The pathway for efficient catalytic hydrodeoxygenation of biomass represents a powerful, yet challenging route for production of value-added liquid fuels. Herein, we describe a one-step synthetic approach to fabricate WO 2.72 decorated with atomically dispersed palladium atoms that bond covalently to the nearby oxygen atoms. The presence of isolated palladium atoms is confirmed by spherical aberration correction electron microscopy, extended X-ray absorption fine structure measurement, and diffuse reflectance infrared Fourier transform spectroscopy. This catalyst manifests outstanding catalytic performance in hydrodeoxygenation of vanillin to yield 2-methoxy-4-methylphenol (MMP) efficiently and selectively, along with exceptional stability and scalability. Density functional theory (DFT) calculations indicate that this high activity results from the unique electronic structure of isolated palladium atoms confined in defective WO 2.72 . These findings may pave the way for the facile creation of single atom catalysts in a coordination-engineered strategy for the advance of single atom catalysis.
Metal–support interactions are of great importance in determining the support-activity in heterogeneous catalysis. Here we report a low-temperature synthetic strategy to create atomically dispersed palladium atoms anchored on defective hexagonal boron nitride (h-BN) nanosheet. Density functional theory (DFT) calculations suggest that the nitrogen-containing B vacancy can provide stable anchoring sites for palladium atoms. The presence of single palladium atoms was confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurement. This catalyst showed exceptional efficiency in chemoselective hydrogenation of cinnamaldehyde, along with excellent recyclability, sintering-resistant ability, and scalability. We anticipate this synthetic approach for the synthesis of high-quality SACs based on h-BN support is amenable to large-scale production of bench-stable catalysts with maximum atom efficiency for industrial applications.
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