Salzmann Kevin, Segarra Candela, Albrecht Martin
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, 3012, Bern, Switzerland.
Angew Chem Int Ed Engl. 2020 Jun 2;59(23):8932-8936. doi: 10.1002/anie.202002014. Epub 2020 Mar 25.
An exceptionally efficient ruthenium-based catalyst for olefin oxidation has been designed by exploiting N,N'-bis(pyridylidene)oxalamide (bisPYA) as a donor-flexible ligand. The dynamic donor ability of the bisPYA ligand, imparted by variable zwitterionic and neutral resonance structure contributions, paired with the redox activity of ruthenium provided catalytic activity for Lemieux-Johnson-type oxidative cleavage of olefins to efficiently prepare ketones and aldehydes. The ruthenium bisPYA complex significantly outperforms state-of-the-art systems and displays extraordinary catalytic activity in this oxidation, reaching turnover frequencies of 650 000 h and turnover numbers of several millions.
通过利用N,N'-双（吡啶叉）草酰胺（bisPYA）作为供体灵活的配体，设计出了一种用于烯烃氧化的高效钌基催化剂。bisPYA配体的动态供体能力由可变的两性离子和中性共振结构贡献赋予，与钌的氧化还原活性相结合，为烯烃的Lemieux-Johnson型氧化裂解提供了催化活性，从而有效地制备酮和醛。钌bisPYA配合物明显优于现有技术体系，并且在这种氧化反应中表现出非凡的催化活性，周转频率达到650000 h，周转数达到数百万。
