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 (NPy)-mediated strategy to regulate the SMSI between NPy 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@NPy−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 H2SO4, 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 NPy−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.
Zhao et al. (Wed,) studied this question.