Abstract

There are surging demands to separate carbon dioxide from methane in upgrading low-quality natural gas including biogas with an energy efficient process. In this work, adsorption equilibria and kinetics of CO2 and CH4 on a zeolitic imidazolate framework ZIF-7 were determined at various temperatures and gas pressures up to 1bar, to evaluate the feasibility of removing CO2 from CH4 in a vacuum swing adsorption process using ZIF-7 as adsorbent. The as-synthesized ZIF-7 sample was characterized with scanning electron microscopy for crystal structure, powder X-ray diffraction for phase structure, thermal gravimetric analysis for thermal stability, and carbon dioxide adsorption at 0°C for pore textural properties. To study the gate-opening of ZIF-7, CO2 adsorption was measured at five different temperatures (273, 298, 323, 348 and 373K) and pressures up to 10bar. A thermodynamic model was employed to estimate the free energy of phase transition between narrow pore and large pore, and a modified dual-site Sips equation could fit the S shape CO2 isotherms well. Adsorption equilibrium selectivity (α) and adsorbent selection parameter for pressure swing adsorption processes (S) were calculated from the adsorption equilibrium data. The relatively high values of adsorption selectivities suggest that ZIF-7 is a promising adsorbent candidate for CO2/CH4 separation in a pressure swing adsorption process.

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