Journal
NANO RESEARCH
Volume 14, Issue 11, Pages 4347-4355Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-021-3857-2
Keywords
heterogeneous catalysis; photochemical reduction; palladium single atoms and clusters; atomic dispersion; hydrodeoxygenation; vanillin
Categories
Funding
- China Postdoctoral Science Foundation [2019M661247, 2020T130091]
- Postdoctoral Science Foundation of Heilongjiang Province [LBH-Z19047]
- Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China [719900091]
- Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education
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This study presents a novel palladium catalyst with exceptional activity and selectivity for the hydrodeoxygenation of vanillin to produce 2-methoxy-4-methylphenol. The catalyst features atomically dispersed palladium single atoms and clusters, along with strong metal-support interactions, leading to superior catalytic performance and potential for the design of fully exposed metal catalysts.
Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals. Herein, we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31 (SAPO-31) as a highly active, chemoselective, and reusable catalyst for hydrodeoxygenation of vanillin. Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed, without forming strong palladium-palladium metallic bonding, over the SAPO-31 support. This catalyst, with a full metal availability to the reactants, exhibits exceptional catalytic activity (TOF: 3,000 h(-1), Yield: > 99%) in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol (MMP) under mild conditions (1 atm, 80 degrees C, 30 min), along with excellent stability, scalability (up to 100-fold), and wide substrate scope. The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters, as well as the strong metal-support interactions. This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.
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