Chirality Engineering of Nanostructured Copper Oxide for Enhancing Oxygen Evolution from Water Electrolysis

Abstract The exploration of a new conceptual strategy for improving the oxygen evolution reaction (OER) of earth‐abundant electrocatalysts is critical. In this study, chiral copper oxide nanoflower is explored by a self‐assembly method. The characterization suggests the chiral structure originates from the crystal plane‐level helical stack of the secondary nanosheets. Of note, the assembly illustrates a record‐high degree of spin polarization of 96%, indicating the ideal alignment of electron spin. Moreover, density function theory calculations show the chiral structure reducing the reaction energy barrier (REB) while switching the potential‐determining step from *O→*OOH to *OH→*O. Together with the enhanced electrochemical active surface area and accelerated charge transfer, the production of ground‐state triplet O 2 is improved via a spin‐forbidden route that involves the singlet H 2 O/OH•. Consequently, the chiral nanoflower shows a overpotential of 308 mV at 10 mA cm −2 and a Tafel slope of 93.5 mV dec −1 , which is even superior to the commercial RuO 2 (310 mV, 101 mV dec −1 ). This study presents a new strategy for improving the OER activity by simultaneously enhancing electronic properties and lowering the REB of an non‐noble electrocatalyst via chirality engineering.