Peng Qiupeng, Hwang Meemie U, Rentería-Gómez Ángel, Mukherjee Poulami, Young Ryan M, Qiu Yunfan, Wasielewski Michael R, Gutierrez Osvaldo, Scheidt Karl A
Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
Department of Chemistry, Texas A&M University, College Station, TX 77843, USA.
Science. 2024 Sep 27;385(6716):1471-1477. doi: 10.1126/science.adr0771. Epub 2024 Sep 26.
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.
羰基化合物通过光激发产生自由基中间体的过程,在历史上一直局限于酮类和醛类;由于能量需求高且量子效率低,羧酸一直被忽视。一种成功的活化策略需要在吸收光谱上发生红移,增加三线态双自由基寿命,并便于进一步官能化。我们展示了一种单瓶法,可将羧酸转化为酰基膦酸酯,该方法能在可见光或近紫外光照射下生成具有合成用途的三线态双自由基。磷的使用避免了无生产性的I型Norrish反应,提高了选择性,从而实现氢原子转移反应性。使用该策略可通过各种环化、缩合和扩环反应途径,促进羧酸的高效骨架重塑。