Single-atom Ru catalyst for selective synthesis of 3-pentanone via ethylene hydroformylation
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作者
GAS SHIFT REACTION; DIETHYL KETONE; ETHENE HYDROFORMYLATION; CARBON-MONOXIDE; RH; CO; HYDROCARBONYLATION; KETONIZATION; ALCOHOLS; OLEFINS
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刊物名称
Green Chem.
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年、卷、文献号
2021, 23,
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关键词
GAS SHIFT REACTION; DIETHYL KETONE; ETHENE HYDROFORMYLATION; CARBON-MONOXIDE; RH; CO; HYDROCARBONYLATION; KETONIZATION; ALCOHOLS; OLEFINS
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摘要
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 delta+) 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 C2H5CO* with C2H5* 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 C2H5CO* and H*. This strategy may provide a potential green route for the one-pot synthesis of 3-pentanone with high atomic economy.
