Arresting dissolution of two-dimensional metal-organic frameworks enables long life in electrochemical devices.

Two-dimensional conjugated metal-organic frameworks (2D cMOFs) are emerging as promising materials for electrochemical energy storage (EES). Despite considerable interest, an understanding of their electrochemical stability and the factors contributing to their degradation during cycling is largely lacking. Here we investigate three Cu-based MOFs and report that the dissolution of 2D cMOFs into electrolytes is a prevalent and significant degradation pathway. Several factors, such as the inherent solubility of ligands in electrolyte solvents and the duration of charge-discharge cycling exert a strong influence on the dissolution process. When these factors combine within a MOF, severely limited cycling stability is observed, with dissolution accounting for up to 80% of capacity degradation. Conversely, excellent cycling stability is observed when testing a Cu-MOF with a sparingly soluble ligand within an optimized potential window. Overall, these findings represent essential insights into the electrochemical stability of 2D cMOFs, offering crucial guidelines for their targeted development in EES applications.