Synthesis of Tostadas‐Shaped Metal‐Organic Frameworks for Remitting Capacity Fading of Li‐Ion Batteries

Abstract Electrode design strategies that aim to increase the electrochemical performance of Li‐ion batteries (LIBs) play a key role in tapping into the power of the energy transformations involved. Metal‐organic frameworks (MOFs) have attracted scientific interest as electrode materials for LIBs, while the utilization of pristine MOFs is hindered by limited conductivity and stability, partly due to their lack of hierarchically structured pores. Herein a hydrothermal‐mechanical synthesis is reported by combining the one‐pot chemical fabrication of Ni₃(2,3,6,7,10,11‐hexaiminotriphenylene)₂ sheets and particles, and the mechanical assembly of these building blocks to improve electrical conductivity is also described. The as‐prepared ensemble (denoted as NHM) exhibits a Tostadas‐shaped structure with enriched ultramicropores and micropores. The charge‐discharge profile of NHM gives a superior reversible capacity of 1280 mA h g⁻¹ after 100 cycles at the rate of 0.1 A g⁻¹, surpassing the state‐of‐art pristine MOFs‐based anodes. Moreover, NHM is capable of maintaining 392 mA h g⁻¹ at 1 A g⁻¹ after 1000 cycles, the completion of a stability test in coin cell‐powered light emitting diodes further visualizes the remitted capacity fading of NHM. This work breaks through the limitation of capacity for pristine MOFs, providing a new pathway for achieving better energy conversion and storage.