Partial oxidation of Rh/Ru nanoparticles within carbon nanofibers for high-efficiency hydrazine oxidation-assisted hydrogen generation.

ABSTRACT

Hydrazine oxidation reaction (HzOR), an alternative to oxygen evolution reaction, effectively mitigates hydrazine pollution while achieving energy-efficient hydrogen production. Herein, partially oxidized Ru/Rh nanoparticles embedded in carbon nanofibers (CNFs) are fabricated as a bifunctional electrocatalyst for hydrogen evolution reaction (HER) and HzOR. The presence of multiple components including metallic Ru and Rh and their oxides provides numerous electrochemically active sites and superior charge transfer properties, thus improving the electrocatalytic performance. Additionally, the confinement of the active components within CNFs further enhances structural stability. Consequently, the optimized electrocatalyst exhibits ultralow overpotentials of 16 mV at 10 mA cm-2 and 176 mV to reach an industry-level current density of 1 A cm-2 for HER, considerably outperforming the benchmark Pt/C catalyst. Furthermore, it shows an outstanding anodic HzOR activity, achieving a small potential of -0.019 V to generate 10 mAcm-2. A two-electrode overall hydrazine splitting (OHzS) cell prepared using the electrocatalyst operates at a compelling voltage that is 1.953 V lower than that of the overall water splitting (OWS) cell at 200 mA cm-2. Furthermore, the OHzS cell achieves a hydrogen production rate of 1.17 mmol h-1, which is 15-fold that of OWS. Additionally, Rh1Ru1Ox-CNFs-350 is used to construct a Zn-hydrazine battery with excellent performance. This study presents an effective system for achieving high-yielding green H2 production with low energy consumption while simultaneously addressing hydrazine pollution.