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Electrochemical and Spectroscopic Data supported by Computational Models for Exploring the Metal- and Ligand-Based Oxidation of Mackinawite Nanoparticles

Sanden, Sebastian A.; Szilagyi, Robert K.; McGlynn, Shawn E,

Supporting information to our study, where under anaerobic conditions, ferrous iron reacts with sulfide producing FeS precipitate, which can then undergo a temperature, redox potential, and pH dependent maturation process resulting in the formation of oxidized mineral phases such as gregite or pyrite. The dataset provide information about the chemical speciation of iron-sulfide by cyclic voltammetry, Raman and X-ray absorption spectroscopic techniques. Nanoparticulate FeS was found to get oxidized to a Fe3+ containing FeS phase at -0.5 V vs. Ag/AgCl (pH = 7) and in a concomitant oxidation step, polysulfides are proposed to give a material described as Fe2+(1−3x)Fe3+(2x)S2-(1-y)(Sn2-)y. The thermodynamic differences between ligand- and metal-based oxidation processes from density functional theory can be used to describe one- and two-electron electronic and structural transformations. These findings together point to the existence of a previously unknown, metastable FeS phase located between FeS and greigite (Fe2+Fe3+2S2-4) along a metal oxidation path, and Fe2+S2- and pyrite (Fe2+S22-) along a ligand oxidation path, respectively.

Manuscript is under consideration at Dalton Trans. 2021 DT-ART-05-2021-001684. S. A. S. acknowledges a graduate scholarship received from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan. S. E. M. acknowledges support by NSF award # 1724300. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The SSRL Structural Molecular Biology Program is supported by the DOE Office of Biological and Environmental Research, and by the National Institutes of Health, National Institute of General Medical Sciences (P30GM133894). The contents of this publication are solely the responsibility of the authors and do not necessarily represent the official views of NIGMS or NIH. Access to CCDB and ICSD crystal structures databases and subsequent computational research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DESC0020246 (RKSz).
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2Fe2S-FeSSFe.zip
md5:1d04c928dcdd459ad4d8425579726139 		203.5 MB Download
[2Fe-2S]_Raman.zip
md5:9b0dc127b78110b711e51575b11702dc 		41.1 MB Download
___README.txt
md5:95ad8dcee8d02bdd953fe47891311e0a 		4.1 kB Download
combinatorial_models.zip
md5:77490e0aabe19a54739dbbf3bc6ec561 		10.5 MB Download
core_extraction.zip
md5:10dfdd5888262606b811bbc1b50e6198 		53.8 MB Download
FeS_complexes.zip
md5:17c0683d900b195b73bae0a642187d81 		130.2 MB Download
FeS_PO4_voltammetry.xlsx
md5:ba7a81a56911c5c8e773262f7dbaa199 		6.0 MB Download
FeS_Raman.xlsx
md5:c82ebc784a7f9436c93611e732497f24 		3.8 MB Download
FeS_XANES.xlsx
md5:fcaa16776f177c00a25541510a2fb42a 		995.3 kB Download
files.txt
md5:fddd1256f1a7ffe20deac7a2f0362e5d 		54.4 kB Download
fragments_for_merging.zip
md5:a5ee7ae5f9b3ac73768f3202d94b6f6e 		8.3 MB Download
mackinawite_nanoparticles.zip
md5:42c490854b3b872734b5a301597a2b5f 		2.0 GB Download
xrd-based_models.zip
md5:005219e7e4c215491b307e5f5ea8e1f5 		44.5 MB Download
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Publication date:
July 1, 2021
DOI:
10.5281/zenodo.5056738

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Keyword(s):
mackinawite nanoparticles ferric mackinawite FeS oxidation cyclic voltammetry S K-edge X-ray absorption spectroscopy Raman spectroscopy density functional theory modeling metal-based redox chemistry ligand-based redox chemistry
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