Abstract
In order to clarify competitive reactions between lattice oxygen oxidation mechanism (LOM) with lower energy barrier and conventional adsorbate evolution mechanism (AEM), O-hetero-Fe-N3.6 active site was built in ZIF-derived carbon nanotubes to transform traditional AEM mechanism on iron-unsaturated active site into LOM mechanism during electrocatalytic oxygen evolution reaction (OER). In-situ attenuated total reflectance infrared (ATR-FTIR) and X-ray absorption fine structure results confirmed the formation of Fe-O bonds and a Fe-N3.6 structure, indicating that O-hetero-Fe-N3.6 active sites were built. A key intermediate O* was detected on ATR-FTIR, which suggests that OER proceeded via LOM mechanism. The alkaline OER activity and stability are enhanced on the O-hetero-Fe-N3.6 active sites to accelerate rate-determining step of water oxidation. The ZIF-derived carbon nanotubes expose more O-hetero-Fe-N3.6 active sites to facilitate electron and mass transfer during electrocatalytic OER. The Fe-NC catalyst exhibits excellent OER activity with an overpotential of 235 mV at 10 mA cm−2 and Tafel slope of 98 mV dec−1 in 1 M KOH.
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