Carbon capture & sequestration (CCS) could reduce CO 2 emissions from large fossil-fuel power plants on the short term, but the high energy penalty of the process hinders its industrial deployment. Moreover, the utility of nanoporous materials, known to be selective for the CO 2 /N 2 separation, is drastically reduced due to the competitive adsorption with H 2 O. Taking advantage of the power plant's waste heat to perform CCS while at the same time surmounting the negative effect of H 2 O is therefore an attractive idea. We propose an upside-down approach for CCS in nanoporous materials, high-temperature adsorption & low-temperature desorption (HALD), that exploits the temperature-dependent competitive adsorption of CO 2 and H 2 O. First, we provide a theoretical background for this entropy-driven behavior and demonstrate under what conditions competitive adsorption can be in favor of CO 2 at high temperature and in favor of H 2 O at low temperature. Then, molecular simulations in all-silica MFI provide a proof of concept. The International Zeolite Association database is subsequently screened for potential candidates and finally, the most promising materials are selected using a post-Pareto search algorithm. The proposed post-Pareto approach is able to select the material that shows an optimal combination of multiple criteria, such as CO 2 /H 2 O selectivity, CO 2 /N 2 selectivity, CO 2 uptake and H 2 O uptake. As a conclusion, this work provides new perspectives to reduce the energy requirement for CCS and to overcome the competitive adsorption of H 2 O.
Broader contextUtilizing the residual heat of a power plant's flue gas to capture the CO 2 from this CO 2 /N 2 /H 2 O mixture could drastically reduce the energy requirement of carbon capture and sequestration (CCS). The novel approach to CCS presented here, high-temperature adsorption & low-temperature desorption (HALD) of CO 2 in zeolites, exploits the temperature-dependent competitive adsorption of CO 2 and H 2 O. A theoretical model demonstrates that differences in the adsorption enthalpy and entropy for CO 2 and H 2 O can favor CO 2 adsorption at high temperature and H 2 O uptake at low temperature. Using Grand Canonical Monte Carlo simulations, we perform a screening of the existing zeolite topologies to assess their adsorption properties. Afterwards, a post-Pareto analysis identifies the most promising materials. The proposed HALD behavior can be used in a temperature-swing process, which would not require the input of energy for regeneration, but instead would recover the CO 2 by saturating the material with water. In addition, the deeper understanding of the entropy-driven competitive adsorption of CO 2 and H 2 O opens new perspectives to overcome the detrimental effect of water.