Spin‐Selective Oxygen Evolution in Chiral Molecule‐Intercalated Layered Double Hydroxides

ABSTRACT The chiral‐induced spin selectivity (CISS) effect offers a novel paradigm for designing high‐performance catalysts for spin‐dependent oxygen evolution reactions (OER). Layered double hydroxides (LDHs), are widely used for oxygen evolution reaction (OER) due to their superior electrocatalytic activity and stability in alkaline environments. Here, we demonstrate that intercalating chiral phenylalanine molecules into CoFe‐LDH induces spin‐polarized OER via the CISS effect, while simultaneously expanding the interlayer spacing. The resulting chiral–inorganic hybrid interface directs the reaction along a lower‐energy pathway, promoting the formation of triplet O 2 , and exhibits outstanding OER performance with a lower overpotential of 245 mV at 10 mA cm −2 , as well as faster charge‐transfer kinetics compared to its achiral counterpart. Using in situ XANES, in situ Raman spectroscopy, and nanoscale scanning electrochemical cell microscopy (SECCM), we further uncover the fundamental origin of this chiral‐induced spin‐selective behavior. This study establishes a general strategy for designing advanced, stable oxide‐based electrocatalysts, where intercalated chiral molecules manipulate spin dynamics to improve reaction kinetics and selectivity.