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Effects of C/Mn Ratios on the Sorption and Oxidative Degradation of Small Organic Molecules on Mn-Oxides

Cite this: Environ. Sci. Technol. 2023, 57, 1, 741–750
Publication Date (Web):December 19, 2022
https://doi.org/10.1021/acs.est.2c03633
Copyright © 2022 American Chemical Society

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    Abstract

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    Manganese (Mn) oxides have a high surface area and redox potential that facilitate sorption and/or oxidation of organic carbon (OC), but their role in regulating soil C storage is relatively unexplored. Small OC compounds with distinct structures were reacted with Mn(III/IV)-oxides to investigate the effects of OC/Mn molar ratios on Mn–OC interaction mechanisms. Dissolved and solid-phase OC and Mn were measured to quantify the OC sorption to and/or the redox reaction with Mn-oxides. Mineral transformation was evaluated using X-ray diffraction and X-ray absorption spectroscopy. Higher OC/Mn ratios resulted in higher sorption and/or redox transformation; however, interaction mechanisms differed at low or high OC/Mn ratios for some OC. Citrate, pyruvate, ascorbate, and catechol induced Mn-oxide dissolution. The average oxidation state of Mn in the solid phase did not change during the reaction with citrate, suggesting ligand-promoted mineral dissolution, but decreased significantly during reactions with the other compounds, suggesting reductive dissolution mechanisms. Phthalate primarily sorbed on Mn-oxides with no detectable formation of redox products. Mn–OC interactions led primarily to C loss through OC oxidation into inorganic C, except phthalate, which was predominantly immobilized in the solid phase. Together, these results provided detailed fundamental insights into reactions happening at organo–mineral interfaces in soils.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.2c03633.

    • Mn-oxides synthesis methods; parameters for 1H NMR analysis; characteristics of organic compounds and Mn-oxides; fitting results from XANES spectra; XANES whole spectra of Mn-oxide minerals; XAS spectra of the unreacted Mn-oxides; OC distribution; Mn dissolution; XANES spectra of solid phases; Mn AOS; EXAFS spectra of the Mn-oxides; images of Mn-oxides after the reactions; XRD pattern of the solid phases after the reaction; and 1H NMR spectra of the solution (PDF)

    • XANES Mn whole spectra (XLS)

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