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Abstract <p>We present an innovative catalytic system employing secondary phosphine oxide (SPO)-stabilized palladium-gold nanoalloys (SPO-Au/Pd-NPs) for the sustainable synthesis of aromatic amines in aqueous media. This engineered catalyst demonstrates exceptional chemoselectivity (&gt;99% in most cases) and activity (TOF up to 4.759 h<sup><i>–</i>1</sup>) in the hydrogenation of diverse nitroarenes and <i>N</i>-heterocycles. Mechanistic studies reveal that the synergistic interplay between the bimetallic Pd/Au nanoalloy core and SPO ligands enables: (1) spatial confinement of reactants through alloy effect, (2) dual activation pathways for both molecular hydrogen and nitro groups, and (3) water-mediated proton transfer networks that suppress undesired side reactions. Notably, the aqueous environment facilitates a unique self-assembly process where hydration layers organize reactant molecules at the catalyst interface, achieving near-quantitative yields (&gt;99%) under mild conditions (25°C, 1 atm H<sub>2</sub>). The catalyst’s heterogeneous nature permits phase separation post-reaction, enabling efficient recovery with retained activity (&gt;95% over 6 cycles) through simple decantation. This protocol eliminates the need for organic solvents or energy-intensive procedures, establishing a new paradigm for green amine synthesis with atomic precision.</p>

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Palladium-Gold Alloy Nanocatalysts with Electron-Deficient Surfaces Ultrafast Nitroarene High Chemoselective Hydrogenation via Concerted Molecular Hydrogen Transfer in Water

  • 期刊论文

  • 发表日期：

    2025年11月1日

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  • Chang-Chun Liu,
  • Zhi-Hao Shen,
  • Yuan-Yuan Xu,
  • Guang-Qi Gao,
  • Hong-Jun Kong,
  • Ben-Cai Dai,
  • Jun-An Ma,
  • Yang Zhou

摘要

Abstract

We present an innovative catalytic system employing secondary phosphine oxide (SPO)-stabilized palladium-gold nanoalloys (SPO-Au/Pd-NPs) for the sustainable synthesis of aromatic amines in aqueous media. This engineered catalyst demonstrates exceptional chemoselectivity (>99% in most cases) and activity (TOF up to 4.759 h–1) in the hydrogenation of diverse nitroarenes and N-heterocycles. Mechanistic studies reveal that the synergistic interplay between the bimetallic Pd/Au nanoalloy core and SPO ligands enables: (1) spatial confinement of reactants through alloy effect, (2) dual activation pathways for both molecular hydrogen and nitro groups, and (3) water-mediated proton transfer networks that suppress undesired side reactions. Notably, the aqueous environment facilitates a unique self-assembly process where hydration layers organize reactant molecules at the catalyst interface, achieving near-quantitative yields (>99%) under mild conditions (25°C, 1 atm H2). The catalyst’s heterogeneous nature permits phase separation post-reaction, enabling efficient recovery with retained activity (>95% over 6 cycles) through simple decantation. This protocol eliminates the need for organic solvents or energy-intensive procedures, establishing a new paradigm for green amine synthesis with atomic precision.