Construction of Pd-doped RuO2 nanosheets for efficient and stable acidic water oxidation

Abstract

RuO2 has been considered a potential alternative to commercial IrO2 for the oxygen evolution reaction (OER) due to its superior intrinsic activity. However, its inherent structure dissolution in acidic environments restricts its commercial applications. In this study, we report a novel Pd-doped ruthenium oxide (Pd–RuO2) nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure. The catalyst exhibits excellent performance, achieving an overpotential of only 204 mV at a current density of 10 mA cm−2. Impressively, after undergoing 8000 cycles of cyclic voltammetry testing, the overpotential merely decreased by 5 mV. The PEM electrolyzer with Pd0.08Ru0.92O2 as an anode catalyst survived an almost 130 h operation at 200 mA cm−2. To elucidate the underlying mechanisms responsible for the enhanced stability, we conducted an X-ray photoelectron spectroscopy (XPS) analysis, which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru, thus playing a crucial role in enhancing the catalyst's stability. Furthermore, density functional theory (DFT) calculations provide compelling evidence that the introduction of Pd into RuO2 effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru, thereby preventing the over-oxidation of Ru. Additionally, the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles, further bolstering the structural integrity of the catalyst.

Keywords

• Oxygen evolution reaction
• Pd-doped ruthenium oxide
• Two-dimensional structure
• Electron transfer
• Stability