Pillar-Supported\n2D Layered MOFs with Abundant Active-Site\nDistributions for High-Performance Alkaline Supercapacitors

The development of two-dimensional (2D) layered metal–organic\nframeworks (MOFs) through precise molecular-level design and synthesis\nhas emerged as a prominent research endeavor. However, the utilization\nof MOFs in their pristine form as electrodes for supercapacitors poses\na significant challenge due to their limited tolerance in alkaline\nenvironments. To address these issues, we have developed Co- and Cu-based\npillar-layered MOFs by regulating the structure of their inner layers\nthrough introducing an alkaline N-containing “pillar”\nto enhance the performance of alkaline supercapacitor electrodes.\nFrom the microstructure study and theoretical calculation, the high-density\nredox centers and efficient chemical bonding modes of Co-MOF determine\na unique electron conduction pathway, resulting in excellent energy\nstorage performance. This study underscores the significance of chemical\nbonding modes and active-site distribution in enhancing the energy\nstorage capabilities of pillar-layered MOFs in alkaline environments,\npresenting a promising approach for the development of high-performance\nMOF-based materials for supercapacitor applications.