Robust ruthenium catalysts for the selective conversion of stearic acid to diesel-range alkanes

被引:59
|
作者
Di, Lu [1 ,2 ]
Yao, Sikai [1 ,2 ]
Song, Song [1 ,2 ]
Wu, Guangjun [1 ,2 ]
Dai, Weili [1 ,2 ]
Guan, Naijia [1 ,2 ,3 ,4 ]
Li, Landong [1 ,2 ,3 ,4 ]
机构
[1] Nankai Univ, Sch Mat Sci & Engn, Tianjin 300071, Peoples R China
[2] Nankai Univ, Natl Inst Adv Mat, Tianjin 300071, Peoples R China
[3] Nankai Univ, Minist Educ, Key Lab Adv Energy Mat Chem, Tianjin 300071, Peoples R China
[4] Nankai Univ, Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300071, Peoples R China
基金
中国国家自然科学基金;
关键词
Ruthenium catalysts; Stearic acid; Catalytic deoxygenation; Biofuel; Reaction network; TOTAL-ENERGY CALCULATIONS; SUPPORTED RU CATALYSTS; BIODIESEL PRODUCTION; MICROALGAE OIL; FATTY-ACIDS; DEOXYGENATION; FUEL; ALCOHOLS; ETHANOL; BIOMASS;
D O I
10.1016/j.apcatb.2016.08.023
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Triglycerides represent a type of sustainable energy source and robust catalysts for triglycerides refining to biofuels are very challenging. Herein, we report supported ruthenium catalysts, optimized from group VIII metal catalysts, for the selective conversion of triglycerides to diesel-range alkanes under mild conditions. The catalyst supports and ruthenium loadings show significant impacts on the performance of ruthenium catalysts, and Ru/TiO2 with ruthenium weight loading of 1.68% is optimized for the reaction. Typically, the platform compound stearic acid could be directly converted, or via 1-octadecanol as an intermediate product, to n-heptadecane and n-octadecane in n-heptane solvent using the optimized Ru/TiO2 catalyst at 473 K and under 3 MPa H-2. On the basis of catalytic and spectroscopic characterization results, large ruthenium metal particles are established as the preferred active sites for stearic acid conversion. The complete reaction network of stearic acid deoxygenation on flat Ru (0001) is investigated by theoretical calculations. It is revealed that different pathways run simultaneously during the reaction and the adsorbed acyl species C17H35CO* are the key reaction intermediates for the catalytic deoxygenation on Ru (0001). The removal of adsorbed CO by hydrogenation is the rate-controlling step contributing to the highest energy barrier within the reaction network. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:137 / 149
页数:13
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