Fe-N_4 Sites Embedded into Carbon Nanofiber Integrated with Electrochemically Exfoliated Graphene for Oxygen Evolution in Acidic Medium

摘要

Development of inexpensive and efficient oxygen evolution reaction (OER) catalysts in acidic environment is very challenging, but it is important for practical proton exchange membrane water electrolyzers. A molecular iron-nitrogen coordinated carbon nanofiber is developed, which is supported on an electrochemically exfoliated graphene (FeN4/NF/EG) electrocatalyst through carbonizing the precursor composed of iron ions absorbed on polyaniline-electrodeposited EG. Benefitting from the unique 3D structure, the FeN4/NF/EG hybrid exhibits a low overpotential of approximate to 294 mV at 10 mA cm(-2) for the OER in acidic electrolyte, which is much lower than that of commercial Ir/C catalysts (320 mV) as well as all previously reported acid transitional metal-derived OER electrocatalysts. X-ray absorption spectroscopy coupled with a designed poisoning experiment reveals that the molecular Fe-N-4 species are identified as active centers for the OER in acid. The first-principles-based calculations verify that the Fe-N-4-doped carbon structure is capable of reducing the potential barriers and boosting the electrocatalytic OER activity in acid.