Efficient and Direct Functionalization of Allylic sp3 C-H Bonds with Concomitant CO2 Reduction

Angew Chem Int Ed Engl. 2023 Aug 25:e202311731. doi: 10.1002/anie.202311731. Online ahead of print.ABSTRACTSolar-driven CO2 reduction integrated with C-C/C-X bond-forming organic synthesis represents a substantially untapped opportunity to simultaneously tackle carbon neutrality and create an atom-/redox-economical chemical synthesis. Herein, we demonstrate the first cooperative photoredox catalysis of efficient and tunable CO2 reduction to syngas, paired with direct alkylation/arylation of unactivated allylic sp3 C-H bonds for accessing allylic C-C products, over SiO2-supported single Ni atoms-decorated CdS quantum dots (QDs). Our protocol not only bypasses additional oxidant/reductant and pre-functionalization of organic substrates, affording a broad of allylic C-C products with moderate to excellent yields, but also produces syngas with tunable CO/H2 ratios (1:2-5:1). Such win-win coupling catalysis highlights the high atom-, step- and redox-economy, and good durability, illuminating the tantalizing possibility of a renewable sunlight-driven chemical feedstocks manufacturing industry.PMID:37632151 | DOI:10.1002/anie.202311731
Source: Angewandte Chemie - Category: Chemistry Authors: Source Type: research
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