One of the main bottlenecks to deploying large-scale carbon dioxide capture and storage (CCS) in power plants is the energy required to separate the CO2 from flue gas. For example, near-term CCS technology applied to coal-fired power plants is projected to reduce the net output of the plant by some 30% and to increase the cost of electricity by 60–80%. Developing capture materials and processes that reduce the parasitic energy imposed by CCS is therefore an important area of research. We have developed a computational approach to rank adsorbents for their performance in CCS. Using this analysis, we have screened hundreds of thousands of zeolite and zeolitic imidazolate framework structures and identified many different structures that have the potential to reduce the parasitic energy of CCS by 30–40% compared with near-term technologies.
This is a preview of subscription content
Subscribe to Journal
Get full journal access for 1 year
only $8.25 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Get time limited or full article access on ReadCube.
All prices are NET prices.
Chu, S. Carbon capture and sequestration. Science 325, 1599 (2009).
Pacala, S. & Socolow, R. Stabilization wedges: Solving the climate problem for the next 50 years with current technologies. Science 305, 968–972 (2004).
Metz, B., Davidson, O., deConinck, H., Loos, M. & Meyer, L. IPCC Special Report on Carbon Dioxide Capture and Storage. (Intergovernmental Panel on Climate Change (IPCC), 2005); http://www.ipcc.ch.
Massood, R., Timothy, J. S., Nsakala ya, N. & Liljedahl, G. N. Carbon Dioxide Capture from Existing Coal-Fired Power Plants (National Energy Technology Laboratory, US Department of Energy, 2007).
Bhown, A. S. & Freeman, B. C. Analysis and status of post-combustion carbon dioxide capture technologies. Environ. Sci. Technol. 45, 8624–8632 (2011).
Bottoms, R. Separating acid gases. US Patent 1,783,901 (1930).
Rochelle, G. T. Amine scrubbing for CO2 capture. Science 325, 1652–1654 (2009).
Ciferno, J. P., Marano, J. J. & Munson, R. K. Technology integration challenges. Chem. Eng. Prog. 107, 34–44 (2011).
Ferey, G. Hybrid porous solids: Past, present, future. Chem. Soc. Rev. 37, 191–214 (2008).
Yaghi, O. M. et al. Recticular synthesis and the design of new materials. Nature 423, 708–714 (2003).
D’Alessandro, D. M., Smit, B. & Long, J. R. Carbon dioxide capture: Prospects for new materials. Angew. Chem. Int. Ed. 49, 6058–6082 (2010).
Banerjee, R. et al. High-throughput synthesis of zeolitic imidazolate frameworks and application to CO2 capture. Science 319, 939–943 (2008).
Deem, M. W., Pophale, R. & Cheeseman, P. A. A database of new zeolite-like materials. Phys. Chem. Chem. Phys. 13, 12407–12412 (2011).
Krishna, R. & van Baten, J. M. In silico screening of metal-organic frameworks in separation applications. Phys. Chem. Chem. Phys. 13, 10593–10616 (2011).
Krishna, R. & Long, J. R. Screening metal-organic frameworks by analysis of transient breakthrough of gas mixtures in a fixed bed adsorber. J. Phys. Chem. C 115, 12941–12950 (2011).
Yazaydin, A. O. et al. Screening of metal-organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach. J. Am. Chem. Soc. 131, 18198 (2009).
Freeman, S. A., Dugas, R., Van Wagener, D., Nguyen, T. & Rochelle, G. T. Carbon dioxide capture with concentrated, aqueous piperazine. Energy Procedia 1, 1489–1496 (2009).
Lemmon, E. W., Huber, M. L. & McLinden, M. O. NIST Reference Fluid Thermodynamic and Transport Properties Database (REFPROP): Version 9.0. (NIST, 2010); http://www.nist.gov/srd/nist23.cfm.
Frenkel, D. & Smit, B. Understanding Molecular Simulations: From Algorithms to Applications 2nd edn (Academic, 2002).
Smit, B. & Maesen, T. L. M. Molecular simulations of zeolites: Adsorption, diffusion, and shape selectivity. Chem. Rev. 108, 4125–4184 (2008).
Krishna, R., Calero, S. & Smit, B. Investigation of entropy effects during sorption of mixtures of alkanes in MFI zeolite. Chem. Eng. J. 88, 81–94 (2002).
Myers, A. L. & Prausnitz, J. M. Thermodynamics of mixed gas adsorption. Am. Inst. Chem. Eng. J. 11, 121–130 (1965).
Rao, M. B. & Sircar, S. Thermodynamic consistency for binary gas adsorption equilibria. Langmuir 15, 7258–7267 (1999).
Martin, R. L., Smit, B. & Haranczyk, M. Addressing challenges of identifying geometrically diverse sets of crystalline porous materials. J. Chem. Inf. Modell. 52, 308–318 (2012).
Deem, M. W., Pophale, R., Cheeseman, P. A. & Earl, D. J. Computational discovery of new zeolite-like materials. J. Phys. Chem. C 113, 21353–21360 (2009).
Simancas, R. et al. Modular organic structure-directing agents for the synthesis of zeolites. Science 330, 1219–1222 (2010).
Jariwala, K. & Haranczyk, M. http://www.carboncapturematerials.org (2011).
International Zeolite Association (IZA); http://www.iza-structure.org/databases (2011).
Sanders, M. J., Leslie, M. & Catlow, C. R. A. Interatomic potentials for SiO2 . J. Chem. Soc. Chem. Commun. 1271–1273 (1984).
Beest, B. W. H. v., Kramer, G. J. & Santen, R. A. v. Force fields for silicas and aluminophosphates based on ab initio calculations. Phys. Rev. Lett. 64, 1955–1958 (1990).
Willems, T. F., Rycroft, C. H., Kazi, M., Meza, J. C. & Haranczyk, M. Algorithms and tools for high-throughput geometry-based analysis of crystalline porous materials. Micropor. Mesopor. Mater. 149, 134–141 (2012).
Garcia-Perez, E., Dubbeldam, D., Liu, B., Smit, B. & Calero, S. A computational method to characterize framework aluminum in aluminosilicates. Angew. Chem. Int. Ed. 46, 276–278 (2007).
Löwenstein, W. The distribution of aluminum in the tetrahedra of silicates and aluminates. Am. Miner. 39, 92–96 (1954).
Calero, S. et al. Understanding the role of sodium during adsorption. A force field for alkanes in sodium exchanged faujasites. J. Am. Chem. Soc. 126, 11377–11386 (2004).
Park, K. S. et al. Exceptional chemical and thermal stability of zeolitic imidazolate frameworks. Proc. Natl Acad. Sci. USA 103, 10186–10191 (2006).
Garcia-Perez, E. et al. A computational study of CO2, N2, and CH4 adsorption in zeolites. Adsorption-J. Int. Adsorption Soc. 13, 469–476 (2007).
Garcia-Sanchez, A. et al. Transferable force field for carbon dioxide adsorption in zeolites. J. Phys. Chem. C 113, 8814–8820 (2009).
Mayo, S. L., Olafson, B. D. & Goddard, W. A. DREIDING—a generic force-field for molecular simulations. J. Phys. Chem. 94, 8897–8909 (1990).
Siepmann, J. I. & Potoff, J. J. Vapor-liquid equilibria of mixtures containing alkanes, carbon dioxide, and nitrogen. Aiche J. 47, 1676–1682 (2001).
Zhong, C. L. & Xu, Q. A general approach for estimating framework charges in metal-organic frameworks. J. Phys. Chem. C 114, 5035–5042 (2010).
Kim, J., Rodgers, J. M., Athenes, M. & Smit, B. Molecular Monte Carlo simulations using graphics processing units: To waste recycle or not? J. Chem. Theor. Comput. 7, 3208–3222 (2011).
Bates, S. P., Well, W. J. M. v., Santen, R. A. v. & Smit, B. Energetics of n-alkanes in zeolites: A configurational-bias Monte Carlo investigation into pore size dependence. J. Am. Chem. Soc. 118, 6753–6759 (1996).
Haranczyk, M. & Sethian, J. A. Navigating molecular worms inside chemical labyrinths. Proc. Natl Acad. Sci. USA 106, 21472–21477 (2009).
Haranczyk, M. & Sethian, J. A. Automatic structure analysis in high-throughput characterization of porous materials. J. Chem. Theor. Comput. 6, 3472–3480 (2010).
The research was supported by the US Department of Energy under contracts DE-AC02-05CH11231, #CSNEW918, DE-SC0001015, DE-FG02-03ER15456, ARPA-e, and CCSI and the Office of Innovation at the Electric Power Research Institute (a detailed description can be found in the Supplementary Information).
The authors declare no competing financial interests.
About this article
Cite this article
Lin, LC., Berger, A., Martin, R. et al. In silico screening of carbon-capture materials. Nature Mater 11, 633–641 (2012). https://doi.org/10.1038/nmat3336
Communications Chemistry (2022)
Chemical Research in Chinese Universities (2022)
Nature Materials (2021)
Korean Journal of Chemical Engineering (2021)