External Chirality-Driven Interfacial Spin Filtering in Magnetically Aligned NiFe-LDH Facilitates the Enhancement of Oxygen Evolution Reaction

Abstract

In this study, we demonstrate controlled charge transfer from magnetic particles by introducing an external chiral molecular layer that acts as a spin filter. The system is experimentally validated through electrocatalytic measurements and electrical characterization in two-terminal device configurations. Our approach uniquely integrates magnetic catalysis, chirality, and spin-selective transport, diverging from traditional chiral catalytic systems. Specifically, NiFe-layered double hydroxide (NiFe-LDH) serves as the magnetic catalyst, whose activity is modulated by aligning its magnetic moment with an external magnetic field. While NiFe-LDH is well known for its oxygen evolution reaction (OER) performance, the novelty of our work lies in the unconventional coupling of material components and physical principles. Unlike conventional chiral catalysis, where spin polarization arises from ligands directly coordinated to metal centres via the CISS effect, we introduce chirality as an external layer. This layer facilitates spin-selective charge transfer from hydroxide intermediates to the magnetized, spin-polarized NiFe-LDH, modulating catalytic activity through controlled spin filtering. Our findings provide new mechanistic insight into the interplay of chirality, magnetism, and electrocatalysis and open a pathway for designing spin-dependent catalytic systems beyond conventional coordination-based strategies.