Liu Mingxin, Tan Lida, Rashid Roksana T, Cen Yunen, Cheng Shaobo, Botton Gianluigi, Mi Zetian, Li Chao-Jun
Department of Chemistry and FRQNT Centre for Green Chemistry and Catalysis, McGill University 801 Sherbrooke Ouest Montreal Quebec H3A 0B8 Canada
Department of Electrical Engineering and Computer Science, University of Michigan 1301 Beal Ave Ann Arbor MI 48109 USA
Chem Sci. 2020 Jul 1;11(30):7864-7870. doi: 10.1039/d0sc02718a.
Employing photo-energy to drive the desired chemical transformation has been a long pursued subject. The development of homogeneous photoredox catalysts in radical coupling reactions has been truly phenomenal, however, with apparent disadvantages such as the difficulty in separating the catalyst and the frequent requirement of scarce noble metals. We therefore envisioned the use of a hyper-stable III-V photosensitizing semiconductor with a tunable Fermi level and energy band as a readily isolable and recyclable heterogeneous photoredox catalyst for radical coupling reactions. Using the carbonyl coupling reaction as a proof-of-concept, herein, we report a photo-pinacol coupling reaction catalyzed by GaN nanowires under ambient light at room temperature with methanol as a solvent and sacrificial reagent. By simply tuning the dopant, the GaN nanowire shows significantly enhanced electronic properties. The catalyst showed excellent stability, reusability and functional tolerance. All reactions could be accomplished with a single piece of nanowire on Si-wafer.
利用光能驱动所需的化学转化一直是人们长期追求的课题。然而,均相光氧化还原催化剂在自由基偶联反应中的发展确实引人注目,但也存在明显的缺点,如催化剂分离困难以及频繁需要稀缺的贵金属。因此,我们设想使用具有可调费米能级和能带的超稳定III-V族光敏半导体作为易于分离和循环使用的非均相光氧化还原催化剂用于自由基偶联反应。本文以羰基偶联反应作为概念验证,报道了在室温下以甲醇为溶剂和牺牲试剂,GaN纳米线在环境光下催化的光频哪醇偶联反应。通过简单地调节掺杂剂,GaN纳米线显示出显著增强的电子性能。该催化剂表现出优异的稳定性、可重复使用性和功能耐受性。所有反应都可以用硅片上的一根纳米线完成。