Construction, computation, and characterisation of spin-control powered catalysts for oxygen electrocatalysis

Spin has emerged as a powerful and complementary dimension in the rational design of oxygen electrocatalysts, offering a route to circumvent long-standing limitations imposed by conventional activity descriptors and scaling relationships. This review consolidates recent advances demonstrating how spin states, magnetic ordering, and spin-selective electron transport influence the thermodynamics and kinetics of key OER and ORR steps, particularly the spin-forbidden transition from singlet intermediates to triplet oxygen. We critically examine traditional strategies such as ligand-field engineering, doping, lattice strain, and defect control, as well as spin polarisation approaches including magnetic-field assistance and chiral-induced spin selectivity (CISS), integrating insights from theory, computation, and operando characterisation. Collectively, these studies reveal that manipulating spin polarisation at active sites can accelerate multi-electron transfer pathways, alter intermediate binding, and enhance overall catalytic performance beyond classical design limits. Finally, we highlight remaining mechanistic ambiguities, emerging diagnostic tools, and future opportunities for integrating spin physics into scalable electrocatalyst development.