Formation and transformation of manganese(III) intermediates in the photochemical generation of manganese(IV) oxide minerals

Zhang, Tengfei; Liu, Lihu; Tan, Wenfeng; Suib, Steven L.; Qiu, Guohong

doi:10.1016/j.chemosphere.2020.128082

Formation and transformation of manganese(III) intermediates in the photochemical generation of manganese(IV) oxide minerals

Journal Article · Sat Aug 22 00:00:00 EDT 2020 · Chemosphere

DOI:https://doi.org/10.1016/j.chemosphere.2020.128082· OSTI ID:1776115

Zhang, Tengfei ^[1]; Liu, Lihu ^[2]; Tan, Wenfeng ^[2]; Suib, Steven L. ^[3]; Qiu, Guohong ^[2]

Huazhong Agricultural University, Hubei Province (China); Univ of Connecticut
Huazhong Agricultural University, Hubei Province (China)
University of Connecticut, Storrs, CT (United States)

As important natural oxidants and adsorbents, manganese (Mn) oxide minerals affect the speciation, bioavailability and fate of pollutants and nutrient elements. It was found that birnessite-type Mn(IV) oxide minerals can be formed in the presence of NO₃^– and solar irradiation. However, the photochemical formation and transformation processes from Mn²⁺ to Mn(IV) oxide minerals remain unclear. In this work, the Mn(IV) oxide minerals were confirmed to be photochemically formed mainly due to the disproportionation of Mn(III) intermediates generated from the oxidation of Mn²⁺ in the presence of NO₃^– under UV light irradiation. The oxidation rate of Mn²⁺ to Mn(IV) oxide minerals decreased with increasing initial Mn²⁺ concentration due to the lower disproportionation rate. The increase in NO₃^– concentration, pH and temperature promoted Mn²⁺ photochemical oxidation. The photochemical formation rate of Mn(IV) oxide minerals increased with increasing ligand concentrations at low ligand concentrations. Ligands affected the formation of Mn(IV) oxide minerals by promoting the formation and reducing the reactivity of Mn(III) intermediates. Altogether, this work reveals the important role of Mn(III) intermediates in the formation of natural Mn oxide minerals.

View Accepted Manuscript (DOE)

Research Organization:: University of Connecticut, Storrs, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Key Research and Development Program of China; National Natural Science Foundation of China; Fundamental Research Funds for the Central Universities

Grant/Contract Number:: FG02-86ER13622

OSTI ID:: 1776115

Alternate ID(s):: OSTI ID: 1837953

Journal Information:: Chemosphere, Journal Name: Chemosphere Vol. 262; ISSN 0045-6535

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Formation and transformation of manganese(III) intermediates in the photochemical generation of manganese(IV) oxide minerals

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