4.7 Article

Catalytic performances in methane combustion over Pd nanoparticles supported on pure silica zeolites with different structures

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ELSEVIER
DOI: 10.1016/j.micromeso.2022.112298

关键词

Methane; Catalytic combustion; Pure silica zeolites; Pd nanoparticles

资金

  1. National Natural Science Foundation of China [21802123]
  2. Hangzhou Qianjiang Distinguished Experts Project

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The study found that different siliceous zeolite supports have a significant influence on the catalytic performance of Pd nanoparticles in methane oxidation, with siliceous MFI (ZSM-5-Si) showing the highest activity. The difference in methane adsorption is identified as the critical factor for the discrepancy in catalytic performances.
Catalytic combustion of CH4 to CO2 and H2O was studied over Pd nanoparticles supported on different siliceous zeolites (MFI, BEA and CHA) with gamma-Al2O3 as the reference support, and it was found that as supports, zeolites exert remarkable influence on the catalytic performance of methane oxidation, with the Pd catalyst (1 wt% loading) supported by siliceous MFI (ZSM-5-Si) presenting the highest activity. Over the exceptional catalyst, a complete conversion of methane can be achieved at around 380 degrees C, which is about 120 degrees C lower than the temperature needed for the Pd nanoparticles supported on gamma-Al2O3 (Pd/gamma-Al2O3), one of the best catalysts for the methane combustion. Physicochemical characterizations including X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), temperature programmed desorption of methane (CH4-TPD) and temperature programmed reduction of methane (CH4-TPR) techniques were used to acquire an idea what is behind the discrepancy in the catalytic performances of methane combustion over these Pd-based catalysts. Based on these results, it is proposed that the different methane adsorption and the oxygen migration capability are mainly related to the difference in the catalytic performances of methane combustion over these catalysts. Among these factors, the difference in the methane adsorption is critical for the different catalytic performances, as evidenced by the kinetic measurements.

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