Metal-organic framework (MOF) membranes are energy-efficient candidates for molecular separations, but it remains a considerable challenge to eliminate defects at the atomic scale. The enlargement of pores due to defects reduces the molecular-sieving performance in separations and hampers the wider application of MOF membranes, especially for liquid separations, owing to insufficient stability. Here we report the elimination of lattice defects in MOF membranes based on a high-probability theoretical coordination strategy that creates sufficient chemical potential to overcome the steric hindrance that occurs when completely connecting ligands to metal clusters. Lattice defect elimination is observed by real-space high-resolution transmission electron microscopy and studied with a mathematical model and density functional theory calculations. This leads to a family of high-connectivity MOF membranes that possess ångström-sized lattice apertures that realize high and stable separation performance for gases, water desalination and an organic solvent azeotrope. Our strategy could enable a platform for the regulation of nanoconfined molecular transport in MOF pores.
|Original language||English (US)|
|State||Published - May 11 2023|
Bibliographical noteKAUST Repository Item: Exported on 2023-05-19
Acknowledgements: We thank X. Ren (School of Chemistry and Molecular Engineering, Nanjing Tech University) for discussions. W.Q.J. acknowledges funding from the National Natural Science Foundation of China (grant numbers 22038006 and 21921006) and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). G.P.L. acknowledges funding from the National Natural Science Foundation of China (grant number 22278210) and the Natural Science Foundation of Jiangsu Province (grant number BK20220002). G.Z.L. acknowledges funding from the Project funded by the China Postdoctoral Science Foundation (grant numbers 2022TQ0147 and 2022M721584). We thank the High-Performance Computing Center of Nanjing Tech University for supporting the computational resources.
ASJC Scopus subject areas
- Mechanics of Materials
- Materials Science(all)
- Mechanical Engineering
- Condensed Matter Physics