Solubility and Thermodynamic Parameters of H2S/CH4 in Ionic Liquids Determined by 1H NMR

ACS Omega. 2024 Jan 8;9(3):3588-3595. doi: 10.1021/acsomega.3c07594. eCollection 2024 Jan 23.

Abstract

Natural gas remains an important global source of energy. Usually, sour gas from the well or refinery stream contains H2S among other contaminants that should be removed to fulfill permissible standards of use. Despite the use of different gas-liquid sour gas upgrading technologies, ionic liquids (ILs) have been recognized as promising materials to remove H2S from sour gas. However, data concerned with thermodynamic solution functions of H2S in ILs have scarcely been reported in the literature. In this work, solution 1H NMR spectroscopy was employed for quantifying H2S soluble in [BMIM][Cl] and for gaining a better understanding of the H2S-IL interaction. Experiments were carried out in a Young-Tap NMR tube containing a saturated solution of H2S/CH4/[BMIM][Cl] and recording spectra from 298 to 333 K. The thermodynamic solution functions, determined from the Van't Hoff equation, showed that solubility of the H2S in the [BMIM][Cl] is an exothermic gas-liquid physisorption process (Δsol = -66.13 kJmol-1) with a negative entropy change (Δsol = -168.19 JK-1 mol-1). 1H NMR spectra of the H2S/[BMIM][Cl] solution show a feature of strong solute-solvent interactions. However, solubility enthalpy is a fifth of the H-S bond energy value. Results from 1H NMR spectroscopy also agree with those from the bench dynamic experiments.