CeCO3F-NiFe-LDH/NF System: A Comprehensive Study of Structural Morphological, and Electronic Effects on Oxygen Evolution Reaction
摘要
Developing efficient, durable, and cost-effective electrocatalysts for the oxygen evolution reaction (OER) is crucial for sustainable energy systems. NiFe-LDH is a promising OER catalyst but suffers from limited conductivity, agglomeration, and moderate intrinsic activity. Herein, we stabilize Ce within NiFe-LDH via a unique CeCO3F phase resulting (CeCO3F-NiFe-LDH/NF) as improved OER catalyst. This induces (i) nanoscale exfoliation into thinner nanosheets, (ii) oxygen deficient surface specie, and (iii) high-valence Ni/Fe species. Consequently, catalyst achieving an overpotential of 193 mV and 234 mV to deliver a current density of 10 mA cm-2 and 100 mA cm-2 respectively with a small Tafel slope of 70 mV dec-1. Comprehensive characterization reveals that the synergistic co-doping of Ce and F induces multifaceted enhancements: Ce promotes high-valence Ni/Fe species and according to XPS analysis, the formation of oxygen-deficient surface specie, which aid the charge compensation, while F⁻ incorporation creates atomic-level point defects and induces lattice strain. Furthermore, the in-situ formed CeCO3F phase acts as a structural modifier, leading to nanoscale exfoliation into thinner nanosheets and the creation of a conductive framework. These synergistic effects collectively enhance charge transfer kinetics, increase the number of active sites, increase the electrochemically active surface area, and boost the intrinsic activity of active sites. The catalyst also demonstrates excellent stability over 27 h of operation. This work highlights rational heteroatom co-doping as a promising strategy for designing high-performance, non-precious metal-based electrocatalysts.