Durable and efficient BTC-assisted 2D/0D Al–Ni-MOF nanostructures for modern electrochemical energy systems

Abstract

Most previous MOF-based electrode studies have been limited to single-metal systems without precise morphology control, often resulting in suboptimal electrochemical performance. In this work, we introduce a BTC-assisted linker engineering strategy, coupled with Al–Ni bimetallic centers and CTAB templating, to direct the formation of defect-rich, sheet-like nanostructures. This tailored hydrothermal synthesis not only enhances structural integrity, but also enabling a cooperative improvement in capacitance, energy density (ED), and stability compared with previously reported MOF-based hybrid supercapacitors. The synthesized Al–Ni-MOF exhibited a high specific capacitance of 1631.2 F g⁻¹ at 0.4 A g⁻¹ and exhibited predominantly battery-type charge storage behavior, with a diffusion-controlled contribution of 93.5% at 0.5 mV s⁻¹. Integrated as the positive electrode in an asymmetric hybrid configuration, the device achieved energy and power densities of 20.45 Wh kg⁻¹ and 836.37 W kg⁻¹, respectively, while maintaining 95.7% capacitance retention over 5000 cycles and delivering 13.34 Wh kg⁻¹ at 3200 W kg⁻¹. These findings position BTC-assisted Al–Ni-MOF architectures as a significant advancement in hybrid energy storage, combining controlled morphology with bimetallic synergy to overcome long-standing performance limitations in MOF-based electrodes.