Prediction of CO₂ Adsorption Properties in Zeolites Using Force Fields Derived from Periodic Dispersion-Corrected DFT Calculations

Citations Over TimeTop 10% of 2012 papers

Abstract

We demonstrate a new approach to develop transferable force fields describing molecular adsorption in zeolites by combining dispersion-corrected density functional theory (DFT) calculations and classical atomistic simulations. This approach is illustrated with the adsorption of CO2 in zeolites. Multiple dispersion-corrected DFT methods were tested for describing CO2 adsorption in sodium-exchanged ferrierite. The DFT-D2 approach was found to give the best agreement with high level quantum chemistry results and experimental data. A classical force field for CO2 adsorption in siliceous zeolites was then developed on the basis of hundreds of DFT-D2 calculations that probed the full range of accessible volume in purely siliceous chabazite (Si-CHA) via random sampling. We independently performed experiments with Si-CHA measuring CO2 isotherms and heats of adsorption by microcalorimetry. Excellent agreement was obtained between adsorption isotherms predicted with our first-principles-derived force field and our experiments. The transferability of this force field was examined using available adsorption isotherms for CO2 in siliceous MFI and DDR zeolites, again with reasonably good agreement between calculated and experimental results. The methods demonstrated by these calculations will be broadly applicable in using molecular simulations to predict properties of adsorbed molecules in zeolites and other nanoporous materials.

Related Papers

• → Preparation of zinc chabazite (ZnCHA) for CO2 capture(2016)17 cited
• → The characterization and methane adsorption of Ag-, Cu-, Fe-, and H-exchanged chabazite-rich tuff from Turkey(2019)11 cited
• → Synthesis of a New Zeolite, Intergrowth of Erionite and Chabazite(2021)13 cited
• → Molecular Basis for the High CO₂ Adsorption Capacity of Chabazite Zeolites(2014)1 cited
• Cu-Chabazite SCR Catalysts의 황 피독 및 탈황에 의한 NOx 저감 성능에 관한 연구(2013)