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Crosslinked Microgels as Platform for Hydrolytic Catalysts
Biomacromolecules ( IF 6.2 ) Pub Date : 2018-03-16 00:00:00 , DOI: 10.1021/acs.biomac.8b00019
Babloo Sharma 1 , Susanne Striegler 1
Affiliation  

In an effort to develop biomimetic glycosyl transfer catalysts, a polymerization protocol was developed that is applicable to the synthesis of crosslinked microgels via UV-initiated free radical polymerization of miniemulsions at ambient temperature and below. The catalytic activity of the microgels derived from butyl acrylate, EGDMA, and a catalyst-precursor ligand was established using the hydrolysis of 4-methylumbelliferyl β-d-galactopyranoside as a model reaction. The microgel-catalyzed hydrolysis was up to 3 × 105-fold accelerated over the background reaction and notably 38-fold faster than the hydrolysis catalyzed by its low molecular weight analog. Dynamic light scattering analysis demonstrated mean hydrodynamic diameters of the particles between 210 and 280 nm and chemical stability of the particles in aqueous solution between pH 1 and 13. A bell-shaped correlation between catalytic proficiency and material rigidity was observed that peaks at 40 mol % of crosslinking content of the microgel.

中文翻译:

交联微凝胶作为水解催化剂的平台

为了开发仿生的糖基转移催化剂,开发了一种聚合方案,该方案可用于在环境温度及以下,通过细乳液的紫外线引发的自由基聚合来合成交联的微凝胶。衍生自丙烯酸丁酯,EGDMA和催化剂前体配体的微凝胶的催化活性是通过使用4-甲基伞形酮基β- d-吡喃半乳糖苷的水解反应建立的。微凝胶催化的水解高达3×10 5相对于本底反应,其水解速度提高了两倍,并且比其低分子量类似物催化的水解速度快了38倍。动态光散射分析表明,颗粒的平均流体力学直径在210至280 nm之间,颗粒在水溶液中的化学稳定性在pH 1和13之间。观察到催化能力与材料刚性之间的钟形相关性,该峰在40 mol%时达到峰值。微凝胶的交联含量。
更新日期:2018-03-16
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