Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules

Asanka S. Rathnayake; Hector W. L. Fraser; Euan K. Brechin; Scott J. Dalgarno; Jakob E. Baumeister; Pokpong Rungthanaphatsophon; Justin R. Walensky; Charles L. Barnes; Jerry L. Atwood

doi:10.1021/jacs.8b07775

Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules

Asanka S. Rathnayake, Hector W. L. Fraser, Euan K. Brechin, Scott J. Dalgarno, Jakob E. Baumeister, Pokpong Rungthanaphatsophon, Justin R. Walensky, Charles L. Barnes, Jerry L. Atwood^*

^*Corresponding author for this work

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

11 Citations (Scopus)

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Abstract

Two structurally analogous Mn-seamed C-alkylpyrogallol[4]arene (PgC_n)-based metal-organic nanocapsules (MONCs) have been synthesized under similar reaction conditions and characterized by crystallographic, electrochemical, and magnetic susceptibility techniques. Both MONCs contain 24 Mn centers, but, somewhat surprisingly, marked differences in oxidation state distribution are observed upon analysis. One MONC contains exclusively Mn^II ions, while the other is a mixed-valence Mn^II/ Mn^III assembly. We propose that these disparate oxidation state distributions arise from slight differences in pH achieved during synthesis, a factor that may lead to many spectacular new MONCs (and associated host-guest chemistries).

Original language	English
Pages (from-to)	13022–13027
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	140
Issue number	40
Early online date	14 Sept 2018
DOIs	https://doi.org/10.1021/jacs.8b07775
Publication status	Published - 10 Oct 2018

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.8b07775
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Rathnayake, A. S., Fraser, H. W. L., Brechin, E. K., Dalgarno, S. J., Baumeister, J. E., Rungthanaphatsophon, P., Walensky, J. R., Barnes, C. L., & Atwood, J. L. (2018). Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules. Journal of the American Chemical Society, 140(40), 13022–13027. https://doi.org/10.1021/jacs.8b07775

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title = "Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules",

abstract = "Two structurally analogous Mn-seamed C-alkylpyrogallol[4]arene (PgCn)-based metal-organic nanocapsules (MONCs) have been synthesized under similar reaction conditions and characterized by crystallographic, electrochemical, and magnetic susceptibility techniques. Both MONCs contain 24 Mn centers, but, somewhat surprisingly, marked differences in oxidation state distribution are observed upon analysis. One MONC contains exclusively MnII ions, while the other is a mixed-valence MnII/ MnIII assembly. We propose that these disparate oxidation state distributions arise from slight differences in pH achieved during synthesis, a factor that may lead to many spectacular new MONCs (and associated host-guest chemistries).",

author = "Rathnayake, {Asanka S.} and Fraser, {Hector W. L.} and Brechin, {Euan K.} and Dalgarno, {Scott J.} and Baumeister, {Jakob E.} and Pokpong Rungthanaphatsophon and Walensky, {Justin R.} and Barnes, {Charles L.} and Atwood, {Jerry L.}",

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doi = "10.1021/jacs.8b07775",

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Rathnayake, AS, Fraser, HWL, Brechin, EK, Dalgarno, SJ, Baumeister, JE, Rungthanaphatsophon, P, Walensky, JR, Barnes, CL & Atwood, JL 2018, 'Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules', Journal of the American Chemical Society, vol. 140, no. 40, pp. 13022–13027. https://doi.org/10.1021/jacs.8b07775

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T1 - Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules

AU - Rathnayake, Asanka S.

AU - Fraser, Hector W. L.

AU - Brechin, Euan K.

AU - Dalgarno, Scott J.

AU - Baumeister, Jakob E.

AU - Rungthanaphatsophon, Pokpong

AU - Walensky, Justin R.

AU - Barnes, Charles L.

AU - Atwood, Jerry L.

PY - 2018/10/10

Y1 - 2018/10/10

N2 - Two structurally analogous Mn-seamed C-alkylpyrogallol[4]arene (PgCn)-based metal-organic nanocapsules (MONCs) have been synthesized under similar reaction conditions and characterized by crystallographic, electrochemical, and magnetic susceptibility techniques. Both MONCs contain 24 Mn centers, but, somewhat surprisingly, marked differences in oxidation state distribution are observed upon analysis. One MONC contains exclusively MnII ions, while the other is a mixed-valence MnII/ MnIII assembly. We propose that these disparate oxidation state distributions arise from slight differences in pH achieved during synthesis, a factor that may lead to many spectacular new MONCs (and associated host-guest chemistries).

AB - Two structurally analogous Mn-seamed C-alkylpyrogallol[4]arene (PgCn)-based metal-organic nanocapsules (MONCs) have been synthesized under similar reaction conditions and characterized by crystallographic, electrochemical, and magnetic susceptibility techniques. Both MONCs contain 24 Mn centers, but, somewhat surprisingly, marked differences in oxidation state distribution are observed upon analysis. One MONC contains exclusively MnII ions, while the other is a mixed-valence MnII/ MnIII assembly. We propose that these disparate oxidation state distributions arise from slight differences in pH achieved during synthesis, a factor that may lead to many spectacular new MONCs (and associated host-guest chemistries).

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Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal-Organic Nanocapsules

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