Layered double hydroxides (LDHs) are emerging as efficient oxygen evolution reaction (OER) electrocatalysts due to their structural advantages and compositional flexibility. Despite their promise, Mn-based LDHs are hampered by poor conductivity, limiting their OER efficacy. This research introduces a hydrothermal and chemical etching technique to fabricate NF/NiMn LDH@NiMnFe(OH)x structures, significantly improving OER performance. The study reveals that integrating Fe3+ into the NiMn LDH fosters a synergistic Ni–Fe interaction, markedly boosting electrocatalytic efficiency. The NF/NiMn LDH@NiMnFe(OH)x-90 shows a low overpotential of 250 mV at 10 mA cm−2 and a Tafel slope of 49.9 mV dec−1 in 1 M KOH, surpassing both its NM precursor and other Ni-based LDH catalysts, including commercial RuO2. In situ, Raman spectroscopy indicates a pivotal phase transition in NF/NiMn LDH@NiMnFe(OH)x to NiOOH at elevated potentials, essential for OER activity. Raman peaks at 463 and 585 cm−1 confirm this structural evolution. The OER activity boost is attributed to increased oxygen vacancies and enhanced conductivity. Moreover, NF/NiMn LDH@NiMnFe(OH)x-90 maintains stability with negligible degradation after 24 h, underscoring its durability. These findings offer a strategic approach to designing high-performance OER electrocatalysts, leveraging nickel-based layered double-metal oxides for potential water-splitting applications, and emphasize the significance of surface engineering and compositional tuning.
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