Coupled gravimetric, manometric and calorimetric study of CO 2 , N 2 and CH 4 adsorption on zeolites for the assessment
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Coupled gravimetric, manometric and calorimetric study of CO2, N2 and CH4 adsorption on zeolites for the assessment of classical equilibrium models Alejandro Orsikowsky‑Sanchez1,2 · Frédéric Plantier2 · Christelle Miqueu2 Received: 3 September 2019 / Revised: 19 November 2019 / Accepted: 24 January 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract N2, CO2 and CH4 pure gas adsorption equilibria on five zeolites with different structural properties (Si/Al ratio, type of cations contained inside their structure, pore size and pore volume) have been measured over a wide range of pressures (from 10–5 to 80 bar) and temperatures (from 253 to 363 K) by combining high pressure gravimetric technique and high resolution low pressure manometry. These experimental data, coupled with the measurement of the differential heat of adsorption and with some literature information obtained with microscopic studies, have allowed to identify and to analyze the different adsorption mechanisms. The results show that CO2 adsorption mechanism is controlled by molecule–cation interactions at low pressures and by the pore volume filling at intermediate and high pressures. On the contrary, N 2 and C H4 adsorption mechanism is controlled by the pore volume filling in the whole range of pressures studied in this work. It is shown that the most popular models used in gas separation modeling such as Toth, Sips and bi-Langmuir do not describe the successive physico-chemical phenomena observed for the adsorption of CO2 on zeolites. Moreover, they are not able both to fit the whole range of experimental data and to predict the isosteric heat of adsorption accurately. Keywords Adsorption isotherm · Zeolites · Differential heat of adsorption · Adsorption modeling
1 Introduction Natural gas processing requires complex separation and purification operations involving expensive CAPEX (Capital Costs) and OPEX (Operational Costs) processes. The separation of C O2 is performed using adsorption, absorption or membranes strategies, for which significant expenses can arise related to the removal of impurities. In the case of low Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10450-020-00206-7) contains supplementary material, which is available to authorized users. * Alejandro Orsikowsky‑Sanchez [email protected] * Christelle Miqueu christelle.miqueu@univ‑pau.fr 1
TOTAL EP – Pôle d’Etudes et de Recherche de Lacq (PERL), BP 64170, Lacq, France
CNRS/TOTAL/UNIV PAU & PAYS ADOUR, Laboratoire Des Fluides Complexes Et Leurs Réservoirs - IPRA, UMR5150, 64600 Anglet, France
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to moderate levels of impurities, adsorption processes may be economically preferable. Current research on anthropogenic CO2 capture also highlights many adsorbents (Cheung and Hedin 2014; Wang et al. 2014; Tagliabue et al. 2009). Given the large number of adsorbents developed and cited in the literature for natural gas treatment or C O2 capture, industry is facing with
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