<p>Propane dehydrogenation (PDH) processes typically operate at low weight-hourly space velocities of about 10 h<sup>−1</sup> to ensure catalyst stability, limiting propylene productivity to around 0.1 mol<sub>C3H6</sub> g<sub>catalyst</sub><sup>−1</sup> h<sup>−1</sup>. Here we report that controlling the formation of subnanometre PtSn alloyed clusters encapsulated in silicalite-1 affords a catalyst that can sustain high propylene productivities. At 165 h<sup>−1</sup>, the catalyst achieved about 1 mol<sub>C3H6</sub> g<sub>catalyst</sub><sup>−1</sup> h<sup>−1</sup> for more than 300 hours, with &gt;99% propylene selectivity. Furthermore, the spent catalyst can be effectively regenerated using simple air calcination. Detailed characterization and computational modelling attribute the high PDH performance to the distinctive electronic structures of the Pt sites within subnanometre alloyed clusters. The dynamic structures of these subnanometre alloyed clusters probably allow these Pt sites to access a broader range of electronic and structural configurations, expanding the reaction’s accessible energy landscape and effectively breaking the longstanding trade-off between productivity and stability that constrains conventional PDH catalysts.</p><p></p>

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Subnanometre PtSn alloyed clusters encapsulated in silicalite-1 sustain high productivity in propane dehydrogenation

  • Shangchen Lu,
  • Yaxin Tang,
  • Bingqing Yao,
  • Yishui Ding,
  • Huanhuan Yang,
  • Shibo Xi,
  • Kang Hui Lim,
  • Chaokai Xu,
  • Yankun Du,
  • Xingjie Fu,
  • Shengdong Tan,
  • Binbin Zhao,
  • Wenhao Yuan,
  • C. Austin Wade,
  • Dali Yang,
  • Lu Ma,
  • Sheng Dai,
  • Sibudjing Kawi,
  • Ning Yan,
  • Jiong Lu,
  • Wei Chen,
  • Guangfu Luo,
  • Qian He

摘要

Propane dehydrogenation (PDH) processes typically operate at low weight-hourly space velocities of about 10 h−1 to ensure catalyst stability, limiting propylene productivity to around 0.1 molC3H6 gcatalyst−1 h−1. Here we report that controlling the formation of subnanometre PtSn alloyed clusters encapsulated in silicalite-1 affords a catalyst that can sustain high propylene productivities. At 165 h−1, the catalyst achieved about 1 molC3H6 gcatalyst−1 h−1 for more than 300 hours, with >99% propylene selectivity. Furthermore, the spent catalyst can be effectively regenerated using simple air calcination. Detailed characterization and computational modelling attribute the high PDH performance to the distinctive electronic structures of the Pt sites within subnanometre alloyed clusters. The dynamic structures of these subnanometre alloyed clusters probably allow these Pt sites to access a broader range of electronic and structural configurations, expanding the reaction’s accessible energy landscape and effectively breaking the longstanding trade-off between productivity and stability that constrains conventional PDH catalysts.