Molecular precursor synthesis of the Rh2O3/Fe2O3 spherical architecture for enhanced acidic HER activity and durability

W4414266184 · 수집 2026-10-04 18:16:39

T10030 Electrocatalysts for Energy Conversion

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Efficient hydrogen evolution catalysts that minimize noble metal content while maintaining high activity and durability are critically needed for scalable water electrolysis. Here, we introduce a molecular precursor strategy to synthesize intimately intermixed Rh2O3/Fe2O3 nanocomposites with precisely controlled 1 : 1 metal ratio. Thermal decomposition of heterobimetallic complex [Rh(acac)3Fe(hfac)2] (acac = acetylacetonate, hfac = hexafluoroacetylacetonate) at 300 °C yields 3D spherical Rh2O3/Fe2O3 architectures without high-temperature sintering. Electrochemical evaluation reveals that Rh2O3/Fe2O3 requires only 32 mV to reach -10 mA cm-2, dramatically lower than Rh/Rh2O3 (140 mV), commercial Rh2O3 (260 mV), or α-Fe2O3 (210 mV). The Tafel slope investigation of Rh2O3/Fe2O3 indicates a Volmer-Heyrovsky mechanism with facile proton adsorption and electron transfer, while electrochemical impedance spectroscopy shows its charge-transfer resistance is an order of magnitude lower than that of Rh/Rh2O3. Importantly, chronopotentiometry at -10 mA cm-2 reveals ultrastable performance with no observable decay over 120 hours, highlighting the exceptional long-term stability of Rh2O3/Fe2O3. Post-stability microscopy exhibits intact spherical architecture with no signs of sintering or Ostwald ripening. By integrating earth-abundant sesquioxide that promotes oxophilicity, oxygen-vacancy generation, and enhanced conductivity, the title Rh2O3/Fe2O3 catalyst uses less than half the Rh loading of Rh/Rh2O3 while delivering both superior activity and unmatched durability. This work establishes that although both individual Rh2O3 and Fe2O3 oxides exhibit poor HER activity and stability in acidic media, their intimately intermixed nanocomposite delivers dramatically enhanced performance and long-term stability. The reported mixed-oxide electrocatalyst overcomes the intrinsic limitations of single-phase oxides and provides general guiding principles for designing future high-performance mixed-oxide systems.

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Molecular precursor synthesis of the Rh<sub>2</sub>O<sub>3</sub>/Fe<sub>2</sub>O<sub>3</sub> spherical architecture for enhanced acidic HER activity and durability

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