The atomic dispersion of precious metals accompanied by maximum atom utilization can provide specific chemical properties compared to nanoparticles and clusters that have attracted widespread interest. The selection of a suitable carrier to stabilize platinum atoms while maintaining high stability and propylene selectivity is of great challenge for propane dehydrogenation reactions operating at extremely high temperatures. Here, we report a conceptually designed catalyst comprising isolated Pt atoms stably bonded through skeleton O in a hierarchical-like heteroatomic ferrosilicate zeolite (H-Fe-S-1−3; denoted as "Fe-3"), capable of achieving high propane conversions at different temperatures and atmospheres close to the thermodynamic limit. No significant deactivation was observed for 3 days in a pure propane atmosphere at 580 °C, outperforming most of the cuttingedge Pt-based catalysts. The moderate acidity of Fe-3 and anchoring of hydroxyl species other than silanol nests were responsible for maintaining a suitable C−H break rather than an excessive C−C cleavage capacity and a high degree of Pt dispersion, respectively. X-ray absorption spectra and atomically resolved high-angle annular dark-field electron microscopy demonstrated major atomic dispersion of Pt species, along with complementary density functional theory calculations to determine the structure of �Si−O−Pt−O−Fe� corresponding to the T4 location as the key active site. Pt anchoring by sites other than the T4 site with analogous energies, such as T6, could be accountable for the observation that "cluster-like Pt species" are essentially composed of isolated Pt atoms not interacting with each other.
The Pt1/Co3O4-c catalysts exhibit great catalytic activities in hydrolytic dehydrogenation of ammonia borane (AB) with a specific rate of 6035 molH2 molPt-1 min-1 at room temperature. In-situ DRIFTS spectra and...
Precise adjustment of the electronic structure of heterogeneous
catalysts is an effective strategy to improve their catalytic properties.
By preparing Pd1Ba1/Al2O3 double atom catalysts with a ball milling method as a model catalyst,
we demonstrate an interfacial electronic effect of Pd species induced
by Ba single atoms (SAs) as electronic promoters. The introduction
of Ba SAs promotes the transfer of electrons from Ba atoms to Pd atoms,
forming electron-rich Pdδ+ species. During catalysis,
Pd species with the modification of Ba SAs lower apparent activation
energy and promote H2 dissociation, which dramatically
enhances the catalytic properties in several typical hydrogenation
reactions under mild conditions.
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