2012/09/17 by Claudio Cazorla, Cazorla, Claudio, Stephen A. Shevlin +1
Chemistry · Engineering · #Carbon Dioxide Capture Technologies #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Membrane Separation and Gas Transport #Zeolite Catalysis and Synthesis
paper · pdf · doi:10.48550/arxiv.1209.3660
openalex publication_date 2012/09/17 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We have performed a thorough computational study to assess the accuracy of\ndensity functional theory (DFT) methods in describing the interactions of CO2\nwith model alkali-earth-metal (AEM, Ca and Li) decorated carbon structures,\nnamely anthracene (C14H10) molecules. We find that gas-adsorption energy and\nequilibrium structure results obtained with both standard (i.e. LDA and GGA)\nand hybrid (i.e. PBE0 and B3LYP) exchange-correlation functionals of DFT differ\nsignificantly from results obtained with second-order Moller-Plesset\nperturbation theory (MP2), an accurate computational quantum chemistry method.\nThe major disagreements found can be mostly rationalized in terms of electron\ncorrelation errors that lead to inaccurate charge transfers and electrostatic\nCoulomb interactions between the molecules. Interestingly, we show that when\nthe concentration of AEM atoms in anthracene is tuned to resemble as closely as\npossible to the electronic structure of AEM-decorated graphene, hybrid\nexchange-correlation DFT and MP2 methods provide quantitatively similar\nresults. We discuss the implications of our work in modeling and\ncharacterization of currently sought carbon capture and sequestration\nmaterials.\n