By Introducing Multiple Hydrogen Bonds Endows MOF Electrodes with an Enhanced Structural Stability

Recently, metal-organic frameworks (MOFs) have attracted great interest in energy storage areas. However, the poor structural stability of MOFs derived from weak coordination bonds limits their applications. Here, quadruple hydrogen bonds (H-bonds) were introduced onto the MOFs to enhance their structural stability. Cross-linked networks could be formed between molecules owing to multiple H-bonds, strengthening the framework stability. Moreover, the dynamic reversibility of H-bonds could endow MOFs with self-healing ability. Furthermore, due to lower binding energy compared to coordination bonds, H-bonds break preferentially when subjected to internal stress, thus protecting the MOFs. Consequently, the as-prepared self-healing hybrid (SHH-Cu-MOF@Ti₃C₂T_X) exhibited high capacitance retention (89.4%) after 5000 cycles at 1 A g^-1, while that hybrid without dynamic H-bonds (H-Cu-MOF@Ti₃C₂T_X) presented a 79.9% retention, delivering an enhancement in cycling stability. Moreover, an asymmetric supercapacitor (ASC) was fabricated by employing SHH-Cu-MOF@Ti₃C₂T_X and activated carbon (AC) as the electrodes. The ASC delivered a specific capacitance (47.4 F g^-1 at 1 A g^-1), an energy density (16.9 Wh kg^-1), and a power density (800 W kg^-1) as well as good rate ability (retains 81% of its initial capacitance from 0.2 A g^-1 to 5 A g^-1).