Chromatic Fulleropyrrolidine as Long-Lived Metal-Free Catalyst for CO2 Photoreduction Reaction

Abstract

Conversion of CO₂ into carbonaceous fuels with the aid of solar energy has been an important research subject for decades. Owing to their excellent electron-accepting capacities, fullerene derivatives have been extensively used as n-type semiconductors. This work reports that the fulleropyrrolidine functionalized with 4,7-di(thiophen-2-yl)benzo[c][1,2,5]thiadiazole, abbreviated as DTBT-C₆₀ , could efficiently catalyze the photoreduction of CO₂ to CO. The novel C₆₀ -chromophore dyad structure facilitated better usage of solar light and effective dissociation of excitons. Consequently, the DTBT-C₆₀ exhibited a promising CO yield of 144 μmol g_cat ^-1 under AM1.5G solar illumination for 24 h. Moreover, the isotope experiments demonstrated that water molecules could function as an electron source to reactivate DTBT-C₆₀ . Impressively, DTBT-C₆₀ exhibited an extremely durable catalytic activity for more than one week, facilitating the practical application of photochemical CO₂ reaction.

Keywords: CO2 reduction; fullerenes; organocatalysis; photocatalysis; photosynthesis.