期刊
ROYAL SOCIETY OPEN SCIENCE
卷 8, 期 10, 页码 -出版社
ROYAL SOC
DOI: 10.1098/rsos.211086
关键词
zeolites; hierarchical materials; catalysis; selective oxidation
资金
- UCL [PR16195]
- UK Catalysis Hub [SP15151]
Hierarchical zeolites have the potential to overcome transport limitations and improve active site dispersion and generation, leading to enhanced alcohol conversion rates. Balancing support porosity, acidity, and active site dispersion is crucial for optimal aldehyde production.
Hierarchical zeolites have the potential to provide a breakthrough in transport limitation, which hinders pristine microporous zeolites and thus may broaden their range of applications. We have explored the use of Pd-doped hierarchical ZSM-5 zeolites for aerobic selective oxidation (selox) of cinnamyl alcohol and benzyl alcohol to their corresponding aldehydes. Hierarchical ZSM-5 with differing acidity (H-form and Na-form) were employed and compared with two microporous ZSM-5 equivalents. Characterization of the four catalysts by X-ray diffraction, nitrogen porosimetry, NH3 temperature-programmed desorption, CO chemisorption, high-resolution scanning transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy allowed investigation of their porosity, acidity, as well as Pd active sites. The incorporation of complementary mesoporosity, within the hierarchical zeolites, enhances both active site dispersion and PdO active site generation. Likewise, alcohol conversion was also improved with the presence of secondary mesoporosity, while strong Bronsted acidity, present solely within the H-form systems, negatively impacted overall selectivity through undesirable self-etherification. Therefore, tuning support porosity and acidity alongside active site dispersion is paramount for optimal aldehyde production.
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