Precipitation pathways for ferrihydrite formation in acidic solutions

Zhu, Mengqiang; Khalid, Syed; Frandsen, Cathrine; Wallace, Adam F.; Legg, Benjamin; Zhang, Hengzhong; Morup, Steen; Banfield, Jillian F.; Waychunas, Glenn A.

doi:10.1016/j.gca.2015.09.015

Precipitation pathways for ferrihydrite formation in acidic solutions

Journal Article · Sat Oct 03 00:00:00 EDT 2015 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2015.09.015· OSTI ID:1228832

Zhu, Mengqiang ^[1]; Khalid, Syed ^[2]; Frandsen, Cathrine ^[3]; Wallace, Adam F. ^[4]; Legg, Benjamin ^[5]; Zhang, Hengzhong ^[5]; Morup, Steen ^[3]; Banfield, Jillian F. ^[6]; Waychunas, Glenn A. ^[7]

Univ. of Wyoming, Laramie, WY (United States). Dept. of Ecosystem Science and Management; Lawrence Berkeley National Lab., Berkeley, CA (United States). Earth Sciences Division
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics
Univ. of Delaware, Newark, DE (United States). Dept. of Geological Sciences
Univ. of California, Berkeley, CA (United States). Dept. of Earth and Planetary Science
Univ. of California, Berkeley, CA (United States). Dept. of Earth and Planetary Science; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Earth Sciences Division

In this study, iron oxides and oxyhydroxides form via Fe³⁺ hydrolysis and polymerization in many aqueous environments, but the pathway from Fe³⁺ monomers to oligomers and then to solid phase nuclei is unknown. In this work, using combined X-ray, UV–vis, and Mössbauer spectroscopic approaches, we were able to identify and quantify the long-time sought ferric speciation over time during ferric oxyhydroxide formation in partially-neutralized ferric nitrate solutions ([Fe³⁺] = 0.2 M, 1.8 < pH < 3). Results demonstrate that Fe exists mainly as Fe(H₂O)₆³⁺, μ-oxo aquo dimers and ferrihydrite, and that with time, the μ-oxo dimer decreases while the other two species increase in their concentrations. No larger Fe oligomers were detected. Given that the structure of the μ-oxo dimer is incompatible with those of all Fe oxides and oxyhydroxides, our results suggest that reconfiguration of the μ-oxo dimer structure occurs prior to further condensation leading up to the nucleation of ferrihydrite. The structural reconfiguration is likely the rate-limiting step involved in the nucleation process.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Danish Council for Independent Research (DFF); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; AC02-76SF00515; AC02-98CH10886

OSTI ID:: 1228832

Alternate ID(s):: OSTI ID: 1228090
OSTI ID: 1456925
OSTI ID: 1398140

Report Number(s):: BNL--108457-2015-JA

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 172; ISSN 0016-7037

Publisher:: The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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