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<p>The integration of CO<sub>2</sub> into the dehydrogenation of propane (PDH) holds significant promise for both propylene production and greenhouse gas utilization. However, a pivotal challenge lies in mitigating the undesirable dry reforming of propane (DRP), which diminishes propylene selectivity compared to direct PDH processes. Herein, we describe a coupled process that integrates PDH with reverse water gas shift (RWGS) using a tandem catalytic system. The PtSn/Al<sub>2</sub>O<sub>3</sub> analogue performs the dehydrogenation reaction, while an adjacent defective CeO<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> at nanoscale acts as the hydrogenation sites for CO<sub>2</sub>. Catalysis and kinetic studies demonstrate the in-situ removal of hydrogen from PtSn/Al<sub>2</sub>O<sub>3</sub> to adjacent CeO<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub>, facilitated by CO<sub>2</sub>, shifts the quasi-equilibrium of PDH towards propylene production, while suppressing the competitive DRP side reaction. This hydrogen spillover-mediated coupling mechanism enables superior propylene selectivity of ~98.8%, along with high CO<sub>2</sub> (~43.9%) and propane conversion (~44.2%) at 550 °C, outperforming direct PDH (~40.6%). Analysis of CO<sub>2</sub> footprint indicates the PDH-RWGS tandem process has the potential for carbon utilization to mitigate detrimental CO<sub>2</sub> emissions.</p>

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Unraveling the hydrogen spillover in tandem propane dehydrogenation and reverse water gas shift reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月19日

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  • Kaige Tian,
  • Sai Chen,
  • Guodong Sun,
  • Jiachen Sun,
  • Xianhui Wang,
  • Jianhua Cai,
  • Zhiyuan Wang,
  • Donglong Fu,
  • Zhi-Jian Zhao,
  • Chunlei Pei,
  • Jinlong Gong

摘要

The integration of CO2 into the dehydrogenation of propane (PDH) holds significant promise for both propylene production and greenhouse gas utilization. However, a pivotal challenge lies in mitigating the undesirable dry reforming of propane (DRP), which diminishes propylene selectivity compared to direct PDH processes. Herein, we describe a coupled process that integrates PDH with reverse water gas shift (RWGS) using a tandem catalytic system. The PtSn/Al2O3 analogue performs the dehydrogenation reaction, while an adjacent defective CeOx/Al2O3 at nanoscale acts as the hydrogenation sites for CO2. Catalysis and kinetic studies demonstrate the in-situ removal of hydrogen from PtSn/Al2O3 to adjacent CeOx/Al2O3, facilitated by CO2, shifts the quasi-equilibrium of PDH towards propylene production, while suppressing the competitive DRP side reaction. This hydrogen spillover-mediated coupling mechanism enables superior propylene selectivity of ~98.8%, along with high CO2 (~43.9%) and propane conversion (~44.2%) at 550 °C, outperforming direct PDH (~40.6%). Analysis of CO2 footprint indicates the PDH-RWGS tandem process has the potential for carbon utilization to mitigate detrimental CO2 emissions.