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<p>Single-atom catalysts (SACs) provide isolated, well-defined metal sites that are suited for mechanistic modeling in porous materials such as metal-organic frameworks (MOFs). However, the influence of framework topology and mass transport on catalytic outcomes remains poorly understood. Here we develop a multiscale kinetic model for ethylene oligomerization in Ni-grafted NU-1000 that combines density functional theory (DFT)-derived free-energy barriers with adsorption and diffusion descriptors. The framework predicts product distributions under realistic reaction conditions. The simulations show that <i>flow</i>-mode operation favors selective C<sub>4</sub>H<sub>8</sub> formation across a temperature range. This selectivity window progressively narrows with increasing effective diffusion length and catalytic-site density, as longer residence times enhance chain growth beyond dimerization. In contrast, <i>batch</i>-mode operation shifts the product distribution toward heavier olefins. These trends provide practical guidance for tuning operating conditions and material properties to achieve desired selective Ni-MOF catalysts.</p>

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Multiscale kinetic model of ethylene oligomerization in Ni-NU-1000 metal-organic framework

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月24日

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  • Aleksandr Avdoshin,
  • Nikita A. Matsokin,
  • Thanh-Nam Huynh,
  • Dmitry I. Sharapa,
  • Karin Fink,
  • Felix Studt,
  • Wolfgang Wenzel,
  • Mariana Kozlowska

摘要

Single-atom catalysts (SACs) provide isolated, well-defined metal sites that are suited for mechanistic modeling in porous materials such as metal-organic frameworks (MOFs). However, the influence of framework topology and mass transport on catalytic outcomes remains poorly understood. Here we develop a multiscale kinetic model for ethylene oligomerization in Ni-grafted NU-1000 that combines density functional theory (DFT)-derived free-energy barriers with adsorption and diffusion descriptors. The framework predicts product distributions under realistic reaction conditions. The simulations show that flow-mode operation favors selective C4H8 formation across a temperature range. This selectivity window progressively narrows with increasing effective diffusion length and catalytic-site density, as longer residence times enhance chain growth beyond dimerization. In contrast, batch-mode operation shifts the product distribution toward heavier olefins. These trends provide practical guidance for tuning operating conditions and material properties to achieve desired selective Ni-MOF catalysts.