4.7 Article

Structure-Property Relationships of Pt-Sn Nanoparticles Supported on Al2O3 for the Dehydrogenation of Methylcyclohexane

期刊

ACS APPLIED NANO MATERIALS
卷 4, 期 5, 页码 4532-4541

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c00128

关键词

Pt-Sn catalyst; dehydrogenation; methylcyclohexane; nanoparticle; alloy; local structure

资金

  1. JSPS KAKENHI [18H01787]
  2. Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan [19J15440]
  3. Elements Strategy Initiative for Catalysts & Batteries (ESICB) - MEXT [JPMXP0112101003]
  4. Tanaka Precious Metals Memorial Foundation

向作者/读者索取更多资源

The activity and durability of Pt-Sn/Al2O3 catalysts in the MCH dehydrogenation were found to decrease with an increase in the Sn/Pt ratio. Pt-Sn/Al2O3 catalyst with a Sn/Pt ratio of 2 exhibited the best performance. The dispersion of Pt decreased and structural changes from Pt-Sn clusters to intermetallic nanoparticles were observed with increasing Sn/Pt ratio.
The structure-catalytic property relationships of Al2O3-supported Pt-Sn nanoparticles (Pt-Sn/Al2O3) in the dehydrogenation of methylcyclohexane (MCH) were investigated by varying the Sn/Pt ratios of the catalysts. The initial activity and the deactivation rate of the Pt-Sn/Al2O3 catalysts in the MCH dehydrogenation decreased in line with an increase in the Sn/Pt ratio from 0 to 3. The Pt-Sn/Al2O3 catalyst with a Sn/Pt ratio of 2 showed good activity, durability, and toluene selectivity in the MCH dehydrogenation among the series of catalysts. The dispersion of Pt in the Pt-Sn/Al2O3 catalysts was observed to decrease with an increase in the Sn/Pt ratio. Structural changes in the catalysts from Pt-Sn clusters to intermetallic Pt3Sn and PtSn nanoparticles were also observed using scanning transmission electron microscopy and X-ray diffraction. According to structural analysis using X-ray absorption fine-structure spectroscopy and infrared spectroscopy using carbon monoxide as a probe, the electron density of Pt increased, and the fraction of Pt-Pt adjacent sites decreased with an increase in the Sn/Pt ratio. Comparing the catalytic properties and the structures of the Pt-Sn/Al2O3 catalysts, their initial activities were correlated with the dispersion of Pt. In addition, the durability and selectivity of the catalysts were enhanced due to an increase in the electron density of Pt and a decrease in the number of Pt-Pt adjacent sites. Overall, the properties of the catalysts in the MCH dehydrogenation are determined by the local structure of Pt atoms rather than the crystal structure of the Pt-Sn alloy nanoparticles on Al2O3.

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