Natural gas and hydrogen are attractive fuels for next-generation, cleaner vehicles.  However, these gaseous fuels are difficult to store in a compact volume.  One strategy to address this challenge is to adsorb these gases within nanoporous materials such as metal-organic frameworks (MOFs).  MOFs are synthesized in a building-block approach by combining metal nodes and organic linker molecules, giving rise to an essentially unlimited number of possible materials.  Computational screening is becoming a powerful tool for screening MOFs for applications such as gas storage.  Searching for materials with both promising storage capabilities and high chemical stability, we created 204 proposed MOF structures featuring stable Zr nodes on the computer and calculated their ability to adsorb methane using grand canonical Monte Carlo simulations.  The top-performing MOF, NU-800, was subsequently synthesized by our collaborators and demonstrated to be a promising material for natural gas storage.  We have also used a combination of molecular modeling and macroscopic thermodynamic modeling to understand the role of higher hydrocarbons on natural gas storage performance over many operation cycles (loading/unloading) of the vehicle fuel tank.  Quantum chemical calculations were used to obtain important information about hydrogen binding with metal-catecholate functionalities in MOFs and with a zwitterionic MOF.  And in an effort to more rapidly identify promising candidates, our group has developed high-throughput methods that can generate and screen thousands of MOFs.  Recently, we have applied these methods to explore the physical limits of natural gas and hydrogen storage in nanoporous materials.

Computational screening of metal-organic frameworks for hydrogen and natural gas storage

248th National Meeting (2014)

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