Journal
ACS CATALYSIS
Volume 12, Issue 15, Pages 9270-9280Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02155
Keywords
syngas to hydrocarbons; cu/BEA zeolite; biomass syngas; high-octane gasoline; sustainable aviation fuel; CO2 conversion
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Funding
- U.S. DOE Office of Energy [DE-AC36-08GO28308]
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The research reported the cascade chemistry of converting syngas to branched hydrocarbons using Cu/BEA zeolite as catalyst in a single reactor, achieving a yield of 12.2% with evidence of CO2 incorporation into hydrocarbon products.
The synthesis of branched hydrocarbons for high-octane gasoline and sustainable aviation fuel directly from CO2-rich syngas in a single reactor holds potential to decrease capital and operating costs and increase overall energy and carbon efficiencies in a biorefinery. Here, we report the cascade chemistry of syngas to hydrocarbons under mild reaction conditions in a single reactor with C4+ single-pass yields of 13.7-44.9%, depending on the relative catalyst composition employing our dimethyl ether homologation catalyst, Cu/BEA zeolite. With co-fed CO2 at a concentration representative of biomass-derived syngas, 2.5:1:0.9 for H-2:CO:CO2, a hydrocarbon yield of 12.2% was observed with similar selectivity to C4+ products compared to the CO2-free feed. Definitive evidence of CO2 incorporation into the hydrocarbon products was demonstrated with isotopically labeled (CO2)-C-13 co-feed experiments, where mass spectrometry confirmed the propagation of C-13 into the C4+ hydrocarbons, highlighting the feasibility to co-convert CO and CO2 in this single reactor approach.
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