Developing highly active, cost-effective and stable electrocatalysts for oxygen evolution reaction (OER) is critical to renewable energy systems. Herein, we demonstrate a H2O2-assisted etching method to synthesize mesoporous NiFe layered double hydroxide nanosheets (LDHs) on nickel foam (NF) (NiFe LDHMs/NF). The NiFe LDHMs/NF processed with 200 μL H2O2 exhibited excellent OER performance with an extraordinarily low overpotential of 170 mV at 10 mA cm -2 in 1 M KOH, as well as superior kinetics with a Tafel slope of 39.3 mV dec -1 , being the one of the best non-precious electrocatalysts reported to date. Density functional theory (DFT) calculations revealed that the excellent OER performance arose from pseudo re-oxidized meta-stable Ni 3+ , which evidently suppressed 3d-eg of Ni-site and elevated d-band center towards competitively low electron-transfer barrier. The Fe-sites within the system robustly preserved Ni oxidation state and maintained electron-transfer activities. This protocol is applicable to developments of high-efficiency non-precious metal OER electrocatalysts.
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