Decarboxylation of stearic acid over Ni/MOR catalysts
Decarboxylation of stearic acid over Ni/MOR catalysts
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DOI：
10.1002/jctb.6211
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发表时间：
2019-10
影响因子：
3.4
通讯作者：
James M. Crawford;S. Zaccarine;Nolan C. Kovach;Courtney S. Smoljan;Jolie M. Lucero;B. Trewyn;S. Pylypenko;Moises A. Carreon
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文献类型：
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作者：
James M. Crawford;S. Zaccarine;Nolan C. Kovach;Courtney S. Smoljan;Jolie M. Lucero;B. Trewyn;S. Pylypenko;Moises A. Carreon
背景：来自植物、动物脂肪和藻类的油含有饱和和不饱和脂肪酸。这些脂肪酸可以在活性固体催化剂的存在下转化为液体燃料和化学品。研究结果：通过离子交换合成将镍基催化剂负载在丝光沸石上，并评价其用于硬脂酸脱氧成柴油燃料。通过调节合成pH，获得超过20wt%的Ni负载。在pH 8.5合成的催化剂显示出最高的Ni负载量和最高的活性的脱羧/脱羰硬脂酸在惰性氮气气氛下，产生47%的十七烷。表征包括扫描透射电子显微镜-能量色散光谱（STEM-EDS）、X射线衍射（XRD）、场发射扫描电子显微镜（FE-SEM）、电感耦合等离子体原子发射光谱（ICP-AES）、氮氧化物物理吸附和热重分析（TGA），为催化剂的可回收性提供了新的见解。回收时观察到的催化活性损失归因于Ni纳米颗粒的团聚和碳质焦炭的积累。结论：本工作表明丝光沸石负载的镍基催化剂可以有效地将硬脂酸转化为十七烷。十七烷的产率高达47%。从机理上讲，反应通过脱羧和脱羰基途径进行。© 2019化学工业协会
BACKGROUND: Oils derived from plants, animal fats, and algae contain both saturated and unsaturated fatty acids. These fatty acids can be converted into liquid fuels and chemicals in the presence of active solid catalysts. RESULTS: Nickel‐based catalysts were supported on mordenite via ion exchange synthesis and evaluated for the deoxygenation of stearic acid to diesel fuels. By tuning the synthesis pH, loadings of over 20 wt% Ni were obtained. Catalysts synthesized at pH 8.5 displayed the highest Ni loading and the highest activity for the decarboxylation/decarbonylation of stearic acid under inert nitrogen gas atmospheres, yielding 47% heptadecane. Characterization included scanning transmission electron microscopy‐energy‐dispersive spectroscopy (STEM‐EDS), X‐ray diffraction (XRD), field emission scanning electron microscopy (FE‐SEM), inductively coupled plasma atomic emission spectroscopy (ICP‐AES), N₂ physisorption and thermogravimetric analysis (TGA), providing new insights into the recyclability of the catalyst. The observed loss of catalytic activity upon recycling was attributed to the agglomeration of Ni nanoparticles and the accumulation of carbonaceous coke. CONCLUSION: This work demonstrates that Ni‐based catalysts supported on mordenite zeolite can effectively convert stearic acid into heptadecane. Yields to heptadecane were as high as 47%. Mechanistically, the reaction proceeds by decarboxylation and decarbonylation pathways. © 2019 Society of Chemical Industry