Copper Cocatalyst Modulated Radical Generation for Selective Heterogeneous Photosynthesis of α-Haloketones.

Autor: Han F; Soochow Institute for Energy and Materials Innovations (SIEMIS), Soochow University, Suzhou, Jiangsu 215006, China.; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China., Zhang D; Soochow Institute for Energy and Materials Innovations (SIEMIS), Soochow University, Suzhou, Jiangsu 215006, China.; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China., Salli S; School of Chemistry, Cardiff University, Park Place, Cardiff CF10 3AT, U.K., Ye J; Soochow Institute for Energy and Materials Innovations (SIEMIS), Soochow University, Suzhou, Jiangsu 215006, China., Li Y; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China.; State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, CAS, Taiyuan 030001, China., Rosei F; Center for Energy, Materials and Telecommunications, Institut National de la Recherche Scientifique, 1650 Boulevard Lionel-Boulet, Varennes, Québec J3X 1P7, Canada., Wen XD; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China.; State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, CAS, Taiyuan 030001, China., Niemantsverdriet H; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China.; SynCat@DIFFER, Syngaschem BV, HH Eindhoven 6336, The Netherlands., Richards E; School of Chemistry, Cardiff University, Park Place, Cardiff CF10 3AT, U.K., Su R; Soochow Institute for Energy and Materials Innovations (SIEMIS), Soochow University, Suzhou, Jiangsu 215006, China.; SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Huairou, Beijing 101407, China.
Jazyk: angličtina
Zdroj: ACS catalysis [ACS Catal] 2023 Jan 06; Vol. 13 (1), pp. 248-255. Date of Electronic Publication: 2022 Dec 15.
DOI: 10.1021/acscatal.2c05189
Abstrakt: The α-haloketones are important precursors for synthetic chemistry and pharmaceutical applications; however, their production relies heavily on traditional synthetic methods via halogenation of ketones that are toxic and environmentally risky. Here, we report a heterogeneous photosynthetic strategy of α-haloketone production from aromatic olefins using copper-modified graphitic carbon nitride (Cu-C 3 N 4 ) under mild reaction conditions. By employing NiX 2 (X = Cl, Br) as the halogen source, a series of α-haloketones can be synthesized using atmospheric air as the oxidant under visible-light irradiation. In comparison with pristine carbon nitride, the addition of Cu as a cocatalyst provides a moderate generation rate of halogen radicals and selective reduction of molecular oxygen into • OOH radicals, thus leading to a high selectivity to α-haloketones. The Cu-C 3 N 4 also exhibits high stability and versatility, rendering it a promising candidate for solar-driven synthetic applications.
Competing Interests: The authors declare no competing financial interest.
(© 2022 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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