Magnetically Triggered Interplay of Capacitive and Diffusion Contributions for Boosted Supercapacitor Performance

The chemistry involved in supercapacitors in terms of their mechanistic contributions leading to improved specific capacity will aid in easy commercialization. The main contributory factors in a supercapacitor are either capacitive (non-diffusion controlled) or ion-diffusion behavior, which results in enhanced charge-discharge characteristics of a supercapacitor reflected in its power density, whereas ion-diffusion behavior will lead to the enhanced energy density of a supercapacitor. In this context, the present article attempts to understand the use of external magnetic fields, leading to the interplay between capacitive and ion-diffusion behavior in a high-performance supercapacitor. The model system chosen in the present study, nickel cobalt copper carbonate hydroxide (NiCoCuCH), can effectively address the interplay between capacitive and ion diffusion contributions by varying total magnetic effects involving magnetic dilution. The magneto-enhancement of the electrodes nickel cobalt copper carbonate hydroxide (NiCoCuCH) and aluminum-doped nickel cobalt copper carbonate hydroxide (Al-NiCoCuCH) was demonstrated under the magnetic field from 0 to 250 mT. Both NiCoCuCH and Al-NiCoCuCH show dominant non-diffusion-controlled (capacitive) and diffusion-controlled behavior as a function of the applied external magnetic field. Under the influence of the external magnetic field, ferromagnetic coupling between metal-oxygen-metal centers via oxygen 2p orbitals enhances, leading to a facile redox pathway. To further control the charge-discharge behavior of the electrode via the interplay between diffusive and capacitive, a non-magnetic ion, Al3+, was doped into the bare metal carbonate hydroxide crystal lattice. The Al3+ ion not only alters the crystal symmetry but also restricts the alignment of the magnetic domains in the electrode, leading to a sluggish redox pathway, effectively increasing the capacitive contribution, and leading to improved charge-discharge characteristics at the expense of energy density. We have constructed an asymmetric device with the best-performing (110 mT) NiCoCuCH electrode as a positive electrode and activated carbon as a negative electrode. The NiCoCuCH/AC ASC device at 110 mT has the largest specific capacity (1100 C g-1 at 2 A g-1) at 110 mT, leading to a high energy density (250 W h kg-1) and a power density (1.7 kW kg-1) of the electrode.