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<p>Metal single-atom catalysts offer improved activity and selectivity due to their unique electronic and coordination properties compared with bulk metals. However, many single-atom catalysts suffer from randomly dispersed active sites and limited electron-donating ability due to bonding with electronegative elements or less reactive metals. Here we demonstrate that Mg-rich intermetallic Mg<sub>29</sub>TM<sub>4</sub> (TM = Pd, Rh, Ir, Pt) nanocatalysts overcome these limitations. These materials feature periodically dispersed, electron-rich single-atom sites of noble metals within a uniform chemical environment. Mg<sub>29</sub>TM<sub>4</sub> exhibits high activity and selectivity in C<sub>2</sub>H<sub>2</sub> semihydrogenation (Mg<sub>29</sub>Pd<sub>4</sub>) and olefin hydroformylation (Mg<sub>29</sub>Rh<sub>4</sub>), with Mg<sub>29</sub>Rh<sub>4</sub> achieving high regioselectivity for branched aldehydes (branched:linear &gt; 200:1). Kinetic and density functional theory studies suggest that the Mg–TM ensemble enables precise control over carbon–carbon multiple bond adsorption and activation, enhancing both activity and selectivity. Furthermore, the ternary Mg<sub>29</sub>Pd<sub>1.3</sub>Rh<sub>2.7</sub> catalyst, with its synergistic Mg–Pd and Mg–Rh dual single-atom sites, efficiently catalyses a cascade reaction involving phenylacetylene hydrogenation followed by hydroformylation.</p><p></p>

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Ordered single active sites for cascade hydrogenation and hydroformylation reactions

  • 期刊论文

  • 发表日期：

    2025年5月26日

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  • Xiaojun Lu,
  • Jiazhen Wu,
  • Xinyi He,
  • Zichuang Li,
  • Yangfan Lu,
  • Wenqian Li,
  • Jiang Li,
  • Miao Xu,
  • Yanpeng Qi,
  • Qing Zhang,
  • Yijia Liu,
  • Meng Du,
  • Toshio Kamiya,
  • Hideo Hosono,
  • Fusheng Pan,
  • Jie-Sheng Chen,
  • Tian-Nan Ye

摘要

Metal single-atom catalysts offer improved activity and selectivity due to their unique electronic and coordination properties compared with bulk metals. However, many single-atom catalysts suffer from randomly dispersed active sites and limited electron-donating ability due to bonding with electronegative elements or less reactive metals. Here we demonstrate that Mg-rich intermetallic Mg29TM4 (TM = Pd, Rh, Ir, Pt) nanocatalysts overcome these limitations. These materials feature periodically dispersed, electron-rich single-atom sites of noble metals within a uniform chemical environment. Mg29TM4 exhibits high activity and selectivity in C2H2 semihydrogenation (Mg29Pd4) and olefin hydroformylation (Mg29Rh4), with Mg29Rh4 achieving high regioselectivity for branched aldehydes (branched:linear > 200:1). Kinetic and density functional theory studies suggest that the Mg–TM ensemble enables precise control over carbon–carbon multiple bond adsorption and activation, enhancing both activity and selectivity. Furthermore, the ternary Mg29Pd1.3Rh2.7 catalyst, with its synergistic Mg–Pd and Mg–Rh dual single-atom sites, efficiently catalyses a cascade reaction involving phenylacetylene hydrogenation followed by hydroformylation.