Polymer‐Derived Nickel‐Iron Silicide‐Based Bimetallic Catalysts: Synthesis, Characterization, and Enhanced Catalytic Properties Toward the Oxygen Evolution Reaction

The growing demand for green energy highlights the need for efficient hydrogen production through water splitting. Designing bimetallic electrocatalysts is crucial for this goal. Transition metal silicides are promising due to their abundance and high electrical conductivity. Here, a novel Ni2Si/FexSiy/SiOC composite was synthesized via a polymer‐derived ceramics (PDCs) route using a single‐source precursor (SSP). The SSP was prepared by modifying a high‐carbon polysiloxane (SPR‐684) with nickel and iron acetylacetonates. Fourier transform infrared spectroscopy (FT‐IR) analysis confirmed the formation of SiOM (M = Fe, Ni) bonds, indicating chemical incorporation of metals. During pyrolysis, in situ formed carbon coated the active sites, enhancing conductivity. The resulting Ni2Si/FexSiy/SiOC catalyst showed a low overpotential of 323 mV versus RHE at 10 mA cm−2disk (0.25 mg cm−2 loading) under alkaline conditions, attributed to the synergy of Fe and Ni in improving the oxygen evolution reaction (OER). X‐ray absorption spectroscopy (XAS) reveals surface reconstruction of NiFe silicide toward a hydroxide during OER. Compared to previous Ni2Si/SiOC systems, the dual‐metal design notably enhanced catalytic performance. This study presents the successful synthesis of NiFe silicide catalysts for OER via the PDCs approach, demonstrating tunability of properties by the nickel to iron ratio, promising potential for water‐splitting and broader electrocatalytic applications.