Potential modulation of Nickel-Cobalt hydroxide nanosheets with conductive Poly(3,4-Ethylenedioxythiophene) skin for aqueous hybrid supercapacitors

Transition metal hydroxides with tuned structure and superior electrochemical activities are of potential as positive electrodes for aqueous hybrid supercapacitors (AHSs), yet their conductivities and stacking behaviors need to be optimized to further improve the electrical potential distribution from the electronic multi-contact border to the electroactive center. Herein, we report a new approach to coat poly(3,4-ethylenedioxythiophene) (PEDOT) skin with a controlled thickness on nickel–cobalt layered double hydroxide (NiCo-LDH) nanosheets via a simple yet efficient oxidative chemical vapor deposition (oCVD). The conductive PEDOT skin is ionically permeable, resulting in uniform distribution of the electrical potential and fast transport of ions to active sites. The density functional theory (DFT) calculations reveal that the PEDOT layer can build an embedded electric field at the interface and enable a low desorption energy of hydrogen for electrochemical redox reactions. The as-obtained NiCo-LDH nanosheets with the PEDOT skin of 10 nm thick (LDH/PEDOT-10) as the battery-type electrode deliver a high specific capacity of 167 mAh g⁻¹ (1250F g⁻¹) with a greatly improved rate capability of 79 % at 50 A g⁻¹ and cycling stability of 92 % for 6000 cycles, which endows AHS devices with superior charge-storage performance. This study has demonstrated for the first time that the modulation of electrical potential for redox electrodes via an interface engineering strategy can achieve simultaneously fast reaction kinetics and excellent structure stability for aqueous energy-storage devices. © 2023 Elsevier B.V.