Repository logo

Self-Assembled Liposomes Enhance Electron Transfer for Efficient Photocatalytic CO2 Reduction.

Accepted version



Change log


Light-driven conversion of CO2 to chemicals provides a sustainable alternative to fossil fuels, but homogeneous systems are typically limited by cross reactivity between different redox half reactions and inefficient charge separation. Herein, we present the bioinspired development of amphiphilic photosensitizer and catalyst pairs that self-assemble in lipid membranes to overcome some of these limitations and enable photocatalytic CO2 reduction in liposomes using precious metal-free catalysts. Using sodium ascorbate as a sacrificial electron source, a membrane-anchored alkylated cobalt porphyrin demonstrates higher catalytic CO production (1456 vs 312 turnovers) and selectivity (77 vs 11%) compared to its water-soluble nonalkylated counterpart. Time-resolved and steady-state spectroscopy revealed that self-assembly facilitates this performance enhancement by enabling a charge-separation state lifetime increase of up to two orders of magnitude in the dye while allowing for a ninefold faster electron transfer to the catalyst. Spectroelectrochemistry and density functional theory calculations of the alkylated Co porphyrin catalyst support a four-electron-charging mechanism that activates the catalyst prior to catalysis, together with key catalytic intermediates. Our molecular liposome system therefore benefits from membrane immobilization and provides a versatile and efficient platform for photocatalysis.



Carbon Dioxide, Catalysis, Electrons, Liposomes, Porphyrins

Journal Title

J Am Chem Soc

Conference Name

Journal ISSN


Volume Title


American Chemical Society (ACS)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (828838)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (891338)
Engineering and Physical Sciences Research Council (EP/R020965/1)
European Commission Horizon 2020 (H2020) ERC (883703)
Engineering and Physical Sciences Research Council (EP/P030467/1)
Is supplemented by: