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Catalytic Decomposition of Long-Chain Olefins to Propylene via Isomerization-Metathesis Using Latent Bicyclic (Alkyl)(Amino)Carbene-Ruthenium Olefin Metathesis Catalysts
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DOI：10.1002/anie.202204413.png)
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Abstract
En 中文
One of the most exciting scientific challenges today is the catalytic degradation of non-biodegradable polymers into value-added chemical feedstocks. The mild pyrolysis of polyolefins, including high-density polyethylene (HDPE), results in pyrolysis oils containing long-chain olefins as major products. In this paper, novel bicyclic (alkyl)(amino)carbene ruthenium (BICAAC-Ru) temperature-activated latent olefin metathesis catalysts, which can be used for catalytic decomposition of long-chain olefins to propylene are reported. These thermally stable catalysts show significantly higher selectivity to propylene at a reaction temperature of 75 degrees C compared to second generation Hoveyda-Grubbs or CAAC-Ru catalysts under ethenolysis conditions. The conversion of long-chain olefins (e.g., 1-octadecene or methyl oleate) to propylene via isomerization-metathesis is performed by using a (RuHCl)(CO)(PPh3)(3) isomerization co-catalyst. The reactions can be carried out at a BICAAC-Ru catalyst loading as low as 1 ppm at elevated reaction temperature (75 degrees C). The observed turnover number and turnover frequency are as high as 55 000 and 10 000 mol(propylene) mol(catalyst)(-1) h(-1), respectively.
Keywords:
BICAAC
Hydrocarbon Decomposition
ISOMET
Metathesis
Propylene
Ruthenium
Journal
IF:
16.9
Papers:
5.6W
Citations:
53.0W
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