The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

Abstract Exploring efficient transition‐metal‐based electrocatalysts for oxygen evolution reaction (OER) is imperative but remain challenging for sustainable energy storage and conversion systems. Foreign species doping is a significant regulation strategy to enhance the intrinsic activity of host matrix. However, the potential relationship of structure‐activity caused by guest doping elements is seldom tracked systematically. In this case, both theoretical screening and experimental verification are complementarily employed to investigate the guest doping effects of ten first‐row transition metals (Sc∼Zn) on bimetallic NiCo layered double hydroxide (NiCo‐LDH). As a result, the optimized Fe‐doped NiCo‐LDH is identified as the most promising candidate toward alkaline electrocatalytic OER, which exhibits the quasi‐industrial current density of 1000 mA cm −2 at overpotential of 400 mV. Meanwhile, it also shows impressively long‐term stability of 500 h at 500 mA cm −2 with a negligible activity loss. Moreover, in situ electrochemical Raman spectroscopy unveils the dynamic structure evolution from pre‐catalytic state (Fe‐NiCo‐LDH) to metal oxyhydroxide (Fe‐(NiCo)OOH) during the oxidation reaction, and ab‐initio molecular dynamics simulations are further performed to confirm the thermodynamic stability of activated Fe‐(NiCo)OOH phase. This work provides a promising platform for exploring the critical role of transition metal guest doping on host matrix in developing industrially required OER electrocatalysts.