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<p>The conversion of CO<sub>2</sub> into high-value syngas (CO and H<sub>2</sub>) using Cu-based catalysts has garnered considerable interest. However, these catalysts deactivate rapidly due to Ostwald-ripening and thermal aggregation. Herein, we propose to encapsulate Cu-cluster into mMOR zeolite for engineering a separation-site catalyst Cu@mMOR. In the reverse water-gas shift reaction (RWGS), mMOR zeolite of Cu@mMOR directly captures and then activates CO<sub>2</sub>, and simultaneously serves as a molecular fence to prevent CO<sub>2</sub> contact with Cu-clusters surrounding with small pore of mMOR (&lt;3.0 Å) channels. These encapsulated Cu-clusters in mMOR possess considerable Cu vacancies, which significantly facilitate H<sub>2</sub> heterolytic dissociation, transferring H<sup>*</sup> species towards activated CO<sub>2</sub> on mMOR and converting them into CO. This separation-site strategy efficiently increases catalytic activation while intelligently altering the CO<sub>2</sub> reaction pathway, preventing Cu from thermal agglomeration and Oswald ripening in the catalyst. Consequently, Cu@mMOR attains a space-time yield of CO as high as 3290 mmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, with catalytic stability extending up to 788 hours.</p>

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Molecular fence Cu-based catalyst for CO2 hydrogenation to CO with high activity and durability

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月6日

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  • Weige Su,
  • Xuehui Jia,
  • Xintan Deng,
  • Xu Fan,
  • Syed Jalil Shah,
  • Changhao Li,
  • Jiajun Zeng,
  • Yilin Lou,
  • Jianhua Chen,
  • Zhongxing Zhao,
  • Zhenxia Zhao

摘要

The conversion of CO2 into high-value syngas (CO and H2) using Cu-based catalysts has garnered considerable interest. However, these catalysts deactivate rapidly due to Ostwald-ripening and thermal aggregation. Herein, we propose to encapsulate Cu-cluster into mMOR zeolite for engineering a separation-site catalyst Cu@mMOR. In the reverse water-gas shift reaction (RWGS), mMOR zeolite of Cu@mMOR directly captures and then activates CO2, and simultaneously serves as a molecular fence to prevent CO2 contact with Cu-clusters surrounding with small pore of mMOR (<3.0 Å) channels. These encapsulated Cu-clusters in mMOR possess considerable Cu vacancies, which significantly facilitate H2 heterolytic dissociation, transferring H* species towards activated CO2 on mMOR and converting them into CO. This separation-site strategy efficiently increases catalytic activation while intelligently altering the CO2 reaction pathway, preventing Cu from thermal agglomeration and Oswald ripening in the catalyst. Consequently, Cu@mMOR attains a space-time yield of CO as high as 3290 mmol gcat-1 h-1, with catalytic stability extending up to 788 hours.