Engineering Cobalt-Based Bimetallic Compounds via NH4F-Directed ZIF67 Transformation for Battery–Supercapacitor Hybrids with Enhanced Energy Storage Performance

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Author list: Cheng, T.-M.; Lu, Y.-A.; Lee, P.-C.; Kongvarhodom, C.; Husain, S.; Yougbaré, S.; Chen, H.-M.; Lin, L.-Y.

Publisher: American Chemical Society

Publication year: 2025

Volume number: 10

Issue number: 35

Start page: 40089

End page: 40100

Number of pages: 12

eISSN: 2470-1343

URL: https://www.scopus.com/inward/record.uri?eid=2-s2.0-105015367413&doi=10.1021%2Facsomega.5c04906&partnerID=40&md5=6a41b53daef5db0971d6c2a84aa882c0

Languages: English-Great Britain (EN-GB)

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Abstract

Cobalt-based compounds have attracted considerable attention as electroactive materials for energy storage owing to their high theoretical capacitance and cost-effectiveness. Zeolitic imidazolate framework-67 (ZIF67) is a cobalt-containing metal–organic framework that features a high surface area and a tunable porous architecture, but inherently low conductivity limits its electrochemical performance. To address this issue, structure-directing agents (SDAs) have been employed to enhance the surface characteristics and energy storage behavior of ZIF67 derivatives. In particular, the redox activity of battery-type electrodes is largely governed by the nature of the metal species involved. In this study, a series of cobalt-based bimetallic compounds incorporating Ni, Cu, Al, Zn, and Mn are synthesized using NH4F as the SDA in 2-methylimidazole medium. Morphology and composition of the resulting materials are strongly dependent on the secondary metal species. The cobalt–nickel (CoNi) electrode achieves the highest specific capacitance (CF) of 997.3 F/g at 20 mV/s, attributed to the synergistic redox behavior of cobalt and nickel. The contributions from both diffusion-controlled and surface-capacitive processes are also quantitatively assessed. A BSH assembled using the CoNi and carbon electrodes achieves a maximum energy density of 9.2 Wh/kg at 375 W/kg, along with a CFretention of 83.1% and a Coulombic efficiency of 94.2% after 10,000 cycles. © 2025 The Authors. Published by American Chemical Society

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