Modulation in the d Band of Ir by Core–Shell Construction for Robust Water Splitting Electrocatalysts in Acid

The realization of commercialization of proton electrolyte membrane water splitting technology significantly depends on the anodic electrocatalyst working at a high potential and strong acidic conditions requiring superior oxygen evolution reaction activity and stability. In this work, we devise the construction of ultrasmall [email protected] core–shell nanoparticles (5 nm) with atomic layer Ir (3 atomic layers) on carbon nanotubes ( [email protected] /CNT) as an exceptional bifunctional electrocatalyst in acidic water splitting. Due to the core–shell structure, strain generated at heterointerfaces leads to an upshifted d band center of Ir atoms contributing to a 62-fold better mass activity at 1.63 V vs RHE than commercial IrO 2; besides, the electronic hybridization suppresses the electrochemical dissolution of Ir; as a result, robust stability is also achieved. In hydrogen evolution reaction catalysis, [email protected] /CNT exhibits a 3.7 times higher mass activity than Pt/C. Furthermore, only 1.7 V is required to reach a water splitting current density of 100 mA cm –2, 251 mV lower than that of Pt/C–IrO 2, indicating its superiority in acidic water splitting.