Abstract
High Resolution Image Download MS PowerPoint Slide In this work, we explored the catalytic decomposition of methanol to syngas at 300 °C using intermetallic Ni 3 Sn 2 nanoparticles (NPs) synthesized via a chemical route. Our study employed a comprehensive approach combining operando Ambient Pressure soft X-ray absorption spectroscopy with a suite of ex situ techniques─including X-ray diffraction, X-ray photoelectron spectroscopy, electron microscopy, and Mössbauer spectroscopy─and density functional theory (DFT) calculations. Consistent with the behavior observed in Ni 3 Sn 2 single crystals, we found that the Ni–Sn bonds stabilize the unique electronic structure of the intermetallic Ni active sites, even under strongly oxidizing conditions. Additionally, the nanoparticles exhibit a distinctive morphology characterized by a SnO x -rich protective shell, which further enhances the stability of the Ni sites. These stabilized sites enable the selective decomposition of CH 3 OH into H 2 and CO while effectively suppressing coke formation, a major limitation of conventional metallic Ni catalysts, which are currently a benchmark for this reaction. Our findings suggest a promising strategy for the design of scalable, stable, and cost-effective Ni-based catalysts, unlocking the full potential of methanol as a liquid, portable hydrogen carrier.