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Growth of and contaminant incorporation in complex carbonate coatings at mineral/water interfaces

EMSL Project ID


All realistic mineral surfaces in natural waters can be expected to be coated, and their reactive properties influenced by the presence of coatings. It is a common but challenging interfacial process to understand because the nature of the coatings is a complex function of solution conditions, solubility, and interfacial structure, and because of difficulties in detecting and probing thin, often structurally and/or chemically similar minerals on minerals. The long-term vision of this research is therefore to provide fundamental insights into and quantitative understanding of mineral coatings and the mineral/fluid interfacial properties that emerge as they form. In particular, this research will determine the ability of mineral coatings to incorporate contaminants.

Due to their broad relevance to biogeochemical, environmental, and energy-related systems, metal carbonates will be used as a model system to quantify the effects of several thermodynamic and kinetic controlling factors (structural mismatch, solubility of competing phases, and dynamics of water exchange). A combination of state-of-the-art experimental capabilities and molecular simulations will be deployed to overcome current limitations and yield fundamental insights. Atomic force microscopy and high-resolution transmission electron microscopy will be employed to characterize the structure of mineral coatings from the atomic to the micron scale and will provide both lateral and cross-sectional views. X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy will be used to determine the depth-dependent composition of the mineral coatings with and without contaminants present. Inductively coupled plasma mass spectrometry will serve to quantify the solution chemistry. In addition, an atomistic model of heteroepitaxial carbonate films will be constructed to help interpret and rationalize experimental observations and, once validated, predict the energetics of contaminant incorporation.

Project Details

Project type
Large-Scale EMSL Research
Start Date
End Date


Principal Investigator

Sebastien Kerisit
Pacific Northwest National Laboratory

Team Members

Xiaonan Lu
Pacific Northwest National Laboratory

Sebastian Mergelsberg
Pacific Northwest National Laboratory

Amreen Jan
CEA Marcoule

Micah Prange
Pacific Northwest National Laboratory

Shawn Riechers
Pacific Northwest National Laboratory

Eugene Ilton
Pacific Northwest National Laboratory

Odeta Qafoku
Environmental Molecular Sciences Laboratory

Related Publications

Jan A., J. Delaye, S. Gin, and S.N. Kerisit. 2019. "Molecular dynamics simulation of ballistic effects in simplified nuclear waste glasses." Journal of Non-crystalline Solids 505. PNNL-SA-138390. doi:10.1016/j.jnoncrysol.2018.11.021
Jan A., J. Delaye, S. Gin, and S.N. Kerisit. 2019. "Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses." Journal of Non-crystalline Solids 519. PNNL-SA-140805. doi:10.1016/j.jnoncrysol.2019.05.025
Kerisit S.N., F.N. Smith, M.E. Hoover, S.A. Saslow, and N. Qafoku. 2018. "Incorporation Modes of Iodate in Calcite." Journal of Environmental Science and Technology 52, no. 10:5902-5910. PNNL-SA-129924. doi:10.1021/acs.est.8b00339
Kerisit S.N., J. Du, and J. Du. 2019. "Monte Carlo Simulation of Borosilicate Glass Dissolution using Molecular Dynamics-Generated Glass Structures." Journal of Non-crystalline Solids 522. PNNL-SA-143886. doi:10.1016/j.jnoncrysol.2019.119601
Ling F.T., J.E. Post, P.J. Heaney, and E.S. Ilton. 2018. "The relationship between Mn oxidation state and structure in triclinic and hexagonal birnessites." Chemical Geology 479. PNNL-SA-135583. doi:10.1016/j.chemgeo.2018.01.011
Riechers SL, and SN Kerisit. 2018. "Anisotropic Growth of Otavite on Calcite: Implications for Heteroepitaxial Growth Mechanisms." Crystal Growth & Design 18(1):159-170. doi:10.1021/acs.cgd.7b01055
Saslow S.A., S.N. Kerisit, T. Varga, K.C. Johnson, N.M. Avalos, A.R. Lawter, and N. Qafoku. 2019. "Chromate Effect on Iodate Incorporation into Calcite." Environmental Science & Technology Letters 3, no. 8:1624-1630. PNNL-SA-141592. doi:10.1021/acsearthspacechem.9b00047