Enhancing oxygen evolution reaction performance of Ruddlesden–Popper perovskite oxide through heteroatom incorporation
Prior studies have demonstrated that Ruddlesden–Popper (RP) type perovskite oxides exhibit promising electrocatalytic properties for oxygen evolution reaction (OER). However, the limited electrocatalytic activity has impeded their widespread utilization. The incorporation of heteroatoms into the Ruddlesden–Popper type structure has been identified as an effective strategy to enhance the electrocatalytic performance. This research presents the systematic design and synthesis of RP type perovskite oxide LaSrFeO 4 (LSFO), followed by the optimization of electrocatalytic activity through Ni substitution at the Fe site of SLFO to create LaSrFe 1- x Ni x O 4 (LSFNO- x , x = 0.2, 0.4, and 0.5). Therein, the LSFNO-0.4 sample achieved a current density of 10 mA·cm −2 with an overpotential of only 340 mV. Additionally, it displayed exceptional stability over 120 h in a 1.0 M KOH solution. Both experimental and theoretical studies suggest that the addition of Ni cation increases the Fe − O covalency, and impacts the morphology and surface electron density of LSFO. This substitution results in a greater electrochemically active surface area, improved electron transfer, and optimization of hydrogen/water absorption free energy. This study presents a successful approach for enhancing the OER performance of Ruddlesden–Popper LSFO through the deliberate control of Fe − O covalent bonding.
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