Plasmonic photosynthesis of C1–C3 hydrocarbons from carbon dioxide assisted by an ionic liquid

Sungju Yu and Prashant K. Jain ()
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Sungju Yu: University of Illinois at Urbana-Champaign
Prashant K. Jain: University of Illinois at Urbana-Champaign

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Photochemical conversion of CO2 into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light-driven synthesis of C1–C3 hydrocarbons from CO2 and H2O. In this approach, plasmonic excitation of Au nanoparticles produces a charge-rich environment at the nanoparticle/solution interface conducive for CO2 activation, while an ionic liquid stabilizes charged intermediates formed at this interface, facilitating multi-step reduction and C–C coupling. Methane, ethylene, acetylene, propane, and propene are photosynthesized with a C2+ selectivity of ~50% under the most optimal conditions. Hydrocarbon turnover exhibits a volcano relationship as a function of the ionic liquid concentration, the kinetic analysis of which coupled with density functional theory simulations provides mechanistic insights into the synergy between plasmonic excitation and the ionic liquid.

Date: 2019
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DOI: 10.1038/s41467-019-10084-5

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