Rate and mechanism of the photoreduction of birnessite (MnO 2 ) nanosheets

Marafatto, Francesco Femi; Strader, Matthew L.; Gonzalez-Holguera, Julia; Schwartzberg, Adam; Gilbert, Benjamin; Peña, Jasquelin

doi:10.1073/pnas.1421018112

Title: Rate and mechanism of the photoreduction of birnessite (MnO ₂ ) nanosheets

Journal Article · Mon Mar 30 00:00:00 UTC 2015 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1421018112 · OSTI ID:1235165

Marafatto, Francesco Femi ^[1]; Strader, Matthew L. ^[2]; Gonzalez-Holguera, Julia ^[1]; Schwartzberg, Adam ^[3]; Gilbert, Benjamin ^[4]; Peña, Jasquelin ^[1]

Institute of Earth Surface Dynamics, University of Lausanne, CH-1015 Lausanne, Switzerland, and
Chemical Sciences Division,
Molecular Foundry, and
Earth Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720

Significance The photoreductive dissolution of Mn oxides governs the biogeochemical cycle of Mn and the fate of organic and inorganic species associated with Mn oxides in the euphotic zones of marine and freshwater systems. Mn oxide minerals also have garnered interest as water oxidation catalysts inspired by the Mn ₄ CaO ₄ cluster of photosystem II. However, the mechanism of water oxidation by MnO ₂ and the rate limiting steps for this reaction are unknown. In this study, we couple flow-through experiments and ultrafast pump–probe optical and X-ray absorption spectroscopy to develop a photoreduction model that includes the mechanism and timescales for the initial electron transfer steps in the oxidation of water by MnO ₂ .

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Research Organization:: Advanced Photon Source (APS), Argonne National Laboratory (ANL), Argonne, IL (US)

Sponsoring Organization:: FOREIGNOTHER; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1235165

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 15 Vol. 112; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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