Deep Reconstruction of Ruthenate Perovskite Oxide Enables Efficient pH-Universal Hydrogen Evolution Reaction

Designing highly efficient, stable, and pH-universal perovskites for hydrogen evolution reaction (HER) is urgently needed yet remains a grand challenge. Herein, a titanium-containing strontium ruthenate (SrTi0.5Ru0.5O3, STRO) is developed as an excellent HER electrocatalyst in a wide pH range. The introduction of Ti into SrRuO3 significantly reduces the size of STRO, endowing with a high reactivity that facilitates a deep surface-reconstruction during HER. Furthermore, Sr2+ leaching triggered reconstruction leads to STRO breaking into tiny nanoparticles accompanied by high-valence ruthenium (Ru) species reducing to metallic Ru. The generated active species, increased accessible sites, and improved electrical conductivity greatly boost HER. The reconstructed STRO displays remarkable HER activities with exceptional low overpotentials of 18, 24, and 55 mV at 10 mA cm-2 in 1 m KOH, 0.5 m H2SO4, and 1 m PBS, respectively, surpassing most perovskites reported previously and comparable to or even outperforming that of commercial Pt/C. Moreover, the STRO exhibits excellent stabilities over 200 h in alkaline and acidic media, superior to that of Pt/C. This work not only provides insights into structure reconstruction of perovskites during HER, but also opens new perspectives for developing high-efficiency and pH-universal electrocatalysts for future energy applications. The SrTi0.5Ru0.5O3 perovskite exhibits dramatic hydrogen evolution reaction (HER) enhancements at all pH values after cyclic voltammetry activation in alkaline media. The Sr2+ leaching triggered reconstruction leads to perovskite breaking into tiny nanoparticles accompanied by high-valence ruthenium (Ru) species reducing to metallic Ru. The increased number of active sites and improved electrical conductivity are responsible for its superior HER performances. image