Phosphazene-Based Covalent Organic Polymer Decorated with NiCo₂O₄ Nanocuboids as a Trifunctional Electrocatalyst: A Unique Replacement for the Conventional Electrocatalysts

Developing nonprecious metal-based electrocatalysts to convert water into green fuels (H₂ and O₂) is key to address urgent climate and energy challenges. We have prepared an electrocatalyst by the immobilization of NiCo₂O₄ on a phosphazene-based covalent organic polymer (P-COP) through a facile hydrothermal method. The elemental composition of the P-COP showed the presence of a greater amount of heteroatoms N (6.62%) and P (5.62%) throughout the polymer support. Scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS) were utilized to determine the atomic structure of the nanocuboids, which depicted the formation of an inverse spinel structure. A NiCo₂O₄-P-COP-based electrode was simultaneously used for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), and it displayed a minimum overpotential of 270 and 130 mV (V vs RHE), respectively, at a current density of 10 mA cm^–2. In addition, it acted as an oxygen reduction catalyst with a half-wave potential of 0.83 V (V vs RHE) and a maximum current density of 4.5 mA cm^–2. The electrocatalytic activity is comparable with that of the commercially available Pt and RuO₂ catalysts. The combined experimental and computational studies confirm that the catalytic centers formed through the interaction between the heteroatoms (N and P) in the phosphazene matrix and metal oxides (Co and Ni) play an important role in its improved durability and electrocatalytic activity.