

confidence: 99%

“…The charges for the Ow and Hw atoms were −0.8476e and +0.4238e, respectively. The harmonic oscillating mode follows the SPC water model described in Berendsen et al 71 A summary of the interatomic potentials 18 is listed in Table S1 in the Supporting Information.…”

Section: ■ MD Simulationsmentioning

confidence: 99%

“…Thus, at higher water coverage, H x CO 3 (2−x)formation occurs within the water films without direct reaction with the forsterite surface. 17 In our previous work, 18 we performed an MD simulation to illustrate the stochastic dynamics of water on the forsterite (010) surface and correlated the results with data from quasi-elastic neutron scattering (QENS) experiments. We found that the water structure on the hydroxylated surface is composed of three distinct layers, transitioning from a well-ordered and nearly immobile layer closest to the surface to less structured layers at greater distances.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Significant effort has also gone into modeling the interface of olivine with H 2 O/CO 2 fluids. , For example, Kerisit et al carried out a molecular dynamics (MD) simulation of the interface between the (010) and (011) surfaces of forsterite and supercritical (sc) CO 2 /H 2 O to track CO 2 sequestration via carbonation . They found that H 2 O displaced CO 2 on the forsterite surface and that CO 2 could only directly contact the surface if less than two monolayers of water were present.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces

Liu

Gautam

Daemen

et al. 2020

ACS Earth Space Chem.

Self Cite

View full text Add to dashboard Cite

The dynamics of water on or in a mineral substrate plays an important role in interfacial processes. This is because the structure and dynamics of interfacial water deviate from those of bulk water due to the change of interactions between surface water molecules and the interactions between the surface water and the substrate. This work presents a study of the vibrational behavior of water on a forsterite (Mg- end member of olivine) surface using inelastic neutron scattering (INS) and molecular dynamics (MD) simulations as complementary tools. The synthetic nano-forsterite used (dominated by the (010) crystal face), i.e., “dry” sample, inherently has a partial hydration/hydroxylation layer on the surface, as shown by previous studies and TGA. In the INS experiments, three water loadings (0.5, 1, and 2 monolayers) were added to the nano-forsterite surfaces. For samples with lower water loadings, i.e., dry and 0.5 monolayers, the INS spectra exhibited a red shift (lower frequency) of the water libration band and strengthening (blue shift, higher frequency) of the O–H stretching modes, implying weakening of the hydrogen bonding acting on the water molecules. In the simulations, we modeled the forsterite (010) surface and titrated it with two water loadings representing the lower and higher experimental water loadings. The lower loading in the simulation is equivalent to the dry and 0.5 monolayer samples in the experiment, thus suggesting weak hydrogen bonding between water molecules. The higher-loading simulation emulates the multilayer adsorption experiment. This produced a more significant shift of the vibrational bands, implying increased hydrogen-bonding strength and disorder between water molecules. The MD simulations complement the INS study by providing a detailed interfacial structure, and the combination of the two approaches provides a fundamental understanding of how the presence of the olivine surface impacts the vibrational behavior of water under different degrees of hydrationa phenomenon widely associated with terrestrial and extraterrestrial surfaces and near-surface processes.

show abstract

Section: Methodssupporting

confidence: 90%

Section: ■ MD Simulationsmentioning

confidence: 99%

Section: ■ MD Simulationsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces

Liu

Gautam

Daemen

et al. 2020

ACS Earth Space Chem.

Self Cite

View full text Add to dashboard Cite

show abstract

Neutron Scattering Studies of Heterogeneous Catalysis

Yu,

Cheng,

et al. 2023

Chem. Rev.

Self Cite

View full text Add to dashboard Cite

show abstract

Thin Water Films Enable Low-Temperature Magnesite Growth Under Conditions Relevant to Geologic Carbon Sequestration

Kerisit

Mergelsberg

Thompson

et al. 2021

Environ. Sci. Technol.

View full text Add to dashboard Cite

Injecting supercritical CO2 (scCO2) into basalt formations for long-term storage is a promising strategy for mitigating CO2 emissions. Mineral carbonation can result in permanent entrapment of CO2; however, carbonation kinetics in thin H2O films in humidified scCO2 is not well understood. We investigated forsterite (Mg2SiO4) carbonation to magnesite (MgCO3) via amorphous magnesium carbonate (AMC; MgCO3·xH2O, 0.5 < x < 1), with the goal to establish the fundamental controls on magnesite growth rates at low H2O activity and temperature. Experiments were conducted at 25, 40, and 50 °C in 90 bar CO2 with a H2O film thickness on forsterite that averaged 1.78 ± 0.05 monolayers. In situ infrared spectroscopy was used to monitor forsterite dissolution and the growth of AMC, magnesite, and amorphous SiO2 as a function of time. Geochemical kinetic modeling showed that magnesite was supersaturated by 2 to 3 orders of magnitude and grew according to a zero-order rate law. The results indicate that the main drivers for magnesite growth are sustained high supersaturation coupled with low H2O activity, a combination of thermodynamic conditions not attainable in bulk aqueous solution. This improved understanding of reaction kinetics can inform subsurface reactive transport models for better predictions of CO2 fate and transport.

show abstract

Structure and dynamics of water on the forsterite surface

Abstract: A combination of QENS experiments and MD simulations quantifies the structure and dynamics of water on the olivine surface.

Cited by 12 publications

References 30 publications

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces

Neutron Scattering Studies of Heterogeneous Catalysis

Thin Water Films Enable Low-Temperature Magnesite Growth Under Conditions Relevant to Geologic Carbon Sequestration

Contact Info

Product

Resources

About

Structure and dynamics of water on the forsterite surface

Abstract: A combination of QENS experiments and MD simulations quantifies the structure and dynamics of water on the olivine surface.

Cited by 12 publications

References 30 publications

Vibrational Behavior of Water Adsorbed on Forsterite (Mg2SiO4) Surfaces

Vibrational Behavior of Water Adsorbed on Forsterite (Mg2SiO4) Surfaces

Neutron Scattering Studies of Heterogeneous Catalysis

Thin Water Films Enable Low-Temperature Magnesite Growth Under Conditions Relevant to Geologic Carbon Sequestration

Contact Info

Product

Resources

About

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces

Vibrational Behavior of Water Adsorbed on Forsterite (Mg₂SiO₄) Surfaces