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<p>Supported-metal catalysts are well-established for industrial catalysis, but controlling the metal-oxide interaction (MSI) is challenging because of the intricate geometric and electronic effects. Herein, this paper describes the strategy of controlling metal-oxide interaction by pre-tailoring the oxygen vacancy (O<sub>v</sub>) concentrations on defective metal oxides for supported Pt catalysts. ZnO distinguishes itself among the metal oxides examined, with the structural and chemical attributes of O<sub>v</sub> playing a pivotal role in determining its effectiveness. At lower O<sub>v</sub> concentration (less than 0.82 mmol/g<sub>ZnO</sub>), the O<sub>v</sub> in defective ZnO<sub><i>x</i></sub> impedes Pt growth, while higher O<sub>v</sub> concentration (0.82 to 5.63 mmol/g<sub>ZnO</sub>) induces an electron-sufficient Pt state without compromising Pt dispersion. During propane dehydrogenation (PDH), performed under reducing conditions, the optimized Pt/ZnO<sub><i>x</i></sub> achieved 44% of propane conversion and 90% of propylene selectivity at 600 °C under 4 h<sup>−1</sup> of C<sub>3</sub>H<sub>8</sub>, which is comparable to that of PtSn/Al<sub>2</sub>O<sub>3</sub> analogue. This oxygen vacancy engineering strategy provides mechanistic insights into disentangling geometric and electronic factors, advancing the rational design of MSI-controlled PDH catalysts.</p>

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Decoupling size and electronic effects of Pt through oxygen vacancy engineering in propane dehydrogenation

  • 期刊论文

  • 发表日期：

    2025年6月27日

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  • Xianhui Wang,
  • Sai Chen,
  • Guodong Sun,
  • Xin Chang,
  • Kaige Tian,
  • Zhenyi Zhao,
  • Zelin Wu,
  • Donglong Fu,
  • Zhi-Jian Zhao,
  • Chunlei Pei,
  • Jinlong Gong

摘要

Supported-metal catalysts are well-established for industrial catalysis, but controlling the metal-oxide interaction (MSI) is challenging because of the intricate geometric and electronic effects. Herein, this paper describes the strategy of controlling metal-oxide interaction by pre-tailoring the oxygen vacancy (Ov) concentrations on defective metal oxides for supported Pt catalysts. ZnO distinguishes itself among the metal oxides examined, with the structural and chemical attributes of Ov playing a pivotal role in determining its effectiveness. At lower Ov concentration (less than 0.82 mmol/gZnO), the Ov in defective ZnOx impedes Pt growth, while higher Ov concentration (0.82 to 5.63 mmol/gZnO) induces an electron-sufficient Pt state without compromising Pt dispersion. During propane dehydrogenation (PDH), performed under reducing conditions, the optimized Pt/ZnOx achieved 44% of propane conversion and 90% of propylene selectivity at 600 °C under 4 h−1 of C3H8, which is comparable to that of PtSn/Al2O3 analogue. This oxygen vacancy engineering strategy provides mechanistic insights into disentangling geometric and electronic factors, advancing the rational design of MSI-controlled PDH catalysts.