Semicrystalline IrO x with Abundant Boundaries for Overall Water Splitting.

Inorganic compounds with different crystalline and amorphous states may show distinct properties in catalytic applications. In this work, we control the crystallization level by fine thermal treatment and synthesize a semicrystalline IrO x material with the formation of abundant boundaries. Theoretical calculation reveals that the interfacial iridium with a high degree of unsaturation is highly active for the hydrogen evolution reaction compared to individual counterparts based on the optimal binding energy with hydrogen (H*). At the heat treatment temperature of 500 °C, the obtained IrO x -500 catalyst has dramatically promoted hydrogen evolution kinetics, endowing the iridium catalyst with a bifunctional activity for acidic overall water splitting with a total voltage of only 1.554 V at a current density of 10 mA cm -2 . In light of the remarkable boundary-enhanced catalysis effects, the semicrystalline material should be further developed for other applications.