Direct 2,3-Butanediol Conversion to Butene-Rich C3+ Olefins over Copper-Modified 2D Pillared MFI: Consequence of Reduced Diffusion Length
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Maryland, College Park, MD (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Maryland, College Park, MD (United States)
2,3-Butanediol (2,3-BDO), a critical C4 platform chemical derived from biomass, syngas, or CO2, can be converted to C3+ olefins, serving as important renewable feedstocks for producing sustainable aviation fuels to decarbonize the hard-to-electrify air transportation sector. Herein, we report a bifunctional Cu-modified diffusion-free 2D pillared MFI catalyst (Cu/PMFI) which can selectively catalyze 2,3-BDO conversion to butene-rich C3+ olefins (95% selectivity at 97% conversion, 523 K). 2,3-BDO conversion to butenes over Cu/PMFI primarily occurs via methyl ethyl ketone intermediate while 2-methyl propanal is also observed as another minor dehydration product that leads to butene formation. In comparison with a control mesoporous Cu/ZSM-5 sample prepared by the postsynthetic approach, Cu/PMFI shows favorable C3+ olefin selectivity (95% over Cu/PMFI vs 80% over Cu/ZSM-5 at ~5.1 h TOS). The coke formation over Cu/PMFI is dramatically suppressed by >50% in contrast to Cu/ZSM-5 in 90 h 2,3-BDO conversion due to the reduced diffusion length. Cu/PMFI also favors butene formation and minimizes nonbutene C3+ olefins by inhibiting the downstream oligomerization and cracking reactions. This study highlights the usefulness of the diffusion-free 2D PMFI materials in catalytic conversion of biomass-derived platform molecules and the significance of diffusion impact on catalyst coke formation and product distributions.
- Research Organization:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office
- Grant/Contract Number:
- AC02-06CH11357; AC05-00OR22725
- OSTI ID:
- 1844869
- Journal Information:
- ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 4 Vol. 10; ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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