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Title: Weakly bound water structure, bond valence saturation and water dynamics at the goethite (100) surface/aqueous interface: ab initio dynamical simulations

Journal Article · · Geochemical Transactions
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Many important geochemical and biogeochemical reactions occur in the mineral/formation water interface of the highly abundant mineral, goethite [alpha-Fe(OOH)]. Ab initio molecular dynamics (AIMD) simulations of the goethite alpha-FeOOH (100) surface and the structure, water bond formation and dynamics of water molecules in the mineral/aqueous interface are presented. Several exchange correlation functionals were employed (PBE96, PBE96 + Grimme, and PBE0) in the simulations of a (3 x 2) goethite surface with 65 absorbed water molecules in a 3D-periodic supercell (a = 30 angstrom, FeOOH slab similar to 12 angstrom thick, solvation layer similar to 18 angstrom thick).

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC06-76RLO 1830; AC05-76RL01830; AC06-76RL01830
OSTI ID:
1619403
Alternate ID(s):
OSTI ID: 1353314; OSTI ID: 1367658
Report Number(s):
PNNL-SA-123047; 3; PII: 40
Journal Information:
Geochemical Transactions, Journal Name: Geochemical Transactions Vol. 18 Journal Issue: 1; ISSN 1467-4866
Publisher:
Springer Science + Business MediaCopyright Statement
Country of Publication:
United Kingdom
Language:
English
Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

References (60)

Effects of Phosphate on Uranium(VI) Adsorption to Goethite-Coated Sand journal November 2004
Mössbauer spectroscopy on Mars: goethite in the Columbia Hills at Gusev crater journal November 2005
Molecular statics calculations of proton binding to goethite surfaces: A new approach to estimation of stability constants for multisite surface complexation models journal May 1996
Periodic density functional theory calculations of bulk and the (010) surface of goethite journal May 2008
Mineral–water interfacial structures revealed by synchrotron X-ray scattering journal January 2004
The Principles Determining the Structure of Complex Ionic Crystals journal April 1929
The inorganic crystal structure data base journal May 1983
Theoretical Study of Properties of Goethite (α-FeOOH) at Ambient and High-Pressure Conditions journal March 2012
Arsenic Adsorption onto Minerals: Connecting Experimental Observations with Density Functional Theory Calculations journal March 2014
Second-harmonic generation and theoretical studies of protonation at the water/α-TiO2 (110) interface journal August 2005
Water Structure and Hydrogen Bonding at Goethite/Water Interfaces: Implications for Proton Affinities journal February 2012
Recent Developments in the Methods and Applications of the Bond Valence Model journal December 2009
Norm-Conserving Pseudopotentials journal November 1979
First Principles Simulation of the Bonding, Vibrational, and Electronic Properties of the Hydration Shells of the High-Spin Fe 3+ Ion in Aqueous Solutions journal February 2010
Nanominerals, Mineral Nanoparticles, and Earth Systems journal March 2008
Large-Scale Plane-Wave-Based Density Functional Theory: Formalism, Parallelization, and Applications book July 2011
Infrared study of surface hydroxyl groups on goethite
  • Rochester, Colin H.; Topham, Susan A.
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 75, Issue 0 https://doi.org/10.1039/f19797500591
journal January 1979
Molecular Dynamics Simulations of the Goethite-water Interface journal January 2003
Arsenate and Chromate Retention Mechanisms on Goethite. 1. Surface Structure journal February 1997
Uranium(VI) Adsorption on Goethite and Soil in Carbonate Solutions journal September 1996
Structures and energies of AlOOH and FeOOH polymorphs from plane wave pseudopotential calculations journal March 2001
Unified Approach for Molecular Dynamics and Density-Functional Theory journal November 1985
NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations journal September 2010
A First-Principles Molecular Dynamics Study of Calcium in Water journal September 2005
A unified formulation of the constant temperature molecular dynamics methods journal July 1984
Hydration Shell Structure and Dynamics of Curium(III) in Aqueous Solution: First Principles and Empirical Studies journal May 2011
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
The adsorption and dissociation of water molecule on goethite (010) surface: A DFT approach journal January 2017
Bond-valence parameters obtained from a systematic analysis of the Inorganic Crystal Structure Database journal August 1985
Variability in goethite surface site density: evidence from proton and carbonate sorption journal December 2003
Efficient pseudopotentials for plane-wave calculations journal January 1991
Nanogoethite is the dominant reactive oxyhydroxide phase in lake and marine sediments journal January 2003
Benzenecarboxylate Surface Complexation at the Goethite (α-FeOOH)/Water Interface:  I. A Mechanistic Description of Pyromellitate Surface Complexes from the Combined Evidence of Infrared Spectroscopy, Potentiometry, Adsorption Data, and Surface Complexation Modeling journal June 2000
The mechanism of cadmium surface complexation on iron oxyhydroxide minerals journal October 1999
Ligand Substitution Reactions at Inorganic Centers † journal June 2005
Effects of pH and ionic strength on the adsorption of phosphate and arsenate at the goethite–water interface journal May 2005
Water structure at hematite–water interfaces journal April 2011
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] journal February 1997
Molecular Dynamics Simulations of Electrolyte Solutions at the (100) Goethite Surface journal October 2006
A Surface Structural Approach to Ion Adsorption: The Charge Distribution (CD) Model journal May 1996
Structure and dynamics of the hydration shells of the Al3+ ion journal March 2007
Vanadium(V) adsorption onto goethite (α-FeOOH) at pH 1.5 to 12: a surface complexation model based on ab initio molecular geometries and EXAFS spectroscopy journal April 2004
Perspective: Fifty years of density-functional theory in chemical physics journal May 2014
Toward reliable density functional methods without adjustable parameters: The PBE0 model journal April 1999
Computer simulation of electron transfer at hematite surfaces journal April 2006
Thermodynamics of Fe oxides: Part II. Enthalpies of formation and relative stability of goethite (α-FeOOH), lepidocrocite (γ-FeOOH), and maghemite (γ-Fe 2 O 3 ) journal May 2003
Phonon spectra from short non-thermally equilibrated molecular dynamics simulations journal March 1994
Canonical dynamics: Equilibrium phase-space distributions journal March 1985
Recent developments in the bond valence model of inorganic bonding journal October 1987
The adsorption of plutonium IV and V on goethite journal November 1985
The Aqueous Ca 2+ System, in Comparison with Zn 2+ , Fe 3 + , and Al 3 + : An Ab Initio Molecular Dynamics Study journal January 2013
Is the Calcite–Water Interface Understood? Direct Comparisons of Molecular Dynamics Simulations with Specular X-ray Reflectivity Data journal February 2013
Surface simulation studies of the hydration of white rust Fe(OH)2, goethite α-FeO(OH) and hematite α-Fe2O3 journal April 2007
Complexation of carbonate species at the goethite surface: Implications for adsorption of metal ions in natural waters journal May 1994
Hydrated goethite (α-FeOOH) (100) interface structure: Ordered water and surface functional groups journal April 2010
Faster proton transfer dynamics of water on SnO 2 compared to TiO 2 journal January 2011
Equatorial and apical solvent shells of the UO22+ ion journal March 2008
Generalized norm-conserving pseudopotentials journal August 1989
Molecular statics calculations for iron oxide and oxyhydroxide minerals: Toward a flexible model of the reactive mineral-water interface journal May 1996
Perspective: How good is DFT for water? journal April 2016

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Goethite
Goethite (100) surface
Fe-oxyhydroxide
Mineral water interface
Dissociative exchange
Ab initio molecular dynamics
DFT
Electronic structure
Bond valence theory
Water interaction with mineral surface
Condensed matter Grimme corrections