Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer

J. Rooze, R. Groote, R.T.M. Jakobs, R.P. Sijbesma, M.M. Van Iersel, Evgeny Rebrov, J.C. Schouten, J.T.F. Keurentjes

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Scission of a supramolecular polymer-metal complex can be carried out using collapsing cavitation bubbles created by ultrasound. Although the most plausible scission mechanism of the coordinative bonds is through mechanical force, the influence of radicals and high hot-spot temperatures on scission has to be considered. A silver(I)-N-heterocyclic carbene complex was exposed to 20 kHz ultrasound in argon, nitrogen, methane, and isobutane saturated toluene. Scission percentages were almost equal under argon, nitrogen, and methane. Radical production differs by a factor of 10 under these gases, indicating that radical production is not a significant contributor to the scission process. A model to describe the displacement of the bubble wall, strain rates, and temperature in the gas shows that critical strain rates for coil-to-stretch transition, needed for scission, are achieved at reactor temperatures of 298 K, an acoustic pressure of 1.2 x 10(5) Pa, and an acoustic frequency of 20 kHz. Lower scission percentages were measured under isobutane, which also shows lower strain rates in model simulations. The activation of the polymer-metal complexes in toluene under the influence of ultrasound occurs through mechanical force.
Original languageEnglish
Pages (from-to)11038-11043
Number of pages6
JournalJournal of Physical Chemistry B
Volume115
Issue number38
DOIs
Publication statusPublished - 29 Sep 2011

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carbenes
Butanes
coordination polymers
Silver
Strain rate
cleavage
Polymers
Argon
Ultrasonics
Coordination Complexes
silver
Methane
Toluene
Metal complexes
Nitrogen
Gases
Acoustics
strain rate
Bubbles (in fluids)
Cavitation

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Rooze, J., Groote, R., Jakobs, R. T. M., Sijbesma, R. P., Van Iersel, M. M., Rebrov, E., ... Keurentjes, J. T. F. (2011). Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer. Journal of Physical Chemistry B, 115(38), 11038-11043. https://doi.org/10.1021/jp203780a
Rooze, J. ; Groote, R. ; Jakobs, R.T.M. ; Sijbesma, R.P. ; Van Iersel, M.M. ; Rebrov, Evgeny ; Schouten, J.C. ; Keurentjes, J.T.F. / Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer. In: Journal of Physical Chemistry B. 2011 ; Vol. 115, No. 38. pp. 11038-11043.
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Rooze, J, Groote, R, Jakobs, RTM, Sijbesma, RP, Van Iersel, MM, Rebrov, E, Schouten, JC & Keurentjes, JTF 2011, 'Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer', Journal of Physical Chemistry B, vol. 115, no. 38, pp. 11038-11043. https://doi.org/10.1021/jp203780a

Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer. / Rooze, J.; Groote, R.; Jakobs, R.T.M.; Sijbesma, R.P.; Van Iersel, M.M.; Rebrov, Evgeny; Schouten, J.C.; Keurentjes, J.T.F.

In: Journal of Physical Chemistry B, Vol. 115, No. 38, 29.09.2011, p. 11038-11043.

Research output: Contribution to journalArticle

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T1 - Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer

AU - Rooze, J.

AU - Groote, R.

AU - Jakobs, R.T.M.

AU - Sijbesma, R.P.

AU - Van Iersel, M.M.

AU - Rebrov, Evgeny

AU - Schouten, J.C.

AU - Keurentjes, J.T.F.

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Y1 - 2011/9/29

N2 - Scission of a supramolecular polymer-metal complex can be carried out using collapsing cavitation bubbles created by ultrasound. Although the most plausible scission mechanism of the coordinative bonds is through mechanical force, the influence of radicals and high hot-spot temperatures on scission has to be considered. A silver(I)-N-heterocyclic carbene complex was exposed to 20 kHz ultrasound in argon, nitrogen, methane, and isobutane saturated toluene. Scission percentages were almost equal under argon, nitrogen, and methane. Radical production differs by a factor of 10 under these gases, indicating that radical production is not a significant contributor to the scission process. A model to describe the displacement of the bubble wall, strain rates, and temperature in the gas shows that critical strain rates for coil-to-stretch transition, needed for scission, are achieved at reactor temperatures of 298 K, an acoustic pressure of 1.2 x 10(5) Pa, and an acoustic frequency of 20 kHz. Lower scission percentages were measured under isobutane, which also shows lower strain rates in model simulations. The activation of the polymer-metal complexes in toluene under the influence of ultrasound occurs through mechanical force.

AB - Scission of a supramolecular polymer-metal complex can be carried out using collapsing cavitation bubbles created by ultrasound. Although the most plausible scission mechanism of the coordinative bonds is through mechanical force, the influence of radicals and high hot-spot temperatures on scission has to be considered. A silver(I)-N-heterocyclic carbene complex was exposed to 20 kHz ultrasound in argon, nitrogen, methane, and isobutane saturated toluene. Scission percentages were almost equal under argon, nitrogen, and methane. Radical production differs by a factor of 10 under these gases, indicating that radical production is not a significant contributor to the scission process. A model to describe the displacement of the bubble wall, strain rates, and temperature in the gas shows that critical strain rates for coil-to-stretch transition, needed for scission, are achieved at reactor temperatures of 298 K, an acoustic pressure of 1.2 x 10(5) Pa, and an acoustic frequency of 20 kHz. Lower scission percentages were measured under isobutane, which also shows lower strain rates in model simulations. The activation of the polymer-metal complexes in toluene under the influence of ultrasound occurs through mechanical force.

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ER -

Rooze J, Groote R, Jakobs RTM, Sijbesma RP, Van Iersel MM, Rebrov E et al. Mechanism of Ultrasound Scission of a Silver-Carbene Coordination Polymer. Journal of Physical Chemistry B. 2011 Sep 29;115(38):11038-11043. https://doi.org/10.1021/jp203780a