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 (Pd₃Au₁/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 Pd₃Au₁(111) facets on the Pd₃Au₁/CNT catalyst. Mechanistic insights combining experimental data with density functional theory calculations reveal that the Pd₃Au₁(111) surface enhances both dehydrogenation and hydrogenation reactions and provides a rationale for the observed enhancements.

胺和醇的催化脱氢和氢化在精细化学品的合成中很重要。尽管已经确定了几种有效的均相催化剂，但高活性的多相催化剂仍然难以捉摸，尽管它们可以满足未满足的需求。在这里，我们表明，固定在多壁碳纳米管（Pd ₃ Au ₁ /CNT）上的Pd/Au摩尔比为3:1的双金属Pd-Au纳米粒子在无氧化剂和无受体的脱氢和氢化中表现出高催化活性。含N和O的杂环化合物、胺/亚胺和醇/酮。透射电子显微镜分析表明Pd ₃ Au ₁ (111)晶面优先暴露在Pd ₃ Au ₁ /CNT催化剂上。实验数据与密度泛函理论计算相结合的机理见解表明，Pd ₃ Au ₁ (111) 表面增强了脱氢和氢化反应，并为观察到的增强提供了理论依据。