Interfacial Hydrolysis of Acetals on Protonated TEMPO-oxidized Cellulose Nanofibers.
Interfacial Hydrolysis of Acetals on Protonated TEMPO-oxidized Cellulose Nanofibers.
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DOI：
10.1038/s41598-018-23381-8
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发表时间：
2018-03-22
影响因子：
4.6
通讯作者：
Kitaoka T
中科院分区：
文献类型：
--
作者：
Tamura Y;Kanomata K;Kitaoka T
2,2,6,6-四甲基哌啶-1-氧基 (TEMPO) 氧化纤维素纳米纤维 (TOCN) 的晶体表面具有高密度的暴露羧酸基团，可有效充当缩醛水解中的酸催化剂。无羧基纤维素纳米纤维、聚合羧酸和均相乙酸在相同反应条件下没有表现出显着的催化活性。与原始 TOCN 晶体结构不同的丝光 TOCN 也无效，这表明 TOCN 独特的纳米结构特征，如规则排列的羧酸基团、大的比表面积和结构刚性，一定是加速乙缩醛水解的主要因素。动力学分析表明底物和/或酸催化剂物质集中在 TOCN 晶体表面，这显着增强了催化活性。
2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNs), which have a high-density of exposed carboxylic acid groups on their crystalline surfaces, effectively act as acid catalysts in acetal hydrolysis. Carboxy-free cellulose nanofibers, polymeric carboxylic acids, and homogeneous acetic acid do not show significant catalytic activity under the same reaction conditions. Mercerized TOCNs differing from the original TOCNs in a crystalline structure were also ineffective, which suggests that the unique nanoarchitectural features of TOCNs, such as regularly aligned carboxylic acid groups, large specific surface areas, and structural rigidity, must be major factors in the acceleration of acetal hydrolysis. Kinetic analysis suggested that substrates and/or acid catalyst species were concentrated on the TOCN crystalline surfaces, which significantly enhanced the catalytic activity.
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