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DOE OSTI · 2475862

Secondary electron emission measurements from imidazolium-based ionic liquids

Capece, A. M.·Enriquez, A. N.
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Abstract

The electron-induced secondary electron emission (SEE) yields of imidazolium-based ionic liquids are presented for primary electron beam energies between 30 and 1000 eV. These results are important for understanding plasma synthesis of nanoparticles in plasma discharges with an ionic liquid electrode. Due to their low vapor pressure and high conductivity, ionic liquids can produce metal nanoparticles in low-pressure plasmas through reduction of dissolved metal salts. In this work, the low vapor pressure of ionic liquids is exploited to directly measure SEE yields by bombarding the liquid with electrons and measuring the resulting currents. The ionic liquids studied are [BMIM][Ac], [EMIM][Ac], and [BMIM][BF 4 ]. The SEE yields vary significantly over the energy range, with maximum yields of around 2 at 200 eV for [BMIM][Ac] and [EMIM][Ac], and 1.8 at 250 eV for [BMIM][BF 4 ]. Molecular orbital calculations indicate that the acetate anion is the likely electron donor for [BMIM][Ac] and [EMIM][Ac], while in [BMIM][BF 4 ], the electrons likely originate from the [BMIM] + cation. The differences in SEE yields are attributed to varying ionization potentials and molecular structures of the ionic liquids. These findings are essential for accurate modeling of plasma discharges and understanding SEE mechanisms in ionic liquids.

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ionic liquidsnanoparticle synthesissecondary electron emission

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Capece, A. M., Enriquez, A. N.. 2024-11-01. Secondary electron emission measurements from imidazolium-based ionic liquids. https://doi.org/10.1088/1361-6463%2Fad89d7

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NASA NTRS2014

Investigation of Structure and Transport in Li-Doped Ionic Liquid Electrolytes: [pyr14][TFSI], [pyr13][FSI], [EMIM][BF4]

Ionic liquid electrolytes have been proposed as a means of improving the safety and cycling behavior of advanced lithium batteries; however, the properties of these electrolytes under high lithium doping are poorly understood. Here, we employ both polarizable molecular dynamics simulation and experiment to investigate the structure, thermodynamics and transport of three potential electrolytes, N-methyl-N-butylpyrrolidinium bis(trifluoromethylsufonyl)imide ([pyr14][TFSI]), N- methyl-N-propylpyrrolidinium bis(fluorosufonyl)imide ([pyr13][FSI]), and 1-ethyl-3-- methylimidazolium boron tetrafluoride ([EMIM][BF4]), as a function of Li (-) salt concentration and temperature. Structurally, Li(+) is shown to be solvated by three anion neighbors in [pyr14][TFSI] and four anion neighbors in both [pyr13][FSI] and [EMIM][BF4], and at all levels of xLi we find the presence of lithium aggregates. Furthermore, the computed density, diffusion, viscosity, and ionic conductivity show excellent agreement with experimental data. While the diffusion and viscosity exhibit a systematic decrease and increase, respectively, with increasing xLi, the contribution of Li(+) to ionic conductivity increases until reaching a saturation doping level of xLi 0.10. Comparatively, the Li(+) conductivity of [pyr14][TFSI] is an order of magnitude lower than that of the other liquids, which range between 0.1-0.3 mScm. The differences in Li(+) transport are reflected in the residence times of Li(+) with the anions, which are revealed to be much larger for [pyr14][TFSI] (up to 100 ns at the highest doping levels) than in either [EMIM][BF4] or [pyr13][FSI]. Finally, we comment on the relative kinetics of Li(+) transport in each liquid and we present strong evidence for transport through anion exchange (hopping) as opposed to the net motion of Li(+) with its solvation shell (vehicular).

ionic liquids↗