Kittikhunnatham Preecha, Leith Gabrielle A, Mathur Abhijai, Naglic Jennifer K, Martin Corey R, Park Kyoung Chul, McCullough Katherine, Jayaweera H D A Chathumal, Corkill Ryan E, Lauterbach Jochen, Karakalos Stavros G, Smith Mark D, Garashchuk Sophya, Chen Donna A, Shustova Natalia B
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208, USA.
Angew Chem Int Ed Engl. 2022 Mar 14;61(12):e202113909. doi: 10.1002/anie.202113909. Epub 2022 Jan 27.
The efficient delivery of reactive and toxic gaseous reagents to organic reactions was studied using metal-organic frameworks (MOFs). The simultaneous cargo vehicle and catalytic capabilities of several MOFs were probed for the first time using the examples of aromatization, aminocarbonylation, and carbonylative Suzuki-Miyaura coupling reactions. These reactions highlight that MOFs can serve a dual role as a gas cargo vehicle and a catalyst, leading to product formation with yields similar to reactions employing pure gases. Furthermore, the MOFs can be recycled without sacrificing product yield, while simultaneously maintaining crystallinity. The reported findings were supported crystallographically and spectroscopically (e.g., diffuse reflectance infrared Fourier transform spectroscopy), foreshadowing a pathway for the development of multifunctional MOF-based reagent-catalyst cargo vessels for reactive gas reagents as an attractive alternative to the use of toxic pure gases or gas generators.
利用金属有机框架（MOF）研究了将活性和有毒气态试剂有效输送至有机反应中的情况。首次以芳构化、氨基羰基化和羰基化铃木-宫浦偶联反应为例，探究了几种MOF同时作为载运工具和催化剂的能力。这些反应表明，MOF可同时充当气体载运工具和催化剂，生成的产物产率与使用纯气体的反应相似。此外，MOF可循环使用而不牺牲产物产率，同时保持结晶度。晶体学和光谱学（如漫反射红外傅里叶变换光谱）研究结果支持了所报道的发现，这预示着开发基于多功能MOF的活性气体试剂载运工具的途径，是使用有毒纯气体或气体发生器的一种有吸引力的替代方案。
