LAUSR

Trifunctional electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are crucial for many electrochemical devices. Herein, novel trifunctional electrocatalysts of a hierarchically-structured Pt/NiO/Ni/CNT with ultrasmall Pt nanoparticles (∼2 nm) were synthesized via substrate-enhanced electroless deposition. The resulting catalysts exhibited a higher ORR activity (half-wave potential at 0.942 V) than that of the benchmark commercial Pt/C (20 wt%) and a similar OER activity (overpotential of 350 mV at 10 mA cm-2) to that of RuO2 in alkaline media. Moreover, the newly-developed Pt/NiO/Ni/CNT catalysts also showed a high mass activity superior to Pt/C towards the HER in both acid and alkaline electrolytes. The Pt/NiO/Ni/CNT catalysts, when used for overall water splitting, self-powered by two Zn-air batteries with the Pt/NiO/Ni/CNT air electrodes connected into series, displayed superb performance with 1.61 V at 10 mA cm-2. This work represents a breakthrough in the development of facile approaches to trifunctional catalysts from low-cost Earth-abundant materials for efficient energy conversion and storage.