Abstract
It was synthesized an Fe-coordination compound (CC) [FeCl3(Hbta)2] (Hbta = benzotriazole) and an Al-doped Fe-CC via a facile one-step grinding method. Upon subsequent annealing, Fe3O4/C and Al-doped Fe3O4/C were obtained, respectively. In the two obtained calcined samples, Fe3O4 nanopolyhedra are not only anchored on the in-situ generated carbon material, but also coated by graphene-like ultrathin nanosheets. The carbon materials not only provide conductive networks to enhance the electrical conductivity of the composite material, but also prevent the aggregation of Fe3O4 nanopolyhedra. Al-doped Fe3O4/C shows outstanding long-term oxygen evolution reaction (OER) activity during 60 h-electrolysis at 20 mA cm−2 with overpotentials of only 215 and 359 mV at 10 and 100 mA cm−2, respectively. Density functional theory (DFT) calculations reveal that the rate-determining steps (RDS) on the Fe3O4 and Al-doped Fe3O4 surfaces are both the formation of ∗OOH, and the doping of Al3+ into Fe3O4 can lower the ΔG (1.969 eV) and overpotential (0.739 V) of the RDS during the OER process, which is due to the fact that the d-band center of Al-doped Fe3O4 is positively shifted in comparison with that of Fe3O4, thus improving the affinity of the catalytic surface toward ∗OOH.
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