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Predicting Mixed-Gas Adsorption Equilibria on Activated Carbon for Precombustion CO2 Capture

Author:
García, S., Pis, J. J., Rubiera, F., Pevida, C.
Source:
Langmuir 2013 v.29 no.20 pp. 6042-6052
ISSN:
1520-5827
Subject:
activated carbon, adsorption, carbon dioxide, hydrogen, magnetism, models, nitrogen, prediction, sorption isotherms, temperature
Abstract:
We present experimentally measured adsorption isotherms of CO₂, H₂, and N₂ on a phenol–formaldehyde resin-based activated carbon, which had been previously synthesized for the separation of CO₂ in a precombustion capture process. The single component adsorption isotherms were measured in a magnetic suspension balance at three different temperatures (298, 318, and 338 K) and over a large range of pressures (from 0 to 3000–4000 kPa). These values cover the temperature and pressure conditions likely to be found in a precombustion capture scenario, where CO₂ needs to be separated from a CO₂/H₂/N₂ gas stream at high pressure (∼1000–1500 kPa) and with a high CO₂ concentration (∼20–40 vol %). Data on the pure component isotherms were correlated using the Langmuir, Sips, and dual-site Langmuir (DSL) models, i.e., a two-, three-, and four-parameter model, respectively. By using the pure component isotherm fitting parameters, adsorption equilibrium was then predicted for multicomponent gas mixtures by the extended models. The DSL model was formulated considering the energetic site-matching concept, recently addressed in the literature. Experimental gas-mixture adsorption equilibrium data were calculated from breakthrough experiments conducted in a lab-scale fixed-bed reactor and compared with the predictions from the models. Breakthrough experiments were carried out at a temperature of 318 K and five different pressures (300, 500, 1000, 1500, and 2000 kPa) where two different CO₂/H₂/N₂ gas mixtures were used as the feed gas in the adsorption step. The DSL model was found to be the one that most accurately predicted the CO₂ adsorption equilibrium in the multicomponent mixture. The results presented in this work highlight the importance of performing experimental measurements of mixture adsorption equilibria, as they are of utmost importance to discriminate between models and to correctly select the one that most closely reflects the actual process.
Agid:
5767679