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Palladium-doped hierarchical ZSM-5 for catalytic selective oxidation of allylic and benzylic alcohols

DOI: 10.1098/rsos.211086 DOI Help

Authors: Shengzhe Ding (University of Manchester) , Muhammad Ganesh (University of Manchester) , Yilai Jiao (Institute of Metal Research, Chinese Academy of Sciences) , Xiaoxia Ou (University of Manchester) , Mark Isaacs (University College London; HarwellXPS, Research Complex at Harwell) , Mark S'Ari (University of Leeds) , Antonio Torres Lopez (University of Manchester; Catalysis Hub, Research Complex at Harwell) , Xiaolei Fan (University of Manchester) , Christopher M. A. Parlett (University of Manchester; Catalysis Hub, Research Complex at Harwell; University of Manchester at Harwell; Diamond Light Source)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Royal Society Open Science , VOL 8

State: Published (Approved)
Published: October 2021
Diamond Proposal Number(s): 15151

Open Access Open Access

Abstract: 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 Brønsted 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.

Subject Areas: Chemistry, Materials


Instruments: B18-Core EXAFS

Added On: 25/10/2021 09:52

Documents:
rsos.211086.pdf

Discipline Tags:

Catalysis Chemical Engineering Physical Chemistry Zeolites Engineering & Technology Materials Science Nanoscience/Nanotechnology Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)