Xie Fukai, Mao Zhan, Curran Dennis P, Liang Hongliang, Dai Wen
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Department of Chemistry, University of Pittsburgh, Pittsburgh, PA, 15208, USA.
Angew Chem Int Ed Engl. 2023 Sep 25;62(39):e202306846. doi: 10.1002/anie.202306846. Epub 2023 Aug 18.
Although the development of radical chain and photocatalytic borylation reactions using N-heterocyclic carbene (NHC)-borane as boron source is remarkable, the persistent problems, including the use of hazardous and high-energy radical initiators or the recyclability and photostability issues of soluble homogeneous photocatalysts, still leave great room for further development in a sustainable manner. Herein, we report a conceptually different approach toward highly functionalized organoborane synthesis by using recoverable ultrathin cadmium sulfide (CdS) nanosheets as a heterogeneous photocatalyst, and a general and mild borylation platform that enables regioselective borylation of a wide variety of alkenes (arylethenes, trifluoromethylalkenes, α,β-unsaturated carbonyl compounds and nitriles), alkynes, imines and electron-poor aromatic rings with NHC-borane as boryl radical precursor. Mechanistic studies and density functional theory (DFT) calculations reveal that both photogenerated electrons and holes on the CdS fully perform their own roles, thereby resulting in enhancement of photocatalytic activity and stability of CdS.
尽管使用N-杂环卡宾(NHC)-硼烷作为硼源的自由基链式和光催化硼化反应取得了显著进展,但一些持续性问题,包括使用危险且高能的自由基引发剂,或可溶性均相光催化剂的可回收性和光稳定性问题,仍为以可持续方式进一步发展留下了很大空间。在此,我们报道了一种概念上不同的方法,通过使用可回收的超薄硫化镉(CdS)纳米片作为非均相光催化剂来合成高度官能化的有机硼烷,以及一个通用且温和的硼化平台,该平台能够以NHC-硼烷作为硼基自由基前体,对多种烯烃(芳基乙烯、三氟甲基烯烃、α,β-不饱和羰基化合物和腈)、炔烃、亚胺和缺电子芳香环进行区域选择性硼化。机理研究和密度泛函理论(DFT)计算表明,CdS上的光生电子和空穴都充分发挥了各自的作用,从而提高了CdS的光催化活性和稳定性。