J. Huck

Cutting the cost of carbon capture: a case for carbon capture and utilization

L. Joos, J. Huck, V. Van Speybroeck, B. Smit
Faraday Discussions
192, 391-414


A significant part of the cost for Carbon Capture and Storage (CCS) is related to the compression of the captured CO2 to its supercritical state, at 150 bar and typically 99% purity. These stringent conditions may however not always be necessary for specific cases of Carbon Capture and Utilization (CCU). In this manuscript, we investigate how much the parasitic energy of an adsorbent-based carbon capture process may be lowered by utilizing CO2 at 1 bar and adapting the final purity requirement for CO2 from 99% to 70% or 50%. We compare different CO2 sources: the flue gases of coal-fired or natural gas-fired power plants and ambient air. We evaluate the carbon capture performance of over 60 nanoporous materials and determine the influence of the initial and final purity on the parasitic energy of the carbon capture process. Moreover, we demonstrate the underlying principles of the parasitic energy minimization in more detail using the commercially available NaX zeolite. Finally, the calculated utilization cost of CO2 is compared with reported prices for CO2 and published costs for CCS.

Open Access version available at UGent repository

Carbon Capture Turned Upside Down: High-Temperature Adsorption & Low-Temperature Desorption (HALD)

L. Joos, K. Lejaeghere, J. Huck, V. Van Speybroeck, B. Smit
Energy & Environmental Science
8, 2480-2491


Carbon Capture & Sequestration (CCS) could reduce CO2 emissions from large fossil-fuel power plants in 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 CO2/N2 separation, is drastically reduced due to the competitive adsorption with H2O. Taking advantage of the power plant's waste heat to perform CCS while at the same time surmounting the negative effect of H2O 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 CO2 and H2O. First, we provide a theoretical background for this entropy-driven behavior and demonstrate under what conditions competitive adsorption can be in favor of CO2 at high temperature and in favor of H2O 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 CO2/H2O selectivity, CO2/N2 selectivity, CO2 uptake and H2O uptake. As a conclusion, this work provides new perspectives to reduce the energy requirement for CCS and to overcome the competitive adsorption of H2O.

Open Access version available at UGent repository
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