The excitation of carbonyl compounds by light to generate radical intermediates has historically been restricted to ketones and aldehydes; carboxylic acids have been overlooked because of high energy requirements and low quantum efficiency. A successful activation strategy would necessitate a bathochromic shift in the absorbance profile, an increase in triplet diradical lifetime, and ease of further functionalization. We present a single-flask transformation of carboxylic acids to acyl phosphonates that can access synthetically useful triplet diradicals under visible light or near-ultraviolet irradiation. The use of phosphorus circumvents unproductive Norrish type I processes, promoting selectivity that enables hydrogen-atom transfer reactivity. Use of this strategy promotes the efficient scaffold remodeling of carboxylic acids through various annulation, contraction, and expansion manifolds.

Download full-text PDF

Source
http://dx.doi.org/10.1126/science.adr0771DOI Listing

Publication Analysis

Top Keywords

carboxylic acids
16
scaffold remodeling
8
remodeling carboxylic
8
photochemical phosphorus-enabled
4
phosphorus-enabled scaffold
4
carboxylic
4
acids
4
acids excitation
4
excitation carbonyl
4
carbonyl compounds
4

Similar Publications

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!