One-step synthesis of single palladium atoms in WO2.72 with high efficiency in chemoselective hydrodeoxygenation of vanillin

• Published in: Applied catalysis. B, Environmental Environmental, 2021-12, Vol.298, p.120535, Article 120535
• Main Authors: Li, Zhijun, Lu, Xiaowen, Sun, Weiwei, Leng, Leipeng, Zhang, Mingyang, Li, Honghong, Bai, Lu, Yuan, Dundong, Horton, J. Hugh, Xu, Qian, Wang, Jun
• Format: Article
• Language: English
• Subjects: Catalysis; Catalysts; Catalytic activity; Chemical bonds; Coordination environments; Density functional theory; Electron microscopy; Electronic structure; Fine structure; Fourier transforms; Heterogeneous catalysis; Hydrodeoxygenation; Liquid fuels; Oxygen atoms; Palladium; Palladium single atom catalyst; Single atom catalysts; Ultrastructure; Vanillin; X ray absorption
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2021.120535

[Display omitted] •Atomically dispersed palladium atoms supported over WO2.72 was created by a one-step synthetic approach.•Density functional theory calculations reveal that WO2.72 can provide stable anchoring sites for palladium atoms.•This catalyst shows excellent catalytic efficiency in hydrodeoxygenation of vanillin to yield MMP.•The high catalytic activity originates from unique electronic structure of isolated palladium atoms confined in WO2.72. 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 WO2.72 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 WO2.72. 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.