Abstract
Hydrogen is targeted to have a significant influence on the energy mix in the upcoming years. Its underground injection is an efficient solution for large-scale and long-term storage. Furthermore, natural hydrogen emissions have been proven in several locations of the world, and the potential underground accumulations constitute exciting carbon-free energy sources. In this context, comprehensive models are necessary to better constrain hydrogen behavior in geological formations. In particular, solubility in brines is a key-parameter, as it directly impacts hydrogen reactivity and migration in porous media. In this work, Monte Carlo simulations have been carried out to generate new simulated data of hydrogen solubility in aqueous NaCl solutions in temperature and salinity ranges of interest for geological applications, and for which no experimental data are currently available. For these simulations, molecular models have been selected for hydrogen, water and Na+and Cl−to reproduce phase properties of pure components and brine densities. To model solvent-solutes and solutes-solutes interactions, it was shown that the Lorentz-Berthelot mixing rules with a constant interaction binary parameter are the most appropriate to reproduce the experimental hydrogen Henry constants in salted water. With this force field, simulation results match measured solubilities with an average deviation of 6%. Additionally, simulation reproduced the expected behaviors of the H2O + H2 + NaCl system, such as the salting-out effect, a minimum hydrogen solubility close to 57 °C, and a decrease of the Henry constant with increasing temperature. The force field was then used in extrapolation to determine hydrogen Henry constants for temperatures up to 300 °C and salinities up to 2 mol/kgH2O. Using the experimental measures and these new simulated data generated by molecular simulation, a binary interaction parameter of the Soreide and Whiston equation of state has been fitted. The obtained model allows fast and reliable phase equilibrium calculations, and it was applied to illustrative cases relevant for hydrogen geological storage or H2natural emissions.
Highlights
Hydrogen (H2) is currently taking an increasing role in the energy mix
The Lorentz-Berthelot combining rules are definitively adopted for this study. We emphasis that this choice is motivated only on hydrogen solubility considerations, which is the focus of this work
Monte Carlo simulations have been carried out to generate new simulated data of hydrogen solubility in aqueous NaCl solutions in temperature and salinity ranges of interest for geological applications, and for which no experimental data are currently available
Summary
Hydrogen (H2) is currently taking an increasing role in the energy mix. First pilot projects are taking place and use electrolyzers to convert solar- and wind-farm electricity to H2 which is stored (Darras et al, 2012; Perez et al, 2016). It can be converted again to electricity (such as the Methycentre project [ADEME, 2018]), injected in the natural gas network (such as the Grhyd project in Dunkerque, France [ENGIE, 2018]) or used as fuel for vehicles. The development of a large-scale use of hydrogen implies increasing storage needs, and injection in geological formations, used extensively in the gas and compressed air energy industries, is an attractive solution to reach sizable storage volumes (Lord et al, 2014). Various options that already proved their efficiency and economic viability for other gases, such as injection in aquifers, depleted oil and gas fields, and salt caverns, are currently under study (Le Duigou et al, 2017)
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