Rational design of lanthanide-based metal-organic frameworks for CO₂ capture using computational modeling

Area of Science:

• Materials Science
• Chemical Engineering
• Computational Chemistry

Background:

• Metal-organic frameworks (MOFs) are tunable materials for CO2 capture and separation.
• Lanthanide MOFs (Ln-MOFs) offer potential for high-performance gas adsorbents due to their high coordination numbers.

Purpose of the Study:

• To design novel hypothetical Ln-MOFs with enhanced CO2/N2 separation performance.
• To identify Ln-MOF structures with superior selectivity and working capacity for carbon capture.

Main Methods:

• Combined molecular simulations and quantum mechanical (QM) calculations.
• Generated 77 hypothetical Ln-MOFs by modifying linkers and metal atoms of a parent Ln-MOF.
• Employed molecular mechanics (MM) for initial optimization and grand canonical Monte Carlo (GCMC) for CO2/N2 separation simulations.
• Utilized QM calculations for final geometry optimization of promising candidates.

Main Results:

• Identified five Ln-MOFs that outperformed the original structure in CO2/N2 separation.
• Two hypothetical Ln-MOFs demonstrated superior CO2/N2 separation performance after QM optimization.
• The study provides a computational framework for designing advanced Ln-based MOFs.

Conclusions:

• Rational design using computational methods can yield Ln-MOFs with improved CO2 separation properties.
• The developed methodology aids in discovering new materials for efficient carbon capture.
• This work facilitates the development of next-generation adsorbents for CO2 mitigation.