"Advanced Computational Insights into Ni(II) Schiff Base Complexes: Addressing Sluggish Kinetics and Stability Challenges in Oxygen Reduction Reaction Catalysis"

The development of efficient and stable catalysts for the oxygen reduction reaction (ORR) remains a critical challenge in the pursuit of next-generation energy technologies. In this study, we designed and investigated a Ni (II) Schiff base complex as a potential solution to address the sluggish kinetics and stability limitations of ORR catalysts. A comprehensive computational approach was adopted, integrating ChemDraw for molecular modeling, DMol3 in Material Studio for electronic structure and catalytic property calculations, and MATLAB for precise overpotential analysis. The Ni (II) complex demonstrated a significantly lower overpotential (−0.55) compared to its Co(II) counterpart (−4.95), highlighting its superior catalytic efficiency and faster reaction kinetics. The Schiff base ligand, with its robust chelating ability and electronic tunability, facilitated the stabilization of intermediates and optimized the electronic properties of the Ni (II) center, enabling efficient electron transfer and intermediate transitions. Gibbs free energy calculations revealed a pathway with hydroperoxide (HO2−) as the first intermediate, further validating the thermodynamic feasibility and kinetic superiority of the Ni (II) complex. These findings underscore the Schiff base ligand as an ideal framework for designing high-performance catalysts and demonstrate the potential of the Ni (II) complex for ORR applications in fuel cells and metal-air batteries. This study provides valuable insights into leveraging computational tools for catalyst design and emphasizes the need for further exploration of Schiff base ligands in energy catalysis to address global energy demands.