Structures of multinuclear U(<scp>vi</scp>) species on the hydroxylated α-SiO<sub>2</sub>(001) surface: insights from DFT calculations

Gao, Pengyuan; Jin, Qiang; Chen, Zongyuan; Wang, Dongqi; Tournassat, Christophe; Guo, Zhijun

doi:10.1039/d3cp04941h

Phys. Chem. Chem. Phys.

2024

DOI: 10.1039/d3cp04941h

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Structures of multinuclear U(vi) species on the hydroxylated α-SiO₂(001) surface: insights from DFT calculations

Pengyuan Gao,

Qiang Jin,

Zongyuan Chen

et al.

Abstract: Multinuclear U(VI) species may be dominant in the aqueous solutions under environmental conditions, while the structures of the multinuclear U(VI) species on mineral surfaces remain unclear. This work reports the...

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Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

Gao,

Liu,

Guo

et al. 2024

Environ. Sci. Technol.

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Among all natural submicrosized phases, clay minerals are ubiquitous in soils and sedimentary rocks in nature as well as in engineered environments, and while clay minerals' adsorption properties have been studied extensively, their unique level of surface reactivity heterogeneities necessitates further investigation at the molecular level to understand and predict the influence of these heterogeneities on their macroscopic properties. In this study, we investigated the surface structures and desorption-free energies of U(VI) species (UO 2 2+ ) and As(V) species (H 2 AsO 4 − and HAsO 4 2−) complexed at different edge surface reactive sites of a cis-vacant montmorillonite layer using first-principles molecular dynamics (FPMD). We show that U(VI) forms bidentate and tridentate complexes on montmorillonite edge surfaces, whereas As(V) monodentate complexes are the most stable. Then, we constrained a state-of-the-art surface complexation model (SCM) with surface acid−base chemistry and surface complexation properties obtained from the molecular-level simulation results. While our results highlighted the complexity of the interfacial chemistry controlling the complexation of inorganic contaminants on clay mineral surfaces, they also evidenced the reliability of an integrated workflow using modern multiscale simulation techniques to address the challenge of predicting heterogeneities in mineral surface reactivity.

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Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

Gao,

Liu,

Guo

et al. 2024

Environ. Sci. Technol.

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scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.

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Structures of multinuclear U(vi) species on the hydroxylated α-SiO₂(001) surface: insights from DFT calculations

Abstract: Multinuclear U(VI) species may be dominant in the aqueous solutions under environmental conditions, while the structures of the multinuclear U(VI) species on mineral surfaces remain unclear. This work reports the...

Cited by 1 publication

References 66 publications

Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

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Structures of multinuclear U(vi) species on the hydroxylated α-SiO2(001) surface: insights from DFT calculations

Abstract: Multinuclear U(VI) species may be dominant in the aqueous solutions under environmental conditions, while the structures of the multinuclear U(VI) species on mineral surfaces remain unclear. This work reports the...

Cited by 1 publication

References 66 publications

Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals

Contact Info

Product

Resources

About

Structures of multinuclear U(vi) species on the hydroxylated α-SiO₂(001) surface: insights from DFT calculations