Highly Dispersed and Active ReOx on Alumina-Modified SBA-15 Silica for 2-Butanol Dehydration
SBA-15 silica supported rhenium catalysts were synthesized using solution-based atomic layer deposition method, and their activity and stability were studied in the acid-catalyzed 2-butanol dehydration. We find that ReOx/SBA-15 exhibited an extremely high initial activity but a fast deactivation for 2-butanol dehydration at 90-105 C. Fast deactivation was likely due to the sintering, sublimation, and reduction of rhenia as confirmed by TEM, elemental analysis, and in situ UV vis (DRS) measurements. To overcome these issues, ReOx/AlOx/SBA-15 catalysts with significantly improved stability were prepared by first modifying the surface identity of SBA-15 with alumina followed by dispersion of rhenia using atomic layer deposition. The AlOx phase stabilizes the dispersion of small and uniform rhenia clusters (<2 nm) as as confirmed by TEM, STEM and UV-vis (DRS) characterizations. Additional 27Al MAS NMR characterization revealed that modification of the SBA-15 surface with alumina introduces a strong interaction between rhenia and alumina, which consequently improves the stability of supported rhenia catalysts by suppressing the sintering, sublimation, and reduction of rhenia albeit at a moderately reduced initial catalytic dehydration activity
- Research Organization:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1042536
- Report Number(s):
- PNNL-SA-84678; 35599; KC0302010
- Journal Information:
- ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 6 Vol. 2
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
27Al MAS NMR
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
CATALYSTS
DEACTIVATION
DEHYDRATION
DEPOSITION
Environmental Molecular Sciences Laboratory
MODIFICATIONS
RHENIUM
SBA-15
SILICA
SINTERING
STABILITY
STRONG INTERACTIONS
SUBLIMATION
aberration-corrected TEM
catalyst stability
in-situ UV-vis (DRS)
rhenia catalyst