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<p>Ethylene, one of the major basic chemicals in the modern chemical industry, has been industrially produced mainly through intensive energy-consuming steam cracking processes from light oil fractions or shale gas operated above 800 °C following the radical mechanism and seriously suffering from high methane selectivity. Herein, we report an efficient catalytic cracking reaction of 1-pentene over a tailored ZSM-5 catalyst at 700 °C with a C<sub>2</sub>H<sub>4</sub>/C<sub>3</sub>H<sub>6</sub> ratio of 1.31 and a CH<sub>4</sub> selectivity below 5%, which provides an energy-saving and economically viable route for ethylene production from light oil fractions, seamlessly integrating with the existing industrial catalytic cracking processes. Mechanistic studies unveil an interesting type of zeolite catalysis different from the typical acid catalysis following the carbenium ion mechanism, termed as the confined catalytic radical (CCR) mechanism in which 1-pentene dehydrogenates to gaseous pentenyl radicals (C<sub>5</sub>H<sub>9</sub>•) at non-acidic [AlO<sub>4</sub>]<sup>0</sup> sites of ZSM-5 in situ formed by dehydrogenation of bridging hydroxyls, whose subsequent reactions confined in ZSM-5 produce more C<sub>2</sub>H<sub>4</sub> than C<sub>3</sub>H<sub>6</sub>. These findings significantly broaden the concept and application of zeolite catalysis.</p>

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In-situ formation of [AlO4]0 site for confined catalytic cracking to ethylene with low methane selectivity

  • 期刊论文

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  • 发表日期：

    2025年12月11日

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  • Wenjie Yang,
  • Yunxing Bai,
  • Mo Zheng,
  • Ruilin Wang,
  • Zhenxuan Yuan,
  • Xingtian Shu,
  • Yanfen Zuo,
  • Xiang Li,
  • Chengyuan Liu,
  • Yang Pan,
  • Bona Lu,
  • Weixin Huang,
  • Mingyuan He,
  • Youhao Xu

摘要

Ethylene, one of the major basic chemicals in the modern chemical industry, has been industrially produced mainly through intensive energy-consuming steam cracking processes from light oil fractions or shale gas operated above 800 °C following the radical mechanism and seriously suffering from high methane selectivity. Herein, we report an efficient catalytic cracking reaction of 1-pentene over a tailored ZSM-5 catalyst at 700 °C with a C2H4/C3H6 ratio of 1.31 and a CH4 selectivity below 5%, which provides an energy-saving and economically viable route for ethylene production from light oil fractions, seamlessly integrating with the existing industrial catalytic cracking processes. Mechanistic studies unveil an interesting type of zeolite catalysis different from the typical acid catalysis following the carbenium ion mechanism, termed as the confined catalytic radical (CCR) mechanism in which 1-pentene dehydrogenates to gaseous pentenyl radicals (C5H9•) at non-acidic [AlO4]0 sites of ZSM-5 in situ formed by dehydrogenation of bridging hydroxyls, whose subsequent reactions confined in ZSM-5 produce more C2H4 than C3H6. These findings significantly broaden the concept and application of zeolite catalysis.