Kinetic measurements and in situ Raman spectroscopy study of the formation of TBAF semi-hydrates with hydrogen and carbon dioxide

• Published in: International journal of hydrogen energy Vol. 38; no. 18; pp. 7326 - 7334
• Main Authors: Trueba, Alondra Torres, Radović, Ivona R., Zevenbergen, John F., Peters, Cor J., Kroon, Maaike C.
• Format: Journal Article
• Language: English
• Published: Kidlington Elsevier Ltd 18.06.2013; Elsevier
• Subjects: Alternative fuels. Production and utilization; Applied sciences; Carbon capture and storage; Carbon dioxide; Energy; Exact sciences and technology; Fuels; Hydrates; Hydrogen; Hydrogen storage; Hydrogen-based energy; In situ Raman spectroscopy; Kinetic measurements; Nucleation; Raman spectroscopy; Semi-hydrate; Tetra n-butyl ammonium fluoride; Uptakes; Tetra n-butyl ammonium fluoride; Semi-hydrate; Kinetic measurements; Hydrogen; In situ Raman spectroscopy; Carbon dioxide; Measurement; Kinetics
• ISSN: 0360-3199; 1879-3487
• DOI: 10.1016/j.ijhydene.2013.03.154

The kinetics of formation of semi-clathrate hydrates of tetra n-butyl ammonium fluoride (TBAF) with hydrogen (H2) and carbon dioxide (CO2) were studied in order to elucidate their potential for H2 storage as well as for CO2 sequestration. The influence of pressure, TBAF concentration (1.8 mol% and 3.4 mol%) and formation method (T-cycle method and T-constant method) on the hydrate nucleation, hydrate growth and the amount of gas uptake were determined. The results showed that the kinetics of formation of H2–TBAF semi-hydrates is favored at high pressures and TBAF concentrations. The TBAF concentration did not display a large influence on the kinetics of formation of CO2–TBAF semi-hydrates and pressure only showed a major influence on the formation rate. Instead, the induction time and the amount of CO2 consumed were favored at low temperatures. Additionally, in situ Raman spectroscopy was used to confirm the gas uptake in the hydrate structure and to observe structural changes. •The kinetics of formation of H2–TBAF and CO2–TBAF semi-hydrates were studied.•The kinetics of formation of H2–TBAF semi-hydrates are favored at high pressures and solute concentrations.•The solute concentration did not have a large influence on the kinetics of formation of CO2–TBAF semi-hydrates.•Semi-hydrates technology has the potential to be applied in novel H2/CO2 separation technologies.