NDLI: Coumarin 153 Dynamics in Ethylammonium Nitrate: The Effects of Dilution with Methanol

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Coumarin 153 Dynamics in Ethylammonium Nitrate: The Effects of Dilution with Methanol

Content Provider	MDPI
Author	Heitz, Mark P. Sabo, Tyler J. Robillard, Stephanie M.
Copyright Year	2021
Abstract	Magic angle intensity decay and dynamic fluorescence anisotropy measurements were made on the binary solvent system composed of ethylammonium nitrate ([N_2,0,0,0⁺][NO₃⁻], EAN) + methanol (MeOH) across the complete EAN mole fraction range (x_IL = 0–1) using the neutral dipolar solute coumarin 153 (C153) at 295 K. Stokes–Einstein–Debye (SED) hydrodynamic theory was used as a model framework to assess the C153 rotational reorientation dynamics. Departure from stick SED prediction was observed (in contrast to literature reports that used cationic or anionic dyes) and indicated a significant influence of domain nanoheterogeneity on probe dynamics. Steady-state spectroscopy indicated minimal changes in spectral peak and width with mole fraction, except at x_IL = 0.3 where absorption widths decreased by ~170 cm⁻¹, signaling that C153 sensed a change in solution heterogeneity. Magic angle intensity decays corroborated the steady-state observation and the excited-state lifetimes showed a marked change from x_IL = 0.2–0.4 where EAN-EAN interactions became notably more significant. C153 average rotation times ( $⟨ τ_{r o t} ⟩$ ) showed significant solvent decoupling with increased EAN. The rotational data were fit to a power law dependence, $⟨ τ_{r o t} ⟩ \propto {(\frac{η}{T})}^{p}$ , where p = 0.82, demonstrating the presence of dynamic heterogeneity in the EAN/MeOH solutions. With increased EAN, rotation times showed that the heterogeneity became increasingly more significant since the rotation times systematically decreased away from the hydrodynamic stick limit.
Ending Page	795
Page Count	18
Starting Page	778
e-ISSN	26734079
DOI	10.3390/suschem2040041
Journal	Sustainable Chemistry
Issue Number	4
Volume Number	2
Language	English
Publisher	MDPI
Publisher Date	2021-12-20
Access Restriction	Open
Subject Keyword	Sustainable Chemistry Spectroscopy Ethylammonium Nitrate Ionic Liquid Coumarin 153 C153 Rotational Dynamics Sed Hydrodynamics
Content Type	Text
Resource Type	Article

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