Adaptive Strong Metal-Support Interactions Enabled by Pyridinic Nitrogen Regulate Hydrogen Kinetics on Ruthenium for pH-Universal Hydrogen Evolution

High Resolution Image Download MS PowerPoint Slide Ruthenium (Ru)-based catalysts exhibit high efficiency for the hydrogen evolution reaction (HER), and interactions between Ru and carbon-based substrates can be used to optimize adsorption behavior. However, precisely engineering strong metal-support interactions (SMSIs) remains a significant challenge. Herein, we report a pyridinic-nitrogen (N Py )-mediated strategy to regulate the SMSI between N Py and Ru nanocrystals, thereby significantly enhancing their catalytic performance for the HER under alkaline, acidic, and seawater conditions. At an overpotential of 100 mV, the optimized Ru@N Py −C achieved a turnover frequency (TOF) of 13.6 s −1 in 1.0 M KOH and 7.2 s −1 in 0.5 M H 2 SO 4, corresponding to enhancements of approximately 13-fold and 1.8-fold compared with Pt/C (1.0 and 4.1 s −1 ), respectively. Structural characterizations and theoretical results show that the N Py −C induces optimization of the Ru nanostructure and electronic energy levels, resulting in a slight downward shift of the d -band center of Ru and thereby tuning the Ru−H binding strength toward a more favorable range. Benefiting from the SMSI, the electrode reached 400 mA cm −2 at 191 mV in alkaline seawater and maintained continuous operation for 300 h in neutral seawater.