Unraveling the Synergistic Role of Sm3+ Doped NiFe‐LDH as High‐Performance Electrocatalysts for Improved Anion Exchange Membrane and Water Splitting Applications

Abstract Effective first‐row transition metal‐based electrocatalysts are crucial for large‐scale hydrogen energy generation and anion exchange membrane (AEM) devices in water splitting. The present work describes that SmNi 0.02 Fe‐LDH nanosheets on nickel foam are used as a bifunctional electrocatalyst for water splitting and AEM water electrolyzer study. Tuning the Ni‐to‐Fe ratios in NiFe‐LDH and doping with Sm ions improves the electrical structure and intrinsic activity. SmNi 0.02 Fe‐LDH has higher oxygen evolution reaction (OER), HER, and TWS activity, achieving 10 mA cm⁻ 2 current density at lower overpotentials (230 mV, 95 mV, and 1.62 V, respectively). In AEMWE cells, SmNi 0.02 Fe‐LDH as a cathode and anode pair exhibits outstanding activity (0.9 A cm⁻ 2 at 2 V) and stability over 120 h. Density Functional Theory (DFT) investigations reveal that the Sm doping in NiFe‐LDH surface enhances its bifunctional activity toward OER and HER. These findings emphasize the potential of non‐noble composites for long‐term water electrolysis in total water splitting and AEMWE applications.