Single-atom Ru catalyst for selective synthesis of 3-pentanone ethylene hydroformylation

• Published in: Green chemistry : an international journal and green chemistry resource : GC 2021-11, Vol.23 (22), p.938-947
• Main Authors: Qin, Tingting, Dang, Yaru, Lin, Tiejun, Mei, Bingbao, Wu, Bo, Li, Xiao, Li, Shenggang, Jiang, Zheng, Tang, Zhiyong, Zhong, Liangshu, Sun, Yuhan
• Format: Article
• ISSN: 1463-9262; 1463-9270
• DOI: 10.1039/d1gc02464g

A Ru single-atom (Ru SA) catalyst supported on activated carbon was adopted to synthesize 3-pentanone with 83.3% selectivity via heterogeneous ethylene hydroformylation, while 52.1% ethane selectivity was obtained for Ru nanoparticles (Ru NPs). The atomically dispersed Ru species with oxidation state (Ru δ + ) and Ru-C4O coordination structure were identified as the active sites for efficient C-C coupling to generate 3-pentanone, while metallic Ru nanoparticles exhibited high activity for ethylene hydrogenation to ethane. Density functional theory (DFT) calculation revealed that the energy barrier of the direct coupling of C 2 H 5 CO* with C 2 H 5 * to form 3-pentanone on Ru SA was much lower than that on Ru NPs. As a result, the formation of 3-pentanone over Ru SA was more favourable than propanal, which was admittedly generated via coupling of C 2 H 5 CO* and H*. This strategy may provide a potential green route for the one-pot synthesis of 3-pentanone with high atomic economy. A Ru single-atom (Ru SA) catalyst supported on activated carbon was adopted to synthesize 3-pentanone with 83.3% selectivity via heterogeneous ethylene hydroformylation, while 52.1% ethane selectivity was obtained for Ru nanoparticles (Ru NPs).