Catalytic Hydrodeoxygenation of High Carbon Furylmethanes to Renewable Jet-fuel Ranged Alkanes over a Rhenium-Modified Iridium Catalyst

被引:74
作者
Liu, Sibao [1 ]
Dutta, Saikat [1 ]
Zheng, Weiqing [1 ]
Gould, Nicholas S. [1 ]
Cheng, Ziwei [1 ]
Xu, Bingjun [1 ]
Saha, Basudeb [1 ]
Vlachos, Dionisios G. [1 ]
机构
[1] Univ Delaware, Dept Chem & Biomol Engn, Catalysis Ctr Energy Innovat, Newark, DE 19716 USA
关键词
HIGH-QUALITY DIESEL; C-O BOND; PLATFORM MOLECULES; CYCLIC ETHERS; SUGAR POLYOLS; BIOMASS; HYDROGENOLYSIS; CONVERSION; 2-METHYLFURAN; HEMICELLULOSE;
D O I
10.1002/cssc.201700863
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Renewable jet-fuel-range alkanes are synthesized by hydro-deoxygenation of lignocellulose-derived high-carbon furylmethanes over ReOx-modified Ir/SiO2 catalysts under mild reaction conditions. Ir-ReOx/SiO2 with a Re/Ir molar ratio of 2:1 exhibits the best performance, achieving a combined alkanes yield of 82-99% from C-12-C-15 furylmethanes. The catalyst can be regenerated in three consecutive cycles with only about 12% loss in the combined alkanes yield. Mechanistically, the furan moieties of furylmethanes undergo simultaneous ring saturation and ring opening to form a mixture of complex oxygenates consisting of saturated furan rings, mono-keto groups, and mono-hydroxy groups. Then, these oxygenates undergo a cascade of hydrogenolysis reactions to alkanes. The high activity of Ir-ReOx/SiO2 arises from a synergy between Ir and ReOx, whereby the acidic sites of partially reduced ReOx activate the C-O bonds of the saturated furans and alcoholic groups while the Ir sites are responsible for hydrogenation with H-2.
引用
收藏
页码:3225 / 3234
页数:10
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