Single-atom electrocatalysts (SAEs) can realize the target of low-cost by maximum atomic efficiency. However, they usually suffer performance decay due to high energy states, especially in a harsh acidic water splitting environment. Here, we conceive and realize a double protecting strategy that ensures robust acidic water splitting on Ir SAEs by dispersing Ir atoms in/onto Fe nanoparticles and embedding IrFe nanoparticles into nitrogen-doped carbon nanotubes (Ir-SA@Fe@NCNT). When Ir-SA@Fe@NCNT acts as a bifunctional electrocatalyst at ultralow Ir loading of 1.14 μg cm −2 , the required overpotentials to deliver 10 mA cm −2 are 250 and 26 mV for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in 0.5 M H 2 SO 4 electrolyte corresponding to 1370-and 61-fold better mass activities than benchmark IrO 2 and Pt/C at an overpotential of 270 mV, respectively, resulting in only 1.51 V to drive overall water splitting. Moreover, remarkable stability is also observed compared to Pt/ C-IrO 2 .

A palladium phosphide electrocatalyst supported on carbon black (PdP2@CB) shows efficient water splitting in both alkaline and neutral electrolytes. Significantly lower overpotentials are required for PdP2@CB (27.5 mV in 0.5 m H2SO4; 35.4 mV in 1 m KOH; 84.6 mV in 1 m PBS) to achieve a HER electrocatalytic current density of 10 mA cm−2 compared to commercial Pt/CB (30.1 mV in 0.5 m H2SO4; 46.6 mV in 1 m KOH; 122.7 mV in 1 m PBS). Moreover, no loss in HER activity is detectable after 5000 potential sweeps. Only 270 mV and 277 mV overpotentials are required to reach a current density of 10 mA cm−2 for PdP2@CB to catalyze OER in 1 m KOH and 1 m PBS electrolytes, which is better OER activity than the benchmark IrO2 electrocatalyst (301 mV and 313 mV to drive a current density of 10 mA cm−2). 1.59 V and 1.72 V are needed for PdP2@CB to achieve stable water splitting catalytic current density of 10 mA cm−2 in 1 m PBS and 50 mA cm−2 in 1 m KOH for 10 h, respectively.

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A palladium phosphide electrocatalyst supported on carbon black (PdP2@CB) shows efficient water splitting in both alkaline and neutral electrolytes. Significantly lower overpotentials are required for PdP2@CB (27.5 mV in 0.5 m H2SO4; 35.4 mV in 1 m KOH; 84.6 mV in 1 m PBS) to achieve a HER electrocatalytic current density of 10 mA cm−2 compared to commercial Pt/CB (30.1 mV in 0.5 m H2SO4; 46.6 mV in 1 m KOH; 122.7 mV in 1 m PBS). Moreover, no loss in HER activity is detectable after 5000 potential sweeps. Only 270 mV and 277 mV overpotentials are required to reach a current density of 10 mA cm−2 for PdP2@CB to catalyze OER in 1 m KOH and 1 m PBS electrolytes, which is better OER activity than the benchmark IrO2 electrocatalyst (301 mV and 313 mV to drive a current density of 10 mA cm−2). 1.59 V and 1.72 V are needed for PdP2@CB to achieve stable water splitting catalytic current density of 10 mA cm−2 in 1 m PBS and 50 mA cm−2 in 1 m KOH for 10 h, respectively.

Rh–Rh2P@C exhibits 4 fold better HER mass activity than commercial Pt/C in both alkaline and acidic mediums.