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<p>This study presents a Co catalyst with coexisting single-atoms and nanoparticles on N-doped carbon (Co<sub>1</sub>+Co<sub>n</sub>/N-C). Synthesized via a sacrificial MgO-template method, it achieves 100% vanillin conversion and &gt;99% selectivity to 2-methoxy-4-methylphenol at 160°C using formic acid, outperforming single-component catalysts. Kinetic studies reveal a water-mediated dual hydrogen transfer pathway, lowering the apparent activation energy to 61.7 kJ/mol. Isotopic studies suggest a water-mediated mechanism, wherein water molecules facilitate proton transfer and hydrogen spillover through a hydrogen-bonding network. This process synergizes with formic acid dehydrogenation to enable a dual hydrogen transfer pathway, involving protonation of the aldehyde group and hydride (H⁻) attack. The catalyst maintains 95% conversion over ten cycles, demonstrating high stability for biomass upgrading.</p>

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Cobalt single-atom and nano catalysts for efficient transfer hydrodeoxygenation of vanillin with formic acid

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月23日

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  • Jiayi Li,
  • Guangling Shi,
  • Zisheng Xu,
  • Lu Wang,
  • Maofei Ran,
  • Tao Dai

摘要

This study presents a Co catalyst with coexisting single-atoms and nanoparticles on N-doped carbon (Co1+Con/N-C). Synthesized via a sacrificial MgO-template method, it achieves 100% vanillin conversion and >99% selectivity to 2-methoxy-4-methylphenol at 160°C using formic acid, outperforming single-component catalysts. Kinetic studies reveal a water-mediated dual hydrogen transfer pathway, lowering the apparent activation energy to 61.7 kJ/mol. Isotopic studies suggest a water-mediated mechanism, wherein water molecules facilitate proton transfer and hydrogen spillover through a hydrogen-bonding network. This process synergizes with formic acid dehydrogenation to enable a dual hydrogen transfer pathway, involving protonation of the aldehyde group and hydride (H⁻) attack. The catalyst maintains 95% conversion over ten cycles, demonstrating high stability for biomass upgrading.