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 gcat−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.

H-Atom Abstraction Reactivity through the Lens of Asynchronicity and Frustration with Their Counteracting Effects on Barriers

“…In the upcoming section, we will test the applicability of the presented Marcus-type model to the blooming field of organocatalytic HAA, − distinct from transition metal-mediated chemistry and where a transferable and predictive method would be paramount for reaction design.…”

H-atom Abstraction Reactivity through the Lens of Asynchronicity and Frustration with their Counter-Acting Effects on Barriers

“…In contrast to canonical equation ( 12), all trained methods were parametrized using metal-oxo oxidants and their transferability to a purely organic chemical space would be paramount as the field of organocatalysis continues to bloom. 36,37,38 The predictions from the four models on the organic test set are condensed in Figure 7. Borovik's model, adapted to the prediction of relative HAA barriers, displays two parameters, (α,…”

Synthesis of 3,3’‐(Ethane‐1,2‐diylidene)bis(indolin‐2‐one) Promoted by Thermally‐activated Electron Transfer and Photoreduction of CO2 to CH4 and CO

“…Organic molecular catalysts are rather limited. A study is established by Wang, Jeng, and co‐workers [14] . A fulleropyrrolidine synthesized from C 60 yielded a R CO of 6 μmol g cat −1 h −1 .…”

“…A study is established by Wang, Jeng, and co-workers. [14] A fulleropyrrolidine synthesized from C 60 yielded a R CO of 6 μmol g cat À 1 h À 1 . Donors with the electron-pushing features and acceptors with the electronpulling characteristics construct organic donor-acceptor (DÀ A) molecules.…”