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 Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1042536
- Report Number(s):
- PNNL-SA-84678; 35599; KC0302010; TRN: US1202790
- Journal Information:
- ACS Catalysis, Vol. 2, Issue 6
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
CATALYSTS
DEACTIVATION
DEHYDRATION
DEPOSITION
MODIFICATIONS
RHENIUM
SILICA
SINTERING
STABILITY
STRONG INTERACTIONS
SUBLIMATION
rhenia catalyst
catalyst stability
2-butanol dehydration
SBA-15
in-situ UV-vis (DRS)
aberration-corrected TEM
27Al MAS NMR
Environmental Molecular Sciences Laboratory