Department of Chemistry and Centre for Sustainable Chemistry, Ghent University, Krijgslaan 281 (S3), 9000, Ghent, Belgium.
Separation and Conversion Technology, VITO (Flemish Institute for Technological Research), Boeretang 200, 2400, Mol, Belgium.
Chemistry. 2023 Jul 14;29(40):e202301259. doi: 10.1002/chem.202301259. Epub 2023 May 30.
Herein, we report the catalytic activity of a series of platinum(II) pre-catalysts, bearing N-heterocyclic carbene (NHC) ligands, in the alkene hydrosilylation reaction. Their structural and electronic properties are fully investigated using X-ray diffraction analysis and nuclear magnetic resonance spectroscopy (NMR). Next, our study presents a structure-activity relationship within this group of pre-catalysts and gives mechanistic insights into the catalyst activation step. An exceptional catalytic performance of one of the complexes is observed, reaching a turnover number (TON) of 970 000 and a turnover frequency (TOF) of 40 417 h at 1 ppm catalyst loading. Finally, an attractive solvent-free and open-to-air alkene hydrosilylation protocol, featuring efficient platinum removal (reduction of residual Pt from 582 ppm to 5.8 ppm), is disclosed.
在此,我们报告了一系列负载氮杂环卡宾(NHC)配体的铂(II)预催化剂在烯烃硅氢化反应中的催化活性。我们使用 X 射线衍射分析和核磁共振波谱(NMR)对其结构和电子性质进行了全面研究。接下来,我们在这组预催化剂中研究了结构-活性关系,并深入了解了催化剂活化步骤的机理。我们观察到其中一种配合物具有出色的催化性能,在催化剂负载量为 1ppm 时,其周转数(TON)达到 970000,转化频率(TOF)达到 40417h。最后,我们还披露了一种具有吸引力的无溶剂、开放空气的烯烃硅氢化方法,该方法能够有效去除铂(将残留的 Pt 从 582ppm 降低至 5.8ppm)。