Redistribution of Electron Equivalents between Magnetite and Aqueous Fe2+ Induced by a Model Quinone Compound AQDS

Peng, Huan; Pearce, Carolyn I.; N’Diaye, Alpha T.; Zhu, Zhenli; Ni, Jinren; Rosso, Kevin M.; Liu, Juan

doi:10.1021/acs.est.8b05098

Redistribution of Electron Equivalents between Magnetite and Aqueous Fe²⁺ Induced by a Model Quinone Compound AQDS

Journal Article · Wed Jan 23 00:00:00 EST 2019 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.8b05098· OSTI ID:1635173

Peng, Huan ^[1]; ^[2]; N’Diaye, Alpha T. ^[3]; Zhu, Zhenli ^[4]; ^[5]; ^[2]; ^[5]

Peking Univ., Beijing (China); China Univ. of Geosciences, Wuhan (China)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
China Univ. of Geosciences, Wuhan (China)
Peking Univ., Beijing (China)

The complex interactions between magnetite and aqueous Fe²⁺ (Fe²⁺_(aq)) pertain to many biogeochemical redox processes in anoxic subsurface environments. The effect of natural organic matter, abundant in these same environments, on Fe²⁺_(aq)-magnetite interactions is an additional complex that remains poorly understood. We investigated the influence of a model quinone molecule anthraquinone-2,6-disulfonate (AQDS) on Fe²⁺_(aq)-magnetite interactions by systematically studying equilibrium Fe²⁺_(aq) concentrations, rates and extents of AQDS reduction, and structural versus surface-localized Fe(II)/Fe(III) ratios in magnetite under different controlled experimental conditions. The equilibrium concentration of Fe²⁺_(aq) in Fe²⁺-amended magnetite suspensions with AQDS proportionally changes with solution pH or initial AQDS concentration, but independent of magnetite loadings through the solid concentrations that were studied here. The rates and extents of AQDS reduction by Fe²⁺-amended magnetite proportionally increased with solution pH, magnetite loading, and initial Fe²⁺_(aq) concentration, which correlates with the corresponding change of reduction potentials for the Fe²⁺-magnetite system. AQDS reduction by surface-associated Fe(II) in the Fe2+-magnetite suspensions induces solid-state migration of electron equivalents from particle interiors to the near-surface region and the production of nonmagnetic Fe(II)-containing species, which inhibits Fe²⁺_(aq) incorporation or electron injection into the magnetite structure. Finally, this study demonstrates the significant influence of quinones on reductive activity of the Fe²⁺-magnetite system.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Basic Research Program of China; National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1635173

Alternate ID(s):: OSTI ID: 1506691

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 4 Vol. 53; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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