Nanostructured PtBi Alloy Enables Direct Oxidation of Linear -Alcohols to Fatty Acids

ACS CATALYSIS(2023)

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摘要
Nanostructured bimetallic Pt-Bi catalysts are designed by defect engineering of N-doped carbons as the hosts. The optimal catalyst delivers good yields (>98%) in the direct oxidation of C-5-C-9 linear alpha-alcohols to corresponding fatty acids, significantly outperforming activated carbon-supported benchmarks and rivaling the state-of-the-art systems. A combined kinetic and computational study on n-heptanol oxidation as a model reaction unveils the kinetic and thermodynamic origins of the better performance of the PtBi alloy than neat or Bi-modified Pt(111) surfaces. Structure-performance correlations further identify that the metal particle size, surface Bi/Pt ratio, and strong basicity strongly influence the catalyst performance in alcohol oxidation. The creation of nitrogen defects facilitates the formation of the surface PtBi alloy and brings strong basicity, accounting for the boosted performance. These findings enable a step closer toward the manufacture of valuable fatty acids from abundant coal by coupling the advanced oxidation with the recently piloted higher alcohol synthesis via the Co-Co2C-catalyzed Fischer-Tropsch reaction.
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关键词
aliphatic alcohol oxidation, fatty acids, nitrogen-dopedcarbon, mechanism, PtBi alloy
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