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Published on: August 13, 2019

Bi-layering at ionic liquid surfaces: a sum-frequency generation vibrational spectroscopy- and molecular dynamics

Takashi Iwahashi¹, Tatsuya Ishiyama², Yasunari Sakai¹

¹Department of Materials Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, O-okayama, Meguro-ku, Tokyo, 152-8552, Japan. ouchi.y.ab@m.titech.ac.jp.

Physical Chemistry Chemical Physics : PCCP

|May 27, 2020

Summary

Room-temperature ionic liquids exhibit a distinct bi-layered surface structure. This finding, revealed by spectroscopy and simulations, is crucial for designing and applying these versatile solvents.

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Published on: December 1, 2023

Area of Science:

Materials Science
Physical Chemistry
Chemical Engineering

Background:

Room-temperature ionic liquids (RTILs) are versatile solvents gaining traction in chemical engineering, electrochemistry, and synthetic chemistry.
Understanding the surface layer structure of RTILs is critical for expanding their application potential.
Previous studies have hinted at complex surface phenomena in RTILs, necessitating detailed structural investigation.

Purpose of the Study:

To elucidate the bi-layering phenomenon at the surfaces of 1-alkyl-3-methylimidazolium ([C_nmim]⁺) and bis(trifluoromethanesulfonyl)amide ([TFSA]^-) ionic liquids.
To investigate the influence of alkyl chain length on the surface structure and vibrational properties of RTILs.
To provide insights into the molecular arrangements and interactions governing RTIL surface behavior.

Main Methods:

Infrared-visible sum-frequency generation (IV-SFG) vibrational spectroscopy was employed to probe the surface molecular structure.
Molecular dynamics (MD) simulations were utilized to model and analyze the RTIL surface and bulk structures.
Analysis focused on the vibrational signals of [TFSA]^- anions and the r⁺ mode of [C_nmim]⁺ cations.

Main Results:

A distinct bi-layered structure was identified at the RTIL surfaces, featuring a 'head-to-head' molecular arrangement.
The sum-frequency (SF) signal from [TFSA]^- anions decreased with increasing alkyl chain length of the cations.
The SF signal from the r⁺ mode of [C_nmim]⁺ cations remained consistent across different alkyl chain lengths.

Conclusions:

The observed decrease in [TFSA]^- SF signals is attributed to destructive interference between the two layers.
The r⁺ mode of [C_nmim]⁺ is less affected by destructive interference due to minimal peak shift between surface and bulk.
The findings suggest that bi-layered structures are common in RTILs, impacting their surface properties and requiring consideration in future applications.