Abstract
The development of two-dimensional (2D) layered metal-organic frameworks (MOFs) through precise molecular-level design and synthesis has emerged as a prominent research endeavor. However, the utilization of MOFs in their pristine form as electrodes for supercapacitors poses a significant challenge due to their limited tolerance in alkaline environments. To address these issues, we have developed Co- and Cu-based pillar-layered MOFs by regulating the structure of their inner layers through introducing an alkaline N-containing "pillar" to enhance the performance of alkaline supercapacitor electrodes. From the microstructure study and theoretical calculation, the high-density redox centers and efficient chemical bonding modes of Co-MOF determine a unique electron conduction pathway, resulting in excellent energy storage performance. This study underscores the significance of chemical bonding modes and active-site distribution in enhancing the energy storage capabilities of pillar-layered MOFs in alkaline environments, presenting a promising approach for the development of high-performance MOF-based materials for supercapacitor applications.
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