Exsolution of Ru Nanoparticles on BaCe0.9Y0.1O3-delta Modifying Geometry and Electronic Structure of Ru for Ammonia Synthesis Reaction Under Mild Conditions

Abstract

Green ammonia is an efficient, carbon-free energy carrier and storage medium. The ammonia synthesis using green hydrogen requires an active catalyst that operates under mild conditions. The catalytic activity can be promoted by controlling the geometry and electronic structure of the active species. An exsolution process is implemented to improve catalytic activity by modulating the geometry and electronic structure of Ru. Ru nanoparticles exsolved on a BaCe0.9Y0.1O3-delta support exhibit uniform size distribution, 5.03 +/- 0.91 nm, and exhibited one of the highest activities, 387.31 mmol(NH3) g(Ru)(-1) h(-1) (0.1 MPa and 450 degrees C). The role of the exsolution and BaCe0.9Y0.1O3-delta support is studied by comparing the catalyst with control samples and in-depth characterizations. The optimal nanoparticle size is maintained during the reaction, as the Ru nanoparticles prepared by exsolution are well-anchored to the support with in-plane epitaxy. The electronic structure of Ru is modified by unexpected in situ Ba promoter accumulation around the base of the Ru nanoparticles.