Scholarlink

<p>Syngas-to-ethanol conversion is economically attractive yet remains challenging due to limited activity and selectivity under practical conditions. Achieving selective C-C coupling and directing *CHO hydrogenation to ethanol require precise control of active-site geometry and electronics. Here we use a coordination–precursor–mediated strategy to construct Ru dual-atom catalysts on N-coordinated carbon supports with tunable local architectures, where the Ru-Ru separation serves as a primary descriptor—together with coordination environment and intersite electronic coupling—governing cooperative CO/H<sub>2</sub> activation and C-C bond formation. Varying the interatomic distance modulates geometric confinement and electronic interactions, improving ethanol formation. Within the optimal reaction window, the catalyst with the shortest Ru-Ru distance exhibits high CO conversion, high ethanol selectivity among oxygenated products, with oxygen-free hydrocarbon products excluded from the selectivity normalization, and stable operation at 1.0 MPa. In situ spectroscopy and DFT reveal that short Ru-Ru spacing enhances d-orbital hybridization and confinement, facilitating synergistic back-donation that lowers the C-C coupling barrier; Bader/charge-density analyses indicate preferential stabilization of hydroxylated intermediates toward ethanol. This work highlights distance-tuned dual-atom cooperativity as a key lever for selective syngas-to-ethanol catalysis.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Spatial and mechanistic elucidation of distance tunable Ru dual atom catalysts for efficient CO hydrogenation to ethanol

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年8月4日

查看全文
  • Haobo Zhao,
  • Yi Wang,
  • Yanling Gao,
  • Jingyu Ran,
  • Zhongqing Yang,
  • Hao Zhang,
  • Qiang Chen,
  • Nianbing Li,
  • Haojie Geng

摘要

Syngas-to-ethanol conversion is economically attractive yet remains challenging due to limited activity and selectivity under practical conditions. Achieving selective C-C coupling and directing *CHO hydrogenation to ethanol require precise control of active-site geometry and electronics. Here we use a coordination–precursor–mediated strategy to construct Ru dual-atom catalysts on N-coordinated carbon supports with tunable local architectures, where the Ru-Ru separation serves as a primary descriptor—together with coordination environment and intersite electronic coupling—governing cooperative CO/H2 activation and C-C bond formation. Varying the interatomic distance modulates geometric confinement and electronic interactions, improving ethanol formation. Within the optimal reaction window, the catalyst with the shortest Ru-Ru distance exhibits high CO conversion, high ethanol selectivity among oxygenated products, with oxygen-free hydrocarbon products excluded from the selectivity normalization, and stable operation at 1.0 MPa. In situ spectroscopy and DFT reveal that short Ru-Ru spacing enhances d-orbital hybridization and confinement, facilitating synergistic back-donation that lowers the C-C coupling barrier; Bader/charge-density analyses indicate preferential stabilization of hydroxylated intermediates toward ethanol. This work highlights distance-tuned dual-atom cooperativity as a key lever for selective syngas-to-ethanol catalysis.