Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 304, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120946
Keywords
Selectively reductive coupling; Carbon-carbon bond formation; Ketone activation; Visible-light catalysis; Proton-coupled electron transfer
Funding
- National Natural Science Foundation of China [22072082, 21402113, 22003036]
- National Natural Science Foundation of Shaanxi Province [2019JQ-175]
- Fundamental Research Funds for the Central Universities [GK202103026, GK202103033, GK202009068, GK201903041]
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This study demonstrates a mechanism for photocatalytic reductive coupling under visible light using low-cost catalysts, providing a new approach for solar-driven chemical synthesis. By investigating processes such as proton-coupled electron transfer in detail, the key radical formation stage is elucidated.
Photocatalytic reductive coupling of carbon-carbon bond to assemble complex molecular frameworks holds the great promising for solar energy storage and value-added chemicals production. This process generally demands noble-photosensitizer or powered by ultraviolet light, along with harsh conditions, which inevitably induces undesired by-product with poor selectivity. Here, we demonstrated selectively reductive aromatic ketones into pinacol on low-cost photocatalysts Ni-doped quantum dots, in which the yield can reach up to 88% with ketones conversion more than 95% under visible-light irradiation for 5 h. A novel mechanism dedicated to the interaction between in situ generated oxidized sacrificial agents TEA(.+) and reactants for key ketyl radical formation via proton-coupled electron transfer (PCET) is elaborately probed by EPR measurement, iotope labeling experiments and DFT calculation. This work emerges a new family of catalysts for C-C coupling by solar energy. More importantly, it provides more credible demonstration for TEA activated photocatalytic conversion in organic synthesis.
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