High-Throughput Computational Screening of Experimental Zr-Based MOFs for Elemental Mercury Capture

Metal-organic frameworks (MOFs) have been investigated for their unique physical properties, making them suitable for the adsorption and separation of mercury. Zr-MOFs have garnered great attention because of their excellent stability and adsorption performance. However, with the increasing number of Zr-MOFs, conducting experimental studies to identify ideal candidates for the capture of mercury is not feasible due to their high workload and low efficiency. In this work, we calculated the adsorption properties of elemental mercury (Hg-0) in 181 Zr-based MOF candidates using molecular simulations. We identified the Zr-MOFs that exhibited the best performance for the removal of mercury from industrial flue gases using the high-throughput screening method. The differences between the Henry selectivity and GCMC selectivity suggest that the adsorption performance of some MOFs under practical conditions cannot simply be evaluated by Henry selectivity. Based on the best-performing MOFs, we selected two representative candidates to calculate the adsorption isotherms for mercury in the presence of sulfur dioxide. The results emphasize the importance of the structure-property relationships of the Zr-MOFs for the removal of Hg-0.

Automated summary

Metal-organic frameworks (MOFs) are being studied for their unique physical properties in the adsorption and separation of mercury. Zr-MOFs have gained attention due to their stability and adsorption performance. However, experimental studies to identify ideal candidates for mercury capture are not feasible, so we used molecular simulations to calculate the adsorption properties of 181 Zr-based MOF candidates. We identified the best-performing Zr-MOFs for mercury removal from industrial flue gases using a high-throughput screening method, emphasizing the importance of structure-property relationships in Zr-MOFs.