A Manganese Compound I Model with a High Reactivity in the Oxidation of Organic Substrates and Water

Lina Zhang; Mi Sook Seo; Yunhee Choi; Roman Ezhov; Olga Maximova; Deesha D. Malik; Maggie Ng; Yong Min Lee; Ritimukta Sarangi; Yulia N. Pushkar; Kyung Bin Cho; Wonwoo Nam

doi:10.1021/jacs.3c01818

A Manganese Compound I Model with a High Reactivity in the Oxidation of Organic Substrates and Water

Lina Zhang, Mi Sook Seo, Yunhee Choi, Roman Ezhov, Olga Maximova, Deesha D. Malik, Maggie Ng, Yong Min Lee, Ritimukta Sarangi, Yulia N. Pushkar, Kyung Bin Cho, Wonwoo Nam

Chemistry & Nanoscience

Research output: Contribution to journal › Article › peer-review

Abstract

A high-valent manganese(IV)-hydroxo porphyrin π-cation radical complex, [Mn(IV)(OH)(Porp^+•)(X)]⁺, was synthesized and characterized spectroscopically. The Mn porphyrin intermediate was highly reactive in alkane hydroxylation and oxygen atom transfer reactions. More importantly, the Mn porphyrin intermediate reacted with water at a fast rate, resulting in the dioxygen evolution. To the best of our knowledge, we report the first manganese Cpd I model compound bearing a porphyrin π-cation radical ligand with a high reactivity in oxidation reactions, including water oxidation.

Original language	English
Journal	Journal of the American Chemical Society
DOIs	https://doi.org/10.1021/jacs.3c01818
State	Accepted/In press - 2023

Bibliographical note

Funding Information:
This work was supported by the NRF of Korea (NRF-2021R1A3B1076539 to W.N., NRF-2020R1I1A1A01074630 to Y.-M.L., and NRF-2021R1A2C1012851 to K.-B.C). This research was also supported by NSF CHE-2004147 to Y.P. The use of the Advanced Photon Source, an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract DE-AC02- 06CH11357. The PNC/XSD (Sector 20) facilities at the Advanced Photon Source and research at these facilities were supported by the U.S. Department of Energy, Basic Energy Science, and the Canadian Light Source.

Publisher Copyright:
© 2023 American Chemical Society.

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10.1021/jacs.3c01818

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title = "A Manganese Compound I Model with a High Reactivity in the Oxidation of Organic Substrates and Water",

abstract = "A high-valent manganese(IV)-hydroxo porphyrin π-cation radical complex, [Mn(IV)(OH)(Porp+•)(X)]+, was synthesized and characterized spectroscopically. The Mn porphyrin intermediate was highly reactive in alkane hydroxylation and oxygen atom transfer reactions. More importantly, the Mn porphyrin intermediate reacted with water at a fast rate, resulting in the dioxygen evolution. To the best of our knowledge, we report the first manganese Cpd I model compound bearing a porphyrin π-cation radical ligand with a high reactivity in oxidation reactions, including water oxidation.",

author = "Lina Zhang and Seo, {Mi Sook} and Yunhee Choi and Roman Ezhov and Olga Maximova and Malik, {Deesha D.} and Maggie Ng and Lee, {Yong Min} and Ritimukta Sarangi and Pushkar, {Yulia N.} and Cho, {Kyung Bin} and Wonwoo Nam",

note = "Funding Information: This work was supported by the NRF of Korea (NRF-2021R1A3B1076539 to W.N., NRF-2020R1I1A1A01074630 to Y.-M.L., and NRF-2021R1A2C1012851 to K.-B.C). This research was also supported by NSF CHE-2004147 to Y.P. The use of the Advanced Photon Source, an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract DE-AC02- 06CH11357. The PNC/XSD (Sector 20) facilities at the Advanced Photon Source and research at these facilities were supported by the U.S. Department of Energy, Basic Energy Science, and the Canadian Light Source. Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

doi = "10.1021/jacs.3c01818",

language = "English",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

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T1 - A Manganese Compound I Model with a High Reactivity in the Oxidation of Organic Substrates and Water

AU - Zhang, Lina

AU - Seo, Mi Sook

AU - Choi, Yunhee

AU - Ezhov, Roman

AU - Maximova, Olga

AU - Malik, Deesha D.

AU - Ng, Maggie

AU - Lee, Yong Min

AU - Sarangi, Ritimukta

AU - Pushkar, Yulia N.

AU - Cho, Kyung Bin

AU - Nam, Wonwoo

N1 - Funding Information: This work was supported by the NRF of Korea (NRF-2021R1A3B1076539 to W.N., NRF-2020R1I1A1A01074630 to Y.-M.L., and NRF-2021R1A2C1012851 to K.-B.C). This research was also supported by NSF CHE-2004147 to Y.P. The use of the Advanced Photon Source, an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract DE-AC02- 06CH11357. The PNC/XSD (Sector 20) facilities at the Advanced Photon Source and research at these facilities were supported by the U.S. Department of Energy, Basic Energy Science, and the Canadian Light Source. Publisher Copyright: © 2023 American Chemical Society.

PY - 2023

Y1 - 2023

N2 - A high-valent manganese(IV)-hydroxo porphyrin π-cation radical complex, [Mn(IV)(OH)(Porp+•)(X)]+, was synthesized and characterized spectroscopically. The Mn porphyrin intermediate was highly reactive in alkane hydroxylation and oxygen atom transfer reactions. More importantly, the Mn porphyrin intermediate reacted with water at a fast rate, resulting in the dioxygen evolution. To the best of our knowledge, we report the first manganese Cpd I model compound bearing a porphyrin π-cation radical ligand with a high reactivity in oxidation reactions, including water oxidation.

AB - A high-valent manganese(IV)-hydroxo porphyrin π-cation radical complex, [Mn(IV)(OH)(Porp+•)(X)]+, was synthesized and characterized spectroscopically. The Mn porphyrin intermediate was highly reactive in alkane hydroxylation and oxygen atom transfer reactions. More importantly, the Mn porphyrin intermediate reacted with water at a fast rate, resulting in the dioxygen evolution. To the best of our knowledge, we report the first manganese Cpd I model compound bearing a porphyrin π-cation radical ligand with a high reactivity in oxidation reactions, including water oxidation.

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DO - 10.1021/jacs.3c01818

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SN - 0002-7863

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

ER -

A Manganese Compound I Model with a High Reactivity in the Oxidation of Organic Substrates and Water

Abstract

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