Publication date: 21st July 2025
Over the last decade, exsolution technique has emerged as a relevant alternative to deposition methods for generation of nanoparticle-based robust catalysts. This exsolution process leads to stable and active nanoparticles anchored to oxide supports, which in turn grants more efficient and durable catalysts for driving high-interest reactions, such as hydrogen production through ammonia cracking. Nevertheless, some challenges remain unsolved for expanding exsolution to certain materials, such as cerium oxide (CeO2)-based systems due to the limited solubility of transition metals.
In this work, CeO2 lattice modifications -partial substitution of Ce with Gd- enabled an adequate introduction of highly-active metals, namely Ru and Rh. Latter exsolution led to highly-dispersed Ru, Rh and -unprecedent- RuRh alloyed nanoparticles formation (ca. 3 nm). These functionalized materials were employed as catalysts for ammonia decomposition process, exhibiting outstanding performance and long-term stability, even outperforming Ru-impregnated materials, especially Ru-exsolved@Ce0.8Gd0.2O2-δ. These exceptional results were achieved despite the notably low metal loading (~0.7 wt.% Ru) and surface areas. Catalytic performance of the exsolved materials was tested under different temperatures and space velocities, leading to efficient hydrogen production along 260 hours, at 600 and 400 ºC (~110 h and ~150 h respectively), with no evidence of degradation affecting the exsolved nanoparticles, nor the support. Lastly, a comparative with other state-of-the-art catalysts evidenced the outstanding potential of exsolved CeO2-based catalysts, which allows the reduction of metal loading requirements, leading to more efficient catalysts.
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