Abstract |
Selective C-O bond cleavage is an efficient way for the biomass valorization to value-added chemicals, but is challenged to be operated at room temperature via conventional thermal catalysis. Herein, inspired from the DNA biosynthesis which involves a radical-mediated spin-center shift (SCS) C-O bond cleavage process, we report a biomimetic room-temperature C-O bond cleavage of vicinal diol (HOCHCH- OH). We construct a Mn doped CdS (Mn/CdS) as a photocatalyst to mimic the biologic SCS process. The Mn site plays pivotal role: (1) accelerates the photo-induced carrier separation, promoting the hole-mediated C-H bond cleavage to generate carbon-centered radicals, and (2) serves as the binding site for - OH groups, making it to be an easier leaving group. Mn/CdS achieves 0.28 mmol gcat -1 h-1 of hydroxyacetone (HA) from glycerol dehydration at room temperature under visible light irradiation, which is 3.5-fold that over pristine CdS and 40-fold that over bulk MnS/CdS. This study provides a new biomimetic room-temperature C-O bond cleavage process, which is promising for the biomass valorization.
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Authors | Wenjing Zou, Hongru Zhou, Min Wang |
Journal | ChemSusChem
(ChemSusChem)
Vol. 16
Issue 20
Pg. e202300727
(Oct 20 2023)
ISSN: 1864-564X [Electronic] Germany |
PMID | 37486587
(Publication Type: Journal Article)
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Copyright | © 2023 Wiley-VCH GmbH. |