Electrocatalytic overall water splitting is a promising approach for hydrogen production, and the rational design of the catalyst on the atomic level is critical for decreasing the energy barrier in both hydrogen and oxygen evolution reactions (HER/OER). Herein, we report an NiIr single atom alloy loaded NiFe-LDH (NiIrSAA-NiFe-LDH) and Ir single atom loaded NiFe-LDH (IrSAC-NiFe-LDH) for overall water splitting. The Ir single atoms are found via EXAFS fitting and DFT calculations to be located on the top of Fe3+ with Ir–O6 coordination on IrSAC-NiFe-LDH. The as-prepared NiIrSAA-NiFe-LDH presents an overpotential of 28.5 mV at 10 mA cm–2 in the HER and IrSAC-NiFe-LDH exhibits an overpotential of 194 mV at 10 mA cm–2 in the OER, respectively. Moreover, the electrolyzer assembled by NiIrSAA-NiFe-LDH and IrSAC-NiFe-LDH presents a low cell voltage of 1.49 V at 10 mA cm–2 and a long-term stability of over 120 h at 200 mA cm–2 in overall water splitting with an estimated cost of US $1.12 per kilogram of H2, meeting the target raised by the US Department of Energy (

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Introducing different active sites into heterogeneous catalysts provides new prospects to address the challenges in single-atom catalysis. Herein, the Au single atoms together and the Au nanoparticles were loaded onto...

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