Second Harmonic Generation Studies of Fe(II) Interactions with Hematite (α-Fe2O3)

Iron oxides are a ubiquitous class of compounds that are involved in many biological, geological, and technological processes, and the Fe(III)/Fe(II) redox couple is a fundamental transformation pathway; however, the study of iron oxide surfaces in aqueous solution by powerful spectroscopic techniqu...

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Veröffentlicht in:Journal of physical chemistry. C 2013-02, Vol.117 (8), p.4040-4047
Hauptverfasser: Jordan, David S, Hull, Christopher J, Troiano, Julianne M, Riha, Shannon C, Martinson, Alex B. F, Rosso, Kevin M, Geiger, Franz M
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container_end_page 4047
container_issue 8
container_start_page 4040
container_title Journal of physical chemistry. C
container_volume 117
creator Jordan, David S
Hull, Christopher J
Troiano, Julianne M
Riha, Shannon C
Martinson, Alex B. F
Rosso, Kevin M
Geiger, Franz M
description Iron oxides are a ubiquitous class of compounds that are involved in many biological, geological, and technological processes, and the Fe(III)/Fe(II) redox couple is a fundamental transformation pathway; however, the study of iron oxide surfaces in aqueous solution by powerful spectroscopic techniques has been limited due to “strong absorber problem”. In this work, atomic layer deposition (ALD) thin films of polycrystalline α-Fe2O3 were analyzed using the Eisenthal χ(3) technique, a variant of second harmonic generation that reports on interfacial potentials. By determining the surface charge densities at multiple pH values, the point of zero charge was found to be 5.5 ± 0.3. The interaction of aqueous Fe(II) at pH 4 and in 1 mM NaCl with ALD-prepared hematite was found to be fully reversible and to lead to about 4 times more ferrous iron ions adsorbed per square centimeter than on fused-silica surfaces under the same conditions. The data are consistent with a recently proposed conceptual model for net Fe(II) uptake or release that is underlain by a dynamic equilibrium between Fe(II) adsorbed onto hematite, electron transfer into favorable surface sites with attendant Fe(III) deposition, and electron conduction to favorable remote sites that release and replenish aqueous Fe(II).
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By determining the surface charge densities at multiple pH values, the point of zero charge was found to be 5.5 ± 0.3. The interaction of aqueous Fe(II) at pH 4 and in 1 mM NaCl with ALD-prepared hematite was found to be fully reversible and to lead to about 4 times more ferrous iron ions adsorbed per square centimeter than on fused-silica surfaces under the same conditions. The data are consistent with a recently proposed conceptual model for net Fe(II) uptake or release that is underlain by a dynamic equilibrium between Fe(II) adsorbed onto hematite, electron transfer into favorable surface sites with attendant Fe(III) deposition, and electron conduction to favorable remote sites that release and replenish aqueous Fe(II).</description><identifier>ISSN: 1932-7447</identifier><identifier>EISSN: 1932-7455</identifier><identifier>DOI: 10.1021/jp3113057</identifier><language>eng</language><publisher>Columbus, OH: American Chemical Society</publisher><subject>catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly) ; Chemistry ; Exact sciences and technology ; General and physical chemistry ; Solid-liquid interface ; Surface physical chemistry</subject><ispartof>Journal of physical chemistry. 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subjects catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)
Chemistry
Exact sciences and technology
General and physical chemistry
Solid-liquid interface
Surface physical chemistry
title Second Harmonic Generation Studies of Fe(II) Interactions with Hematite (α-Fe2O3)
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