Precipitation pathways for ferrihydrite formation in acidic solutions
Abstract
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+]=0.2M, 1.8
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Danish Council for Independent Research (DFF)
- OSTI Identifier:
- 1228832
- Alternate Identifier(s):
- OSTI ID: 1398140; OSTI ID: 1456925
- Report Number(s):
- BNL-108457-2015-JA
Journal ID: ISSN 0016-7037; R&D Project: LS001
- Grant/Contract Number:
- SC00112704; AC02-05CH11231; EAR-1529937; AC02-98CH10886; AC02-06CH11357; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 172; Journal Issue: C; Journal ID: ISSN 0016-7037
- Publisher:
- The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Zhu, Mengqiang, Khalid, Syed, Frandsen, Cathrine, Wallace, Adam F., Legg, Benjamin, Zhang, Hengzhong, Morup, Steen, Banfield, Jillian F., and Waychunas, Glenn A. Precipitation pathways for ferrihydrite formation in acidic solutions. United States: N. p., 2015.
Web. doi:10.1016/j.gca.2015.09.015.
Zhu, Mengqiang, Khalid, Syed, Frandsen, Cathrine, Wallace, Adam F., Legg, Benjamin, Zhang, Hengzhong, Morup, Steen, Banfield, Jillian F., & Waychunas, Glenn A. Precipitation pathways for ferrihydrite formation in acidic solutions. United States. https://doi.org/10.1016/j.gca.2015.09.015
Zhu, Mengqiang, Khalid, Syed, Frandsen, Cathrine, Wallace, Adam F., Legg, Benjamin, Zhang, Hengzhong, Morup, Steen, Banfield, Jillian F., and Waychunas, Glenn A. Sat .
"Precipitation pathways for ferrihydrite formation in acidic solutions". United States. https://doi.org/10.1016/j.gca.2015.09.015. https://www.osti.gov/servlets/purl/1228832.
@article{osti_1228832,
title = {Precipitation pathways for ferrihydrite formation in acidic solutions},
author = {Zhu, Mengqiang and Khalid, Syed and Frandsen, Cathrine and Wallace, Adam F. and Legg, Benjamin and Zhang, Hengzhong and Morup, Steen and Banfield, Jillian F. and Waychunas, Glenn A.},
abstractNote = {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+]=0.2M, 1.8},
doi = {10.1016/j.gca.2015.09.015},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 172,
place = {United States},
year = {Sat Oct 03 00:00:00 EDT 2015},
month = {Sat Oct 03 00:00:00 EDT 2015}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Cited by: 54 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005
- Ravel, B.; Newville, M.
- Journal of Synchrotron Radiation, Vol. 12, Issue 4
Neutron Pair Distribution Function Study of Two-Line Ferrihydrite
journal, December 2011
- Harrington, Richard; Hausner, Douglas B.; Xu, Wenqian
- Environmental Science & Technology, Vol. 45, Issue 23
Dissimilatory Reduction and Transformation of Ferrihydrite-Humic Acid Coprecipitates
journal, November 2013
- Shimizu, Masayuki; Zhou, Jihai; Schröder, Christian
- Environmental Science & Technology, Vol. 47, Issue 23
Effect of phosphate, silicate, and Ca on Fe(III)-precipitates formed in aerated Fe(II)- and As(III)-containing water studied by X-ray absorption spectroscopy
journal, January 2010
- Voegelin, Andreas; Kaegi, Ralf; Frommer, Jakob
- Geochimica et Cosmochimica Acta, Vol. 74, Issue 1
Iron (III)-silica interactions in aqueous solution: insights from X-ray absorption fine structure spectroscopy
journal, October 2003
- Pokrovski, Gleb S.; Schott, Jacques; Farges, François
- Geochimica et Cosmochimica Acta, Vol. 67, Issue 19
Dynamic Fe-precipitate formation induced by Fe(II) oxidation in aerated phosphate-containing water
journal, September 2013
- Voegelin, Andreas; Senn, Anna-Caterina; Kaegi, Ralf
- Geochimica et Cosmochimica Acta, Vol. 117
Early Stage Formation of Iron Oxyhydroxides during Neutralization of Simulated Acid Mine Drainage Solutions
journal, July 2012
- Zhu, Mengqiang; Legg, Benjamin; Zhang, Hengzhong
- Environmental Science & Technology, Vol. 46, Issue 15
Iron speciation in natural hyperacid water investigated by Mössbauer spectroscopy
journal, November 2009
- Bender Koch, C.; Rasmussen, H. K.; Mørup, S.
- Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 74, Issue 4
Speciation and Crystal Chemistry of Iron(III) Chloride Hydrolyzed in the Presence of SiO 4 Ligands. 3. Semilocal Scale Structure of the Aggregates
journal, August 2001
- Masion, Armand; Doelsch, Emmanuel; Rose, Jérôme
- Langmuir, Vol. 17, Issue 16
Aqueous formation and manipulation of the iron-oxo Keggin ion
journal, February 2015
- Sadeghi, O.; Zakharov, L. N.; Nyman, M.
- Science, Vol. 347, Issue 6228
Studies on the mechanism of hydrolysis and polymerization of aluminum salts in aqueous solution: correlations between the “Core-links” model and “Cage-like” Keggin-Al13 model
journal, March 2004
- Bi, S.
- Coordination Chemistry Reviews, Vol. 248, Issue 5-6
The influence of crystallinity on magnetic ordering in natural ferrihydrites
journal, June 1988
- Murad, E.; Bowen, L. H.; Long, G. J.
- Clay Minerals, Vol. 23, Issue 2
Structure and Mechanisms of Formation of FeOOH(NO 3 ) Oligomers in the Early Stages of Hydrolysis
journal, June 1997
- Rose, Jérôme; Manceau, Alain; Masion, Armand
- Langmuir, Vol. 13, Issue 12
Chromatographic Separation and Characterization of Hydrolyzed Cr(III) Species
journal, July 2002
- Friese, J. I.; Ritherdon, B.; Clark, S. B.
- Analytical Chemistry, Vol. 74, Issue 13
Environmentally Abundant Anions Influence the Nucleation, Growth, Ostwald Ripening, and Aggregation of Hydrous Fe(III) Oxides
journal, May 2012
- Hu, Yandi; Lee, Byeongdu; Bell, Christopher
- Langmuir, Vol. 28, Issue 20
Structure of Sulfate Adsorption Complexes on Ferrihydrite
journal, October 2013
- Zhu, Mengqiang; Northrup, Paul; Shi, Chenyang
- Environmental Science & Technology Letters, Vol. 1, Issue 1
Characterization of Decaaqua-mu-oxodi-iron(III) by Mössbauer and Vibrational Spectroscopy.
journal, January 1975
- Knudsen, J. M.; Larsen, Erik; Moreira, J. E.
- Acta Chemica Scandinavica, Vol. 29a
Molecular Dynamics Simulation Study of the Early Stages of Nucleation of Iron Oxyhydroxide Nanoparticles in Aqueous Solutions
journal, August 2015
- Zhang, Hengzhong; Waychunas, Glenn A.; Banfield, Jillian F.
- The Journal of Physical Chemistry B, Vol. 119, Issue 33
SIXPack a Graphical User Interface for XAS Analysis Using IFEFFIT
journal, January 2005
- Webb, S. M.
- Physica Scripta
Kinetics of Hydrolysis and Precipitation of Ferric Iron in Seawater
journal, September 2003
- Rose, Andrew L.; Waite, T. David
- Environmental Science & Technology, Vol. 37, Issue 17
Reconciling kinetic and equilibrium observations of iron(III) solubility in aqueous solutions with a polymer-based model
journal, December 2007
- Rose, Andrew L.; David Waite, T.
- Geochimica et Cosmochimica Acta, Vol. 71, Issue 23
Sulfate Local Coordination Environment in Schwertmannite
journal, August 2015
- Wang, Xiaoming; Gu, Chunhao; Feng, Xionghan
- Environmental Science & Technology, Vol. 49, Issue 17
The nature of x-ray scattering from geo-nanoparticles: Practical considerations of the use of the Debye equation and the pair distribution function for structure analysis
journal, November 2012
- Harrington, Richard; Neder, Reinhard B.; Parise, John B.
- Chemical Geology, Vol. 329
Fe(III) Nucleation in the Presence of Bivalent Cations and Oxyanions Leads to Subnanoscale 7 Å Polymers
journal, October 2014
- van Genuchten, Case M.; Gadgil, Ashok J.; Peña, Jasquelin
- Environmental Science & Technology, Vol. 48, Issue 20
In Situ Structural Characterization of Ferric Iron Dimers in Aqueous Solutions: Identification of μ-Oxo Species
journal, May 2013
- Zhu, Mengqiang; Puls, Brendan W.; Frandsen, Cathrine
- Inorganic Chemistry, Vol. 52, Issue 12
Nucleation and Growth Mechanisms of Fe Oxyhydroxide in the Presence of PO 4 Ions. 1. Fe K-Edge EXAFS Study
journal, January 1996
- Rose, Jérôme; Manceau, Alain; Bottero, Jean-Yves
- Langmuir, Vol. 12, Issue 26
Formation and secondary mineralization of ferrihydrite in the presence of silicate and Mn(II)
journal, November 2015
- Wang, Xiaoming; Zhu, Mengqiang; Lan, Shuai
- Chemical Geology, Vol. 415
On the Crystal Structure of Some Basic Aluminium Salts.
journal, January 1960
- Johansson, Georg; Gullman, Lars-Otto; Kjekshus, Arne
- Acta Chemica Scandinavica, Vol. 14
Formation Mechanism of the Ga 13 Keggin Ion: A Combined EXAFS and NMR Study
journal, June 2000
- Michot, Laurent J.; Montargès-Pelletier, Emmanuelle; Lartiges, Bruno S.
- Journal of the American Chemical Society, Vol. 122, Issue 25
Speciation of Fe in Fe-modified zeolite catalysts
journal, August 2010
- Smoláková, Lucie; Grygar, Tomáš; Čapek, Libor
- Journal of Electroanalytical Chemistry, Vol. 647, Issue 1
From Fe(III) Ions to Ferrihydrite and then to Hematite
journal, January 1999
- Schwertmann, Udo; Friedl, Josef; Stanjek, Helge
- Journal of Colloid and Interface Science, Vol. 209, Issue 1
Homopolynuclear and heteropolynuclear Rh(III) aqua ions – a review
journal, July 2004
- Spiccia, Leone
- Inorganica Chimica Acta, Vol. 357, Issue 10
Direct Observation of Tetrahedrally Coordinated Fe(III) in Ferrihydrite
journal, March 2012
- Peak, Derek; Regier, Tom
- Environmental Science & Technology, Vol. 46, Issue 6
Hydrolysis of inorganic iron(III) salts
journal, February 1984
- Flynn, Charles M.
- Chemical Reviews, Vol. 84, Issue 1
Nucleation and Growth Mechanisms of Iron Oxyhydroxides in the Presence of PO 4 Ions. 4. Structure of the Aggregates
journal, July 1997
- Masion, Armand; Rose, Jérôme; Bottero, Jean-Yves
- Langmuir, Vol. 13, Issue 14
Size-Dependent Bandgap of Nanogoethite
journal, August 2011
- Zhang, Hengzhong; Bayne, Meredith; Fernando, Sandra
- The Journal of Physical Chemistry C, Vol. 115, Issue 36
The Mössbauer spectrum of “well”-crystallized ferrihydrite
journal, September 1988
- Murad, Enver
- Journal of Magnetism and Magnetic Materials, Vol. 74, Issue 2
A disordered nanoparticle model for 6-line ferrihydrite
journal, August 2013
- Gilbert, B.; Erbs, J. J.; Penn, R. L.
- American Mineralogist, Vol. 98, Issue 8-9
Removing Arsenic from Synthetic Groundwater with Iron Electrocoagulation: An Fe and As K-Edge EXAFS Study
journal, December 2011
- van Genuchten, Case M.; Addy, Susan E. A.; Peña, Jasquelin
- Environmental Science & Technology, Vol. 46, Issue 2
Iron oxides: From molecular clusters to solid. A nice example of chemical versatility
journal, June 2006
- Jolivet, Jean-Pierre; Tronc, Elisabeth; Chanéac, Corinne
- Comptes Rendus Geoscience, Vol. 338, Issue 6-7
Iron(III) Hydrolysis and Solubility at 25 °C
journal, September 2007
- Stefánsson, Andri
- Environmental Science & Technology, Vol. 41, Issue 17
Kinetics of Fe(III) precipitation in aqueous solutions at pH 6.0–9.5 and 25°C
journal, February 2006
- Pham, A. Ninh; Rose, Andrew L.; Feitz, Andrew J.
- Geochimica et Cosmochimica Acta, Vol. 70, Issue 3
Kinetics of ferric oxyhydroxide precipitation
journal, August 1993
- Grundl, Tim; Delwiche, Jim
- Journal of Contaminant Hydrology, Vol. 14, Issue 1
Competing Fe(II)-Induced Mineralization Pathways of Ferrihydrite
journal, September 2005
- Hansel, Colleen M.; Benner, Shawn G.; Fendorf, Scott
- Environmental Science & Technology, Vol. 39, Issue 18
Iron oxide chemistry. From molecular clusters to extended solid networks
journal, January 2004
- Jolivet, Jean-Pierre; Chanéac, Corinne; Tronc, Elisabeth
- Chem. Commun., Issue 5
Surface and mineral structure of ferrihydrite
journal, March 2013
- Hiemstra, Tjisse
- Geochimica et Cosmochimica Acta, Vol. 105
Utilization of crown ethers to stabilize the dinuclear μ-oxo bridged iron(iii) aqua ion, [(H2O)5Fe(μ-O)Fe(OH2)5]4+
journal, January 2002
- Junk, Peter C.; McCool, Brian J.; Moubaraki, Boujemaa
- Journal of the Chemical Society, Dalton Transactions, Issue 6
Structural relationships between colloidal solutions and hydroxide gels of iron(III) nitrate
journal, January 1977
- Magini, M.
- Journal of Inorganic and Nuclear Chemistry, Vol. 39, Issue 3
Formation, aggregation and reactivity of amorphous ferric oxyhydroxides on dissociation of Fe(III)–organic complexes in dilute aqueous suspensions
journal, October 2010
- Bligh, Mark W.; Waite, T. David
- Geochimica et Cosmochimica Acta, Vol. 74, Issue 20
Hydrolysis of Iron(III)…Chaotic Olation Versus Nucleation
journal, March 1984
- Schneider, W.
- Comments on Inorganic Chemistry, Vol. 3, Issue 4
Partial hydrolysis of ferric nitrate salt. Structural investigation by dynamic light scattering and small-angle x-ray scattering
journal, July 1991
- Bottero, Jean Yves.; Tchoubar, D.; Arnaud, M.
- Langmuir, Vol. 7, Issue 7
Composition and Structure of Polynuclear Chromium(III) Hydroxo Complexes
journal, November 2009
- Torapava, Natallia; Radkevich, Artsiom; Davydov, Dmitri
- Inorganic Chemistry, Vol. 48, Issue 21
Minerals as Molecules-Use of Aqueous Oxide and Hydroxide Clusters to Understand Geochemical Reactions
journal, April 2009
- Casey, William H.; Rustad, James R.; Spiccia, Leone
- Chemistry - A European Journal, Vol. 15, Issue 18
Ordered ferrimagnetic form of ferrihydrite reveals links among structure, composition, and magnetism
journal, February 2010
- Michel, F. M.; Barron, V.; Torrent, J.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 7
Structure of Fe(III) precipitates generated by the electrolytic dissolution of Fe(0) in the presence of groundwater ions
journal, February 2014
- van Genuchten, Case M.; Peña, Jasquelin; Amrose, Susan E.
- Geochimica et Cosmochimica Acta, Vol. 127
New Reaction Path in the Dissociation of the Fe 2 (μ-OH) 2 (H 2 O) 8 4+ Complex
journal, February 1999
- Lente, Gábor; Fábián, István
- Inorganic Chemistry, Vol. 38, Issue 3
The Structure of Ferrihydrite, a Nanocrystalline Material
journal, June 2007
- Michel, F. M.; Ehm, L.; Antao, S. M.
- Science, Vol. 316, Issue 5832
Structure and mechanisms of formation of iron oxide hydroxide (chloride) polymers
journal, January 1994
- Bottero, Jean Yves; Manceau, Alain; Villieras, Frederic
- Langmuir, Vol. 10, Issue 1
Basic concepts of the crystallization from aqueous solutions: The example of aluminum oxy(hydroxi)des and aluminosilicates
journal, February 2011
- Jolivet, Jean-Pierre; Chanéac, Corinne; Chiche, David
- Comptes Rendus Geoscience, Vol. 343, Issue 2-3
Formation of iron(III) hydroxides from homogeneous solutions
journal, June 1997
- Deng, Yiwei
- Water Research, Vol. 31, Issue 6
The structure of an iron core analog of ferritin
journal, June 1968
- Brady, G. W.; Kurkjian, C. R.; Lyden, E. F. X.
- Biochemistry, Vol. 7, Issue 6
Mössbauer spectroscopic studies of the magnetic hyperfine interaction in the ferric hexaquo complex in frozen aqueous solution
journal, January 1977
- Knudsen, J. E.
- Journal of Physics and Chemistry of Solids, Vol. 38, Issue 8
Early stages of the hydrolysis of chromium(III) in aqueous solution. 4. The stability constants of the hydrolytic dimer, trimer, and tetramer at 25.degree.C and I = 1.0 M
journal, January 1989
- Stuenzi, Hans; Spiccia, Leone; Rotzinger, Francois P.
- Inorganic Chemistry, Vol. 28, Issue 1
Quick extended x-ray absorption fine structure instrument with millisecond time scale, optimized for in situ applications
journal, January 2010
- Khalid, S.; Caliebe, W.; Siddons, P.
- Review of Scientific Instruments, Vol. 81, Issue 1
New insight into the structure of nanocrystalline ferrihydrite: EXAFS evidence for tetrahedrally coordinated iron(III)
journal, May 2011
- Maillot, Fabien; Morin, Guillaume; Wang, Yuheng
- Geochimica et Cosmochimica Acta, Vol. 75, Issue 10
Nucleation and Growth Mechanisms of Fe Oxyhydroxide in the Presence of PO 4 Ions. 2. P K-Edge EXAFS Study
journal, March 1997
- Rose, Jérôme; Flank, Anne-Marie; Masion, Armand
- Langmuir, Vol. 13, Issue 6
Al30: A Giant Aluminum Polycation
journal, February 2000
- Allouche, Lionel; Gérardin, Corine; Loiseau, Thierry
- Angewandte Chemie International Edition, Vol. 39, Issue 3
Supramolecular Complexation of Polynuclear Aqua Ions: A Crown Ether Adduct of aμ-Oxo-Bridged Iron(III) Aqua Dimer
journal, August 1999
- Junk, Peter C.; McCool, Brian J.; Moubaraki, Boujemaa
- Angewandte Chemie International Edition, Vol. 38, Issue 15
Nucleation and Growth Mechanisms of Iron Oxyhydroxides in the Presence of PO4 Ions. 3. Speciation of Fe by Small Angle X-ray Scattering
journal, July 1997
- Masion, Armand; Rose, Jérôme; Bottero, Jean-Yves
- Langmuir, Vol. 13, Issue 14
Works referencing / citing this record:
Composition-Dependent Sorptive Fractionation of Anthropogenic Dissolved Organic Matter by Fe(III)-Montmorillonite
journal, March 2018
- Young, Robert; Avneri-Katz, Shani; McKenna, Amy
- Soil Systems, Vol. 2, Issue 1
The Role of Bi 3+ in Promoting and Stabilizing Iron Oxo Clusters in Strong Acid
journal, April 2018
- Sadeghi, Omid; Amiri, Mehran; Reinheimer, Eric W.
- Angewandte Chemie International Edition, Vol. 57, Issue 21
Condensed ferric dimers for green photocatalytic synthesis of nylon precursors
journal, January 2019
- Ide, Yusuke; Tominaka, Satoshi; Yoneno, Yumi
- Chemical Science, Vol. 10, Issue 27
Direct Evidence for Ferrous Ion Oxidation and Incorporation in the Absence of Oxidants by Dps from Marinobacter hydrocarbonoclasticus
journal, December 2018
- Penas, Daniela; Pereira, Alice S.; Tavares, Pedro
- Angewandte Chemie, Vol. 131, Issue 4
Evolution of the reactive surface area of ferrihydrite: time, pH, and temperature dependency of growth by Ostwald ripening
journal, January 2019
- Hiemstra, Tjisse; Mendez, Juan C.; Li, Jiayu
- Environmental Science: Nano, Vol. 6, Issue 3
Iron speciation in iron–organic matter nanoaggregates: a kinetic approach coupling Quick-EXAFS and MCR-ALS chemometrics
journal, January 2019
- Vantelon, Delphine; Davranche, Mélanie; Marsac, Rémi
- Environmental Science: Nano, Vol. 6, Issue 8
Direct Evidence for Ferrous Ion Oxidation and Incorporation in the Absence of Oxidants by Dps from Marinobacter hydrocarbonoclasticus
journal, January 2019
- Penas, Daniela; Pereira, Alice S.; Tavares, Pedro
- Angewandte Chemie International Edition, Vol. 58, Issue 4
The Role of Bi 3+ in Promoting and Stabilizing Iron Oxo Clusters in Strong Acid
journal, April 2018
- Sadeghi, Omid; Amiri, Mehran; Reinheimer, Eric W.
- Angewandte Chemie, Vol. 130, Issue 21
Iron Aquo Complex as an Efficient and Selective Homogeneous Photocatalyst for Organic Synthetic Reactions
journal, October 2018
- Iqbal, Muhammad Faisal; Tominaka, Satoshi; Peng, Wenqin
- ChemCatChem, Vol. 10, Issue 20