We employ classical density functional theory coupled with the PC-SAFT equation of state to investigate deformation behavior in carbon nanopores during CO₂ and alkane adsorption. Recent advances in DFT computational algorithms and the development of efficient open-source frameworks have dramatically improved the feasibility of systematic studies. [1-5] Modern DFT implementations reduce calculation times from days to minutes compared to traditional molecular simulation approaches while maintaining quantitative accuracy, enabling the rapid generation of thousands of isotherms. By varying pore size, pore geometry, and adsorbate composition, we generate comprehensive maps revealing how molecular packing phenomena govern structural response. The characteristic nonmonotonic deformation patterns—initial contraction driven by fluid-wall attraction, followed by expansion from molecular crowding—exhibit strong dependencies on pore size and adsorbate properties that cannot be predicted from single-component studies alone.
[1] P. Rehner, G. Bauer, J. Gross, Feos: An open-source framework for equations of state and classical density functional theory, Industrial & Engineering Chemistry Research 62(12) (2023) 5347-5357.
[2] R. Stierle, G. Bauer, N. Thiele, B. Bursik, P. Rehner, J. Gross, Classical density functional theory in three dimensions with GPU-accelerated automatic differentiation: computational performance analysis using the example of adsorption in covalent-organic frameworks, Chemical Engineering Science (2024) 120380.
[3] L.J. dos Santos, V.M. Sermoud, A.G. Barreto Jr, F.W. Tavares, Adsorption-induced deformation of nanoporous carbons: Insight from classical density functional theory based on the PC-SAFT equation of state, Fluid Phase Equilibria 574 (2023) 113882.
[4] L.J.d. Santos, E.d.A. Soares, A.G. Barreto, F.W. Tavares, Comparison of 3D-cDFT and GCMC simulations for fluid–structure analysis in amorphous carbon nanoporous materials, Adsorption 30(5) (2024) 583-594.
[5] N.J. Corrente, E.L. Hinks, A. Kasera, J. Liu, A.V. Neimark, Deformation of Nanoporous Carbons Induced By Multicomponent Adsorption: Insight from the SAFT-DFT Model, The Journal of Physical Chemistry C 128(20) (2024) 8458-8466.