Metal-organic frameworks (MOFs) have extremely high internal surface area, tunable pore size, and exposed active sites making them suitable candidates for use as sorbents for the removal and separation of a variety of molecules. The modular nature of MOFs offers great flexibility in building components, allowing them to exhibit a wide range of characteristics suitable for applications such as gas storage, low concentration contaminant detection, contaminant capture, and catalysis. Host-guest interactions play a significant role in determining the efficiencies of these processes. In this work, we carry out <i>ab initio</i> electronic structure calculations to understand the nature of the selective binding of lanthanide and transition metal-based MOFs. Using density functional theory (DFT) calculations implemented through Quantum Espresso, we study the binding mechanisms and site-specific interactions as well as other small-scale phenomena. As a proof of concept, we benchmark our calculations with recent experimental findings of MOF applications in water treatment. In particular, we will demonstrate the ability of cerium-based MOF to capture and remove phosphates from water to remediate water eutrophication. Additionally, site-specific interactions are investigated using zirconium-based MOF for Per- and polyfluoroalkyl substances (PFASs) removal from aquatic systems. The single point host-guest interactions provide valuable mechanistic insight that can be used to rationally design materials and devices for efficient chemical separation and capture.

Theoretical insights into host-guest interactions of metal-organic frameworks

ACS Spring Meeting 2021

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