54Mn Radiotracers Demonstrate Continuous Dissolution and Reprecipitation of Vernadite (δ-MnO2) during Interaction with Aqueous Mn(II)

Elzinga, Evert J.

doi:10.1021/acs.est.6b02874

⁵⁴Mn Radiotracers Demonstrate Continuous Dissolution and Reprecipitation of Vernadite (δ-MnO₂) during Interaction with Aqueous Mn(II)

Journal Article · Tue Jul 12 00:00:00 EDT 2016 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b02874· OSTI ID:1298280

Elzinga, Evert J. ^[1]

Rutgers Univ., Newark, NJ (United States)

⁵⁴Mn radiotracers were used to assess Mn atom exchange between aqueous Mn(II) and vernadite (δ-MnO₂) at pH 5.0. Continuous solid–liquid redistribution of⁵⁴Mn atoms occurred, and systems are near isotopic equilibrium after reaction for 3 months. Despite this extensive exchange, X-ray diffraction and X-ray absorption spectroscopy data showed no major changes in vernadite bulk mineralogy. These results demonstrate that the vernadite–Mn(II) interface is dynamic, with the substrate undergoing continuous dissolution and reprecipitation mediated by aqueous Mn(II) without observable impacts on its mineralogy. Interfacial redox reactions between adsorbed Mn(II) and solid-phase Mn(IV) and Mn(III) are proposed as the main drivers of this process. Interaction between aqueous Mn(II) and structural Mn(III) likely involves interfacial electron transfer coupled with Mn atom exchange. Here, the exchange of aqueous Mn(II) and solid-phase Mn(IV) is more complex and is proposed to result from coupled interfacial comproportionation–disproportionation reactions, where electron transfer from adsorbed Mn(II) to lattice Mn(IV) produces transient Mn(III) species that disproportionate to regenerate aqueous Mn(II) and structural Mn(IV). These findings provide further evidence of the importance of Mn(II)_(aq)–MnO_2(s) interactions and the attendant production of transient Mn(III) intermediates to the geochemical functioning of phyllomanganates in environments undergoing Mn redox cycling.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation

OSTI ID:: 1298280

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 16 Vol. 50; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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