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Catalytic Tandem Reaction for the Production of Jet and Diesel Fuel Range Alkanes

Journal 2017 · IF 2.789 · 6(6): 1060-1066 · 发表于 2017 年 10 月 25 日
作者: Hu Li,Zhenyou Gui,Song Yang,Zhiwen Qi,Shunmugavel Saravanamurugan,Anders Riisager
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摘要

Jet and diesel fuels are typically composed of C 9 -C 14 and C 12 -C 20 hydrocarbons, respectively, but the carbon-chain length of sugar-derived aldehydes and furanic compounds is no longer than C 6 . Here, a cascade catalytic process involving alkylation and hydrodeoxygenation (HDO) of 2-methylfuran (2-MF) with different aldehydes is conducted to directly produce long-chain alkanes with exclusive carbon number of C 11 -C 17 in overall yields of 50–84 %. Preliminary investigations on the alkylation of 2-MF and formalin show that the relative density of Lewis and Brønsted acidic sites of zeolitic materials remarkably affect their catalytic activity and selectivity. Sn-beta(12.5) with pronounced Lewis acidity (including the acid density and strength) exhibits higher catalytic performance in the alkylation than other zeolites, producing long-chain oxygenates in 58–92 % yields. Even in aqueous solution, the Sn-beta(12.5) catalyst can be reused for at least six reaction cycles with almost constant reactivity. More importantly, the co-addition of Hf(OTf) 4 with Pd/C greatly promotes C−O bond cleavage of the furan-ring during the HDO process under mild reaction conditions, producing long-chain alkanes in high yields of 84–94 %.

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