Direct 2,3-Butanediol Conversion to Butene-Rich C3+ Olefins over Copper-Modified 2D Pillared MFI: Consequence of Reduced Diffusion Length

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 bifu...

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Published inACS sustainable chemistry & engineering Vol. 10; no. 4; pp. 1664 - 1674
Main Authors Adhikari, Shiba, Zhang, Junyan, Unocic, Kinga, Wegener, Evan C, Kunal, Pranaw, Deka, Dhruba J, Toops, Todd, Sinha Majumdar, Sreshtha, Krause, Theodore R, Liu, Dongxia, Li, Zhenglong
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 31.01.2022
American Chemical Society (ACS)
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Summary: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.
Bibliography:AC05-00OR22725; AC02-06CH11357
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office
ISSN:2168-0485
2168-0485
DOI:10.1021/acssuschemeng.1c07670