Song Ziwei, Bai Juan, Wang Jinyao, Liu Lijuan, Zhu Xu, Jin Xin
Hebei Key Laboratory of Applied Chemistry, Nano-biotechnology Key Lab of Hebei Province, School of Environmental and Chemical Engineering, Yanshan University, 438 West Hebei Street, Qinhuangdao 066004, China.
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, No. 66 Changjiang West Road, Qingdao, Shandong Province 266580, China.
Langmuir. 2022 Jul 12;38(27):8469-8476. doi: 10.1021/acs.langmuir.2c01079. Epub 2022 Jun 28.
The catalytic activity of Prussian blue analogues (PBAs) is mainly tuned via the control of material sizes and morphologies. However, the shapes and sizes of many PBAs are difficult to control. In this work, a facile approach is demonstrated using differently charged surfactants to tune the catalytic activity of PBAs. Fe-Fe PBAs prepared with non-ionic P123, cationic cetyltrimethylammonium bromide, and anionic sodium dodecyl sulfate are chosen to study the effect of surfactant charges on the catalytic activity. The transesterification of propylene carbonate to dimethyl carbonate by methanol is selected as a model reaction. Owing to the different agglomeration processes of PB particles after modified with differently charged surfactants, significantly varied shapes and sizes were observed. Accordingly, the catalytic activity is greatly varied by adding surfactants. The different catalytic activities may arise from the different behaviors of agglomeration of PB particles after surfactant modification as well as the material size and shape changes. Besides, apparent activation energies for PBs adding different surfactants were derived. Finally, the agglomeration mechanism of PB particles in the presence of differently charged surfactants was proposed.
普鲁士蓝类似物（PBAs）的催化活性主要通过控制材料的尺寸和形态来调节。然而，许多PBAs的形状和尺寸难以控制。在这项工作中，展示了一种使用不同电荷的表面活性剂来调节PBAs催化活性的简便方法。选择用非离子型P123、阳离子型十六烷基三甲基溴化铵和阴离子型十二烷基硫酸钠制备的铁-铁PBAs来研究表面活性剂电荷对催化活性的影响。选择碳酸丙烯酯与甲醇酯交换生成碳酸二甲酯作为模型反应。由于用不同电荷的表面活性剂改性后PB颗粒的团聚过程不同，观察到形状和尺寸有显著变化。因此，通过添加表面活性剂，催化活性有很大变化。不同的催化活性可能源于表面活性剂改性后PB颗粒的不同团聚行为以及材料尺寸和形状的变化。此外，还推导了添加不同表面活性剂的PBs的表观活化能。最后，提出了在不同电荷表面活性剂存在下PB颗粒的团聚机理。
