Stability of water-stable C60 clusters to OH radical oxidation and hydrated electron reduction

Jaesang Lee; Weihua Song; Seung S. Jang; John D. Fortner; Pedro J.J. Alvarez; William J. Cooper; Jae Hong Kim

doi:10.1021/es903550e

Stability of water-stable C₆₀ clusters to OH radical oxidation and hydrated electron reduction

Jaesang Lee, Weihua Song, Seung S. Jang, John D. Fortner, Pedro J.J. Alvarez, William J. Cooper, Jae Hong Kim

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

29 Citations (Scopus)

Abstract

Reactions of water-stable C₆₀ clusters (nC₆₀) in water with OH radicals (•OH) and hydrated electrons (e_aq ^-), generated by steady-state γ-radiation, were observed and characterized. Ordered C₆₀ clusters were relatively recalcitrant to highly reactive •OH and e_aq^- species, with only a fraction of carbons oxidized and reduced, respectively. Pulse radiolysis suggested that the reactions of nC₆₀ with OH• and e _aq^- were diffusion limited, with rate constants of (7.34 ± 0.31) - 10⁹ M^-1 s^-1 and (2.34 ± 0.02) - 10¹⁰ M^-1 s^-1, respectively. Quantum mechanical calculations of binding energy of the C₆₀-OH adduct as a function of C₆₀ clustering degree indicate, despite an initial fast reaction, a slower overall conversion due to thermodynamic instability of C ₆₀-OH intermediates. The results imply that ordered clustering of C₆₀ in the aqueous phase significantly hinders C₆₀s fundamental reactivity with radical species.

Original language	English
Pages (from-to)	3786-3792
Number of pages	7
Journal	Environmental Science and Technology
Volume	44
Issue number	10
DOIs	https://doi.org/10.1021/es903550e
Publication status	Published - 2010 May 15
Externally published	Yes

ASJC Scopus subject areas

Chemistry(all)
Environmental Chemistry

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title = "Stability of water-stable C60 clusters to OH radical oxidation and hydrated electron reduction",

abstract = "Reactions of water-stable C60 clusters (nC60) in water with OH radicals (•OH) and hydrated electrons (eaq -), generated by steady-state γ-radiation, were observed and characterized. Ordered C60 clusters were relatively recalcitrant to highly reactive •OH and eaq- species, with only a fraction of carbons oxidized and reduced, respectively. Pulse radiolysis suggested that the reactions of nC60 with OH• and e aq- were diffusion limited, with rate constants of (7.34 ± 0.31) - 109 M-1 s-1 and (2.34 ± 0.02) - 1010 M-1 s-1, respectively. Quantum mechanical calculations of binding energy of the C60-OH adduct as a function of C60 clustering degree indicate, despite an initial fast reaction, a slower overall conversion due to thermodynamic instability of C 60-OH intermediates. The results imply that ordered clustering of C60 in the aqueous phase significantly hinders C60s fundamental reactivity with radical species.",

author = "Jaesang Lee and Weihua Song and Jang, {Seung S.} and Fortner, {John D.} and Alvarez, {Pedro J.J.} and Cooper, {William J.} and Kim, {Jae Hong}",

year = "2010",

month = may,

day = "15",

doi = "10.1021/es903550e",

language = "English",

volume = "44",

pages = "3786--3792",

journal = "Environmental Science and Technology",

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publisher = "American Chemical Society",

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TY - JOUR

T1 - Stability of water-stable C60 clusters to OH radical oxidation and hydrated electron reduction

AU - Lee, Jaesang

AU - Song, Weihua

AU - Jang, Seung S.

AU - Fortner, John D.

AU - Alvarez, Pedro J.J.

AU - Cooper, William J.

AU - Kim, Jae Hong

PY - 2010/5/15

Y1 - 2010/5/15

N2 - Reactions of water-stable C60 clusters (nC60) in water with OH radicals (•OH) and hydrated electrons (eaq -), generated by steady-state γ-radiation, were observed and characterized. Ordered C60 clusters were relatively recalcitrant to highly reactive •OH and eaq- species, with only a fraction of carbons oxidized and reduced, respectively. Pulse radiolysis suggested that the reactions of nC60 with OH• and e aq- were diffusion limited, with rate constants of (7.34 ± 0.31) - 109 M-1 s-1 and (2.34 ± 0.02) - 1010 M-1 s-1, respectively. Quantum mechanical calculations of binding energy of the C60-OH adduct as a function of C60 clustering degree indicate, despite an initial fast reaction, a slower overall conversion due to thermodynamic instability of C 60-OH intermediates. The results imply that ordered clustering of C60 in the aqueous phase significantly hinders C60s fundamental reactivity with radical species.

AB - Reactions of water-stable C60 clusters (nC60) in water with OH radicals (•OH) and hydrated electrons (eaq -), generated by steady-state γ-radiation, were observed and characterized. Ordered C60 clusters were relatively recalcitrant to highly reactive •OH and eaq- species, with only a fraction of carbons oxidized and reduced, respectively. Pulse radiolysis suggested that the reactions of nC60 with OH• and e aq- were diffusion limited, with rate constants of (7.34 ± 0.31) - 109 M-1 s-1 and (2.34 ± 0.02) - 1010 M-1 s-1, respectively. Quantum mechanical calculations of binding energy of the C60-OH adduct as a function of C60 clustering degree indicate, despite an initial fast reaction, a slower overall conversion due to thermodynamic instability of C 60-OH intermediates. The results imply that ordered clustering of C60 in the aqueous phase significantly hinders C60s fundamental reactivity with radical species.

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SN - 0013-936X

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JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 10

ER -

Stability of water-stable C₆₀ clusters to OH radical oxidation and hydrated electron reduction

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