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<p>Oxidative dehydrogenation of propane (ODHP) is a promising route for propylene production, but achieving high selectivity towards propylene while minimizing CO<sub>x</sub> byproducts remains a significant challenge for conventional metal oxide catalysts. Here we propose a solution to this challenge by employing atomically dispersed dual-atom catalysts (M<sub>1</sub>M'<sub>1</sub>-TiO<sub>2</sub> DACs). Ni<sub>1</sub>Fe<sub>1</sub>-TiO<sub>2</sub> DACs exhibit an ultralow CO<sub>x</sub> selectivity of 5.2% at a high propane conversion of 46.1% and 520 °C, with stable performance for over 1000 hours. Mechanistic investigations reveal that these catalysts operate via a cooperative Langmuir-Hinshelwood mechanism, distinct from the Mars-van Krevelen mechanism typical of metal oxides. This cooperative pathway facilitates efficient conversion of propane and oxygen into propylene at the dual-atom interface. The superior selectivity arises from facile olefin desorption from the dual-atom sites and suppressed formation of electrophilic oxygen species, which are preferentially adsorbed on Fe<sub>1</sub> sites rather than oxygen vacancies. This work highlights the potential of dual-atom catalysts for highly selective ODHP and provides insights into their unique catalytic mechanism.</p>

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Suppressing COx in oxidative dehydrogenation of propane with dual-atom catalysts

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月19日

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  • Yongbin Yao,
  • Jingnan Wang,
  • Fei Lu,
  • Wenlin Li,
  • Bingbao Mei,
  • Lifeng Zhang,
  • Wensheng Yan,
  • Fangli Yuan,
  • Guiyuan Jiang,
  • Sanjaya D. Senanayake,
  • Xi Wang

摘要

Oxidative dehydrogenation of propane (ODHP) is a promising route for propylene production, but achieving high selectivity towards propylene while minimizing COx byproducts remains a significant challenge for conventional metal oxide catalysts. Here we propose a solution to this challenge by employing atomically dispersed dual-atom catalysts (M1M'1-TiO2 DACs). Ni1Fe1-TiO2 DACs exhibit an ultralow COx selectivity of 5.2% at a high propane conversion of 46.1% and 520 °C, with stable performance for over 1000 hours. Mechanistic investigations reveal that these catalysts operate via a cooperative Langmuir-Hinshelwood mechanism, distinct from the Mars-van Krevelen mechanism typical of metal oxides. This cooperative pathway facilitates efficient conversion of propane and oxygen into propylene at the dual-atom interface. The superior selectivity arises from facile olefin desorption from the dual-atom sites and suppressed formation of electrophilic oxygen species, which are preferentially adsorbed on Fe1 sites rather than oxygen vacancies. This work highlights the potential of dual-atom catalysts for highly selective ODHP and provides insights into their unique catalytic mechanism.