ArticleProceedings of the National Academy of Sciences of the United States of America2015
Rate and mechanism of the photoreduction of birnessite (MnO2) nanosheets.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2015. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 13 papers.
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13 citing papers in PubMed, 85 citations in OpenAlex.
- Predicting rates of manganese oxide reduction from thermodynamic driving forces and structural properties.Proceedings of the National Academy of Sciences of the United States of America · 2026Article
- Structure of HEPES-Reduced δ‑MnOChemistry of materials : a publication of the American Chemical Society · 2026Article
- Utilizing surface water adsorption on layered MnOCommunications chemistry · 2025Article
- Light-Mediated Electrochemical Synthesis of Manganese Oxide Enhances Its Stability for Water Oxidation.ACS nanoscience Au · 2023Article
- Involvement of Bacterial and Fungal Extracellular Products in Transformation of Manganese-Bearing Minerals and Its Environmental Impact.International journal of molecular sciences · 2023Review
- Siderophore-Mediated Mobilization of Manganese Limits Iron Solubility in Mixed Mineral Systems.ACS earth & space chemistry · 2023Article
- Organic buffers act as reductants of abiotic and biogenic manganese oxides.Scientific reports · 2023Article
- An ecophysiological explanation for manganese enrichment in rock varnish.Proceedings of the National Academy of Sciences of the United States of America · 2021Article
- Selective Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran by Visible Light-Driven Photocatalysis over In Situ Substrate-Sensitized Titania.ChemSusChem · 2021Article
- The critical role of point defects in improving the specific capacitance of δ-MnONature communications · 2017Article
- Biological and environmental interactions of emerging two-dimensional nanomaterials.Chemical Society reviews · 2016Review
- Oxidation of arsenite to arsenate on birnessite in the presence of light.Geochemical transactions · 2016Article
- Cryptomelane formation from nanocrystalline vernadite precursor: a high energy X-ray scattering and transmission electron microscopy perspective on reaction mechanisms.Geochemical transactions · 2015Article
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Authors and funding
6 authors at 4 institutions in 3 countries.
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Abstract
The photoreductive dissolution of Mn(IV) oxide minerals in sunlit aquatic environments couples the Mn cycle to the oxidation of organic matter and fate of trace elements associated with Mn oxides, but the intrinsic rate and mechanism of mineral dissolution in the absence of organic electron donors is unknown. We investigated the photoreduction of δ-MnO2 nanosheets at pH 6.5 with Na or Ca as the interlayer cation under 400-nm light irradiation and quantified the yield and timescales of Mn(III) production. Our study of transient intermediate states using time-resolved optical and X-ray absorption spectroscopy showed key roles for chemically distinct Mn(III) species. The reaction pathway involves (i) formation of Jahn-Teller distorted Mn(III) sites in the octahedral sheet within 0.6 ps of photoexcitation; (ii) Mn(III) migration into the interlayer within 600 ps; and (iii) increased nanosheet stacking. We propose that irreversible Mn reduction is coupled to hole-scavenging by surface water molecules or hydroxyl groups, with associated radical formation. This work demonstrates the importance of direct MnO2 photoreduction in environmental processes and provides a framework to test new hypotheses regarding the role of organic molecules and metal species in photochemical reactions with Mn oxide phases. The timescales for the production and evolution of Mn(III) species and a catalytic role for interlayer Ca(2+) identified here from spectroscopic measurements can also guide the design of efficient Mn-based catalysts for water oxidation.
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