Monodispersed ruthenium nanoparticles interfacially bonded with defective nitrogen-and-phosphorus-doped carbon nanosheets enable pH-universal hydrogen evolution reaction

Herein, we significantly accelerated the kinetics of hydrogen evolution reaction (HER) by interfacially bonding ruthenium nanoparticles with defect-rich nitrogen and phosphorus co-doped carbon nanosheets (Ru/D-NPC). The optimal Ru/D-NPC therefore achieves ultralow overpotentials of 23, 61, and 68 mV at the current density of 10 mA cm(-2) for HER in alkaline, neutral, and acidic electrolytes, respectively, demonstrating the excellent pH-universal HER activities. Specially, our Ru/D-NPC catalysts represent a 2 x advance in mass activity (639.9 mA/mg(Ru)) compared to benchmarking Pt/C catalysts (320 mA/mg(Pt)) and high per-site activity (0.13 s(-1)) under alkaline conditions while remaining the excellent stability under all pH conditions. We experimentally demonstrated that Ru-N bonds at the interfaces of Ru/D-NPC strengthen the metal-support interaction and modulates the electronic structure of Ru, optimizing the intrinsic HER kinetics and sintering-resistance of active Ru species, as further rationalized by theoretical calculations. This work shines the light on the effect of interfacial bonds on the intrinsic HER kinetics.

Automated summary

In this study, the kinetics of hydrogen evolution reaction (HER) was significantly accelerated by interfacially bonding ruthenium nanoparticles with defect-rich nitrogen and phosphorus co-doped carbon nanosheets. The optimal catalyst achieved ultralow overpotentials in alkaline, neutral, and acidic electrolytes, demonstrating excellent pH-universal HER activities. The study revealed the importance of interfacial bonds in modulating the intrinsic kinetics of HER.