SrRuO3 as a rare conductive perovskite ruthenate has attracted increasing attention for application in energy conversion. Here, the electrocatalytic activity for the hydrogen evolution reaction (HER) of thermally synthesized layered SrRuO3 is investigated and shows a considerable activation during cathodic polarization in alkaline solution. The analysis demonstrates the electrode activation is caused by the increased hydrophilicity of SrRuO3 surface, revealing the influence of the surface properties on HER performance. For further improving the catalytic activity of perovskite ruthenate, the RuO2/SrRuO3 (RSRO) heterostructure is fabricated in situ by reducing the thermal decomposition temperature of 1000 °C for SrRuO3 to 600 °C. The appropriate lattice parameter of SrRuO3 ensures a good lattice match, which results in a strong interaction between SrRuO3 and RuO2. Hence, the RSRO substantially outperforms the corresponding single‐component oxides. In addition, the increased active sites induced by the rapid improvement of hydrophilicity of RSRO surface further highlight its structural advantage for catalytic hydrogen generation. The experimental and theoretical computation results consistently validate the positive synergistic effect among SrRuO3 and RuO2 in tuning the atomic and electronic configuration.

Ru, RuO2, and MoO3 embedded carbon nanorods with superior HER performance were synthesized through electrospinning and subsequent calcination.

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