Biocidal Potency of Polymers with Bulky Cations
Biocidal Potency of Polymers with Bulky Cations
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DOI：
10.1021/acsmacrolett.2c00726
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发表时间：
2023-01-26
影响因子：
7.015
通讯作者：
Palermo，Edmund F.
中科院分区：
文献类型：
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作者：
Lou，Yang;Gaitor，Jamie;Palermo，Edmund F.
抗微生物聚合物的性能敏感地取决于阳离子种类、电荷密度和阳离子的空间排列。在这里，我们报告的抗微生物聚合物轴承异常庞大的四氨基膦基团的高度离域阳离子电荷的来源。庞大的阳离子大大提高了两亲性聚合物的杀生物活性，导致在亚微摩尔范围内的显着有效的活性。以四氨基膦为侧基的阳离子聚异戊二烯对大肠杆菌的杀灭率达98%以上。大肠杆菌浓度为0.1 μg/mL时，对大肠杆菌的抑制率为4-log。在2 μg/mL的浓度下，2 h内对大肠杆菌显示出非常快速和有效的杀菌活性。聚合物在相似浓度下也具有高度溶血性，表明具有杀生物活性特征。聚合物的化学结构相似，但具有更灵活的主链，以检查聚合物链的灵活性对其活性的影响，这被证明是边际的。我们还探索了具有不同间隔臂基团的变体，所述间隔臂基团将阳离子与主链分开。在所有情况下的抗菌活性是强有力的，但具有较短间隔臂基团的聚合物显示出更快的杀菌动力学。有趣的是，观察到明显的反作用。紧密结合的PF 6-抗衡阴离子在高浓度下表现出较差的活性，由于总的聚集体形成和沉淀从测定介质中，而松散结合的Cl-抗衡离子导致非常有效的活性，单调地增加浓度。在本文中，我们揭示了大体积的鏻阳离子与显着增强的生物杀灭活性，这提供了一个创新的策略，以开发更有效的自消毒材料。
The performance of antimicrobial polymers depends sensitively on the type of cationic species, charge density, and spatial arrangement of cations. Here we report antimicrobial polymers bearing unusually bulky tetraaminophosphonium groups as the source of highly delocalized cationic charge. The bulky cations drastically enhanced the biocidal activity of amphiphilic polymers, leading to remarkably potent activity in the submicromolar range. The cationic polynorbornenes with pendent tetraaminophosphonium groups killed over 98%E. coliat a concentration of 0.1 μg/mL and caused a 4-log reduction ofE. coliwithin 2 h at a concentration of 2 μg/mL, showing very rapid and potent bactericidal activity. The polymers are also highly hemolytic at similar concentrations, indicating a biocidal activity profile. Polymers of a similar chemical structure but with more flexible backbones were made to examine the effects of the flexibility of polymer chains on their activity, which turned out to be marginal. We also explore variants with different spacer arm groups separating the cations from the backbone main chain. The antibacterial activity was comparably potent in all cases, but the polymers with shorter spacer arm groups showed more rapid bactericidal kinetics. Interestingly, pronounced counterion effects were observed. Tightly bound PF6–counteranions showed poor activity at high concentrations due to gross aggregate formation and precipitation from the assay media, whereas loosely bound Cl–counterions resulted in very potent activity that monotonically increased with increasing concentration. In this paper, we reveal that bulky phosphonium cations are associated with markedly enhanced biocidal activity, which provides an innovative strategy to develop more effective self-disinfecting materials.