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Machine Learned Force Field Modeling of Metal Organic Frameworks for CO2 Direct Air Capture

Conference ·
DOI:https://doi.org/10.2172/2426624· OSTI ID:2426624
 [1];  [2]
  1. NETL Site Support Contractor, National Energy Technology Laboratory
  2. NETL

Direct air capture (DAC) is a method for removing CO2 directly from air. Metal organic frameworks (MOFs) have been studied as DAC sorbent materials because of their structural and chemical diversity. Thermodynamic calculations using classical force fields are often used to evaluate MOFs for their performance in separations such as CO2 capture. Machine-learned force fields (MLFFs) can use machine learning to form quantitative relationships between a material’s chemical structure and the forces and energies predicted by more accurate quantum mechanical calculations, such as dispersion-corrected density functional theory (DFT). These descriptions of forces and energies can be used to improve the accuracy of adsorption calculations. In this work, classical models were used to pre-screen MOFs for CO2 capture. DFT calculations were then used to examine the adsorption mechanism. Next, MLFF models were developed for MOFs to achieve DFT-level accuracy for the forces and energies associated with MOF flexibility and CO2 adsorption. These methods were parametrized based on thousands of DFT calculations of CO2 in flexible MOFs and used to predict MOF structural properties as well as CO2 adsorption properties.

Research Organization:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy and Carbon Management (FECM)
OSTI ID:
2426624
Country of Publication:
United States
Language:
English

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