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<p>A two-stage tandem process combining CO<sub>2</sub> Fischer-Tropsch synthesis (CO<sub>2</sub>-FTS) with downstream zeolite upgrading provides a practical route for converting broad Anderson-Schulz-Flory (ASF)-type hydrocarbons into light olefins. In this study, hierarchical MFI zeolites with systematically tuned mesoporosity were synthesized using the amphiphilic organosilane [3-(trimethoxysilyl)propyl]hexadecyldimethylammonium chloride (TPHAC) and compared with commercial microporous ZSM-5 (Si/Al = 15). TPHAC preserved the MFI framework while increasing the external surface area and mesopore volume. The upstream K/Fe-Cu-Al catalyst produced a stable ASF-type hydrocarbon stream at 300&#xa0;°C and 2.5&#xa0;MPa. In the temperature-screening tandem reaction, TPHAC-4% showed the best performance, affording the highest C<sub>2</sub>-C<sub>4</sub> olefin selectivity of 52.34% on a hydrocarbon basis at 500&#xa0;°C while suppressing BTEX formation. Under the 150&#xa0;h long-term operation at the same temperature, it maintained an average C<sub>2</sub>-C<sub>4</sub> olefin selectivity of 56.77% over TOS 40–150&#xa0;h. A 1-octene model reaction reproduced the same trend, indicating that the hierarchical pore structure promoted light-olefin formation while suppressing competing aromatic pathways. Post-reaction coke analysis further showed reduced coke accumulation in the micropores. Overall, the hierarchical pore architecture created a more favorable environment for light-olefin production.</p>

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Hierarchical MFI-Type Zeolites for Light Olefin Production in CO2-Fischer-Tropsch Tandem Catalysis

  • 期刊论文

  • 发表日期：

    2026年5月15日

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  • Hae-Gu Park,
  • Taejeong Lee,
  • Susung Lee,
  • Minkee Choi,
  • Hyung-Ki Min,
  • Jeong-Rang Kim,
  • Min Bum Park,
  • Hyun Wook Hwang,
  • Seok Ki Kim

摘要

A two-stage tandem process combining CO2 Fischer-Tropsch synthesis (CO2-FTS) with downstream zeolite upgrading provides a practical route for converting broad Anderson-Schulz-Flory (ASF)-type hydrocarbons into light olefins. In this study, hierarchical MFI zeolites with systematically tuned mesoporosity were synthesized using the amphiphilic organosilane [3-(trimethoxysilyl)propyl]hexadecyldimethylammonium chloride (TPHAC) and compared with commercial microporous ZSM-5 (Si/Al = 15). TPHAC preserved the MFI framework while increasing the external surface area and mesopore volume. The upstream K/Fe-Cu-Al catalyst produced a stable ASF-type hydrocarbon stream at 300 °C and 2.5 MPa. In the temperature-screening tandem reaction, TPHAC-4% showed the best performance, affording the highest C2-C4 olefin selectivity of 52.34% on a hydrocarbon basis at 500 °C while suppressing BTEX formation. Under the 150 h long-term operation at the same temperature, it maintained an average C2-C4 olefin selectivity of 56.77% over TOS 40–150 h. A 1-octene model reaction reproduced the same trend, indicating that the hierarchical pore structure promoted light-olefin formation while suppressing competing aromatic pathways. Post-reaction coke analysis further showed reduced coke accumulation in the micropores. Overall, the hierarchical pore architecture created a more favorable environment for light-olefin production.