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Title: In situ redox reactions facilitate the assembly of a mixed-valence metal-organic nanocapsule

Abstract

C-alkylpyrogallol[4]arenes (PgCs) have been studied for their ability to form metal-organic nanocapsules (MONCs) through coordination to appropriate metal ions. Here we present the synthesis and characterization of an Mn II/Mn III-seamed MONC in addition to its electrochemical and magnetic behavior. This MONC assembles from 24 manganese ions and 6 PgCs, while an additional metal ion is located on the capsule interior, anchored through the introduction of bridging nitrite ions. The latter originate from an in situ redox reaction that occurs during the self-assembly process, thus representing a new route to otherwise unobtainable nanocapsules.

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of Missouri, Columbia, MO (United States)
  2. Univ. of Edinburgh, Scotland (United Kingdom)
  3. Heriot-Watt Univ., Edinburgh, Scotland (United Kingdom)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1571128
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Rathnayake, Asanka S., Fraser, Hector W. L., Brechin, Euan K., Dalgarno, Scott J., Baumeister, Jakob E., White, Joshua, Rungthanaphatsophon, Pokpong, Walensky, Justin R., Barnes, Charles L., Teat, Simon J., and Atwood, Jerry L. In situ redox reactions facilitate the assembly of a mixed-valence metal-organic nanocapsule. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04541-w.
Rathnayake, Asanka S., Fraser, Hector W. L., Brechin, Euan K., Dalgarno, Scott J., Baumeister, Jakob E., White, Joshua, Rungthanaphatsophon, Pokpong, Walensky, Justin R., Barnes, Charles L., Teat, Simon J., & Atwood, Jerry L. In situ redox reactions facilitate the assembly of a mixed-valence metal-organic nanocapsule. United States. doi:10.1038/s41467-018-04541-w.
Rathnayake, Asanka S., Fraser, Hector W. L., Brechin, Euan K., Dalgarno, Scott J., Baumeister, Jakob E., White, Joshua, Rungthanaphatsophon, Pokpong, Walensky, Justin R., Barnes, Charles L., Teat, Simon J., and Atwood, Jerry L. Tue . "In situ redox reactions facilitate the assembly of a mixed-valence metal-organic nanocapsule". United States. doi:10.1038/s41467-018-04541-w. https://www.osti.gov/servlets/purl/1571128.
@article{osti_1571128,
title = {In situ redox reactions facilitate the assembly of a mixed-valence metal-organic nanocapsule},
author = {Rathnayake, Asanka S. and Fraser, Hector W. L. and Brechin, Euan K. and Dalgarno, Scott J. and Baumeister, Jakob E. and White, Joshua and Rungthanaphatsophon, Pokpong and Walensky, Justin R. and Barnes, Charles L. and Teat, Simon J. and Atwood, Jerry L.},
abstractNote = {C-alkylpyrogallol[4]arenes (PgCs) have been studied for their ability to form metal-organic nanocapsules (MONCs) through coordination to appropriate metal ions. Here we present the synthesis and characterization of an MnII/MnIII-seamed MONC in addition to its electrochemical and magnetic behavior. This MONC assembles from 24 manganese ions and 6 PgCs, while an additional metal ion is located on the capsule interior, anchored through the introduction of bridging nitrite ions. The latter originate from an in situ redox reaction that occurs during the self-assembly process, thus representing a new route to otherwise unobtainable nanocapsules.},
doi = {10.1038/s41467-018-04541-w},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 3 works
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    Works referencing / citing this record:

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    journal, September 1978


    Single-Molecule Magnets
    journal, November 2000

    • Christou, George; Gatteschi, Dante; Hendrickson, David N.
    • MRS Bulletin, Vol. 25, Issue 11
    • DOI: 10.1557/mrs2000.226

    Supramolecular blueprint approach to metal-coordinated capsules
    journal, April 2005

    • McKinlay, R. M.; Cave, G. W. V.; Atwood, J. L.
    • Proceedings of the National Academy of Sciences, Vol. 102, Issue 17
    • DOI: 10.1073/pnas.0408113102

    Mixed-Valent Mn Supertetrahedra and Planar Discs as Enhanced Magnetic Coolers
    journal, August 2008

    • Manoli, Maria; Collins, Anna; Parsons, Simon
    • Journal of the American Chemical Society, Vol. 130, Issue 33
    • DOI: 10.1021/ja802829d

    Possible Intermediates in Biological Metalloporphyrin Oxidative Degradation. Nickel, Copper, and Cobalt Complexes of Octaethylformybiliverdin and Their Conversion to a Verdoheme
    journal, February 1998

    • Koerner, Richard; Olmstead, Marilyn M.; Ozarowski, Andrzej
    • Journal of the American Chemical Society, Vol. 120, Issue 6
    • DOI: 10.1021/ja973088y

    A Mixed-Valence Manganese Cubane Trapped by Inequivalent Trilacunary Polyoxometalate Ligands
    journal, August 2011

    • Mitchell, Scott G.; Molina, Pedro I.; Khanra, Sumit
    • Angewandte Chemie International Edition, Vol. 50, Issue 39
    • DOI: 10.1002/anie.201102727

    Mixed metal-organic nanocapsules
    journal, August 2010

    • Jin, Ping; Dalgarno, Scott J.; Atwood, Jerry L.
    • Coordination Chemistry Reviews, Vol. 254, Issue 15-16
    • DOI: 10.1016/j.ccr.2010.04.009

    Synthesis, Structure, and Magnetic Properties of a Large Lanthanide–Transition-Metal Single-Molecule Magnet
    journal, July 2004

    • Zaleski, Curtis M.; Depperman, Ezra C.; Kampf, Jeff W.
    • Angewandte Chemie International Edition, Vol. 43, Issue 30
    • DOI: 10.1002/anie.200454013

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    • Piela, Barbara; Wrona, Piotr K.
    • Journal of The Electrochemical Society, Vol. 149, Issue 2
    • DOI: 10.1149/1.1433751

    Metallo-supramolecular capsules
    journal, April 2008

    • Dalgarno, Scott J.; Power, Nicholas P.; Atwood, Jerry L.
    • Coordination Chemistry Reviews, Vol. 252, Issue 8-9
    • DOI: 10.1016/j.ccr.2007.10.010

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    • Ritchie, Chris; Ferguson, Alan; Nojiri, Hiroyuki
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    • Bioorganic & Medicinal Chemistry, Vol. 16, Issue 13
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    • Mukhopadhyay, Sumitra; Mandal, Sanjay K.; Bhaduri, Sumit
    • Chemical Reviews, Vol. 104, Issue 9
    • DOI: 10.1021/cr0206014

    Design of functional metalloproteins
    journal, August 2009

    • Lu, Yi; Yeung, Natasha; Sieracki, Nathan
    • Nature, Vol. 460, Issue 7257
    • DOI: 10.1038/nature08304

    Electrochemical Oxidation of Nitrite and the Oxidation and Reduction of NO 2 in the Room Temperature Ionic Liquid [C 2 mim][NTf 2 ]
    journal, July 2007

    • Broder, Tessa L.; Silvester, Debbie S.; Aldous, Leigh
    • The Journal of Physical Chemistry B, Vol. 111, Issue 27
    • DOI: 10.1021/jp0728104

    Novel Zinc Porphyrin Sensitizers for Dye-Sensitized Solar Cells: Synthesis and Spectral, Electrochemical, and Photovoltaic Properties
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    Albumin-Conjugated Corrole Metal Complexes:  Extremely Simple Yet Very Efficient Biomimetic Oxidation Systems
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    • Journal of the American Chemical Society, Vol. 127, Issue 9
    • DOI: 10.1021/ja045372c

    Investigating Reaction Conditions To Control the Self-Assembly of Cobalt-Seamed Nanocapsules
    journal, May 2016

    • Rathnayake, Asanka S.; Feaster, Kyle A.; White, Joshua
    • Crystal Growth & Design, Vol. 16, Issue 7
    • DOI: 10.1021/acs.cgd.6b00306

    Energy conversion catalysis using semiconducting transition metal cluster compounds
    journal, October 1986

    • Vante, N. Alonso; Tributsch, H.
    • Nature, Vol. 323, Issue 6087
    • DOI: 10.1038/323431a0

    Calixarene-supported clusters: employment of complementary cluster ligands for the construction of a ferromagnetic [Mn5] cage
    journal, January 2012

    • Taylor, Stephanie M.; McIntosh, Ruaraidh D.; Piligkos, Stergios
    • Chemical Communications, Vol. 48, Issue 91
    • DOI: 10.1039/c2cc35944h

    Self-assembled biomimetic [2Fe2S]-hydrogenase-based photocatalyst for molecular hydrogen evolution
    journal, January 2009

    • Kluwer, A. M.; Kapre, R.; Hartl, F.
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    • DOI: 10.1073/pnas.0809666106

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    • Sessoli, Roberta; Tsai, Hui Lien; Schake, Ann R.
    • Journal of the American Chemical Society, Vol. 115, Issue 5
    • DOI: 10.1021/ja00058a027

    Nitrate-dependent iron(II) oxidation in paddy soil
    journal, February 2001


    Biological polynuclear clusters coupled by magnetic interactions: From the point dipole approximation to a local spin model
    journal, April 1994

    • Bertrand, Patrick; More, Claude; Guigliarelli, Bruno
    • Journal of the American Chemical Society, Vol. 116, Issue 7
    • DOI: 10.1021/ja00086a042

    The manganese complex of photosystem II in its reaction cycle—Basic framework and possible realization at the atomic level
    journal, February 2008


    Zinc(II)-Directed Self-Assembly of Metal–Organic Nanocapsules
    journal, August 2017

    • Rathnayake, Asanka S.; Barnes, Charles L.; Atwood, Jerry L.
    • Crystal Growth & Design, Vol. 17, Issue 9
    • DOI: 10.1021/acs.cgd.7b00597

    Coordination Polymer Chains of Dimeric Pyrogallol[4]arene Capsules
    journal, July 2011

    • Fowler, Drew A.; Mossine, Andrew V.; Beavers, Christine M.
    • Journal of the American Chemical Society, Vol. 133, Issue 29
    • DOI: 10.1021/ja203651v