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Catalytic dehydrogenation and hydrogenation of amines and alcohols are important in the synthesis of fine chemicals. Despite several efficient homogeneous catalysts having been identified, highly active heterogeneous catalysts remain elusive, although they would meet an unmet need. Here, we show that bimetallic Pd-Au nanoparticles with Pd-to-Au molar ratios of 3:1 immobilized on multiwall carbon nanotubes (Pd 3 Au 1 /CNT) display high catalytic activity in the oxidant-free and acceptorless dehydrogenation and hydrogenation of N- and O-containing heterocyclic compounds, amines/imines, and alcohols/ketones. Transmission electron microscopy analysis demonstrates the preferential exposure of Pd 3 Au 1 (111) facets on the Pd 3 Au 1 /CNT catalyst. Mechanistic insights combining experimental data with density functional theory calculations reveal that the Pd 3 Au 1 (111) surface enhances both dehydrogenation and hydrogenation reactions and provides a rationale for the observed enhancements.

Acceptorless dehydrogenation and hydrogenation of N- and O-containing compounds on Pd 3 Au 1 (111) facets

Acceptorless dehydrogenation and hydrogenation of N- and O-containing compounds on Pd ₃ Au ₁ (111) facets