Catalytic performance and deactivation of sulfonated hydrothermal carbon in the esterification of fatty acids: Comparison with sulfonic solids of different nature

Catalytic performance and deactivation of sulfonated hydrothermal carbon in the esterification of fatty acids: Comparison with sulfonic solids of different nature
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DOI:
10.1016/j.jcat.2014.12.032
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发表时间:
2015-04-01
影响因子:
7.3
通讯作者:
Roldan, Laura
Roldan, Laura
中科院分区:
化学1区
文献类型:
--
作者:
Fraile, Jose M.;Garcia-Bordeje, Enrique;Roldan, Laura

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磺化的水热碳能够催化棕榈酸和甲醇的酯化反应,每个部位的初始速率比其他众所周知的磺酸固体,包括更强的酸,如Nafion SiO_2,更高。虽然这一较高的每个部位的速率的来源尚不清楚,但它似乎与高表面密度的酸性基团(包括羧酸和磺酸)有关。同时,它们的紧密接近使得表面基团与甲醇的酯化反应的相互活化成为可能。磺酸酯在表面的形成为第二反应产生不可逆的固体部分失活。其他能够使磺酸基团接近的固体,如Dowex,显示出相同的失活模式,但它们的位置不如磺化水热碳中的活性。作为一个额外的优点,这种固体表现出对水存在的增强的稳定性,这使得回收后的行为能够通过最大限度地减少表面酸中心的酯化来改善。(C)2015 Elsevier Inc.保留所有权利。
Sulfonated hydrothermal carbon is able to catalyze the esterification of palmitic acid with methanol at a higher initial rate per site than other well-known sulfonic solids, including stronger acids such as Nafion silica. Although the origin of this higher rate per site is not clear, it seems to be related to high surface density of acid groups (both carboxylic and sulfonic). At the same time, their close proximity makes possible the mutual activation of the surface groups for esterification with methanol. The formation of sulfonate esters on the surface produces irreversible partial deactivation of the solid for a second reaction. Other solids able to bring sulfonic groups close, such as Dowex, show the same deactivation pattern, but their sites are less active than those in sulfonated hydrothermal carbon. As an additional advantage, this solid displays enhanced stability against the presence of water, which enables improvement of the behavior after recovery by minimization of the esterification of the surface acid sites. (C) 2015 Elsevier Inc. All rights reserved.