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Stable Ga-MFI zeolite for propane dehydroaromatization constructed by healing Silanol-defect in framework
Meile Yue1, Kankan Bu1, Yahong1
1Department of Chemistry, Shanghai Key Laboratory of Electrochemical and Thermochemical Conversion for Resources Recycling, College of Smart Materials and Future Energy, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Fudan University, Shanghai 200433, PR China.
Researchers developed a new gallosilicate MFI zeolite (Ga-MFI-AHFS) to improve propane dehydroaromatization (PDA). This defect-remediated catalyst shows enhanced stability and resistance to coking, enabling longer catalyst life for producing valuable aromatics.
Area of Science:
- Catalysis
- Materials Science
- Chemical Engineering
Background:
- Propane dehydroaromatization (PDA) offers a non-petroleum route to valuable aromatics like benzene, toluene, and xylene.
- Ga-modified MFI zeolites are active catalysts for PDA but suffer from deactivation due to coke deposition.
- Silanol defects in zeolites significantly contribute to catalyst instability and coking.
Purpose of the Study:
- To develop a stable and highly active Ga-MFI zeolite catalyst for PDA.
- To address the challenge of coke deposition and prolong catalyst longevity.
- To investigate the effect of silanol defect remediation on catalyst performance.
Main Methods:
- Synthesis of gallosilicate MFI zeolite.
- Post-treatment using ammonium hexafluorosilicate to remediate silanol defects.
- Characterization using FTIR and MAS NMR.
- Evaluation of catalytic performance in CO2-assisted PDA reactions.
Main Results:
- The remediated catalyst (Ga-MFI-AHFS) maintained high propane conversion (82.0%) and aromatics selectivity (64.5%) over 20 hours.
- FTIR and MAS NMR confirmed a significant reduction in silanol nests and internal Si-OH groups.
- Ga-MFI-AHFS exhibited a six-fold lower coking rate compared to the raw Ga-MFI zeolite.
- The catalyst demonstrated excellent stability and resistance to deactivation.
Conclusions:
- Remediation of silanol defects via ammonium hexafluorosilicate post-treatment effectively enhances the stability and coking resistance of Ga-MFI zeolites.
- The developed Ga-MFI-AHFS catalyst provides a promising solution for stable and efficient dehydroaromatization of light alkanes.
- This facile post-treatment method offers a pathway to improve the longevity of MFI zeolite catalysts in hydrocarbon conversions.
