Centro de Química Estrutural and Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, Portugal.
Departamento de Química e Bioquímica, Faculdade de Ciências, Universidade de Lisboa, Campo Grande, 1749-016 Lisboa, Portugal.
ACS Appl Mater Interfaces. 2021 Mar 24;13(11):12836-12844. doi: 10.1021/acsami.0c19446. Epub 2021 Mar 11.
This study describes a template-mediated self-assembly synthesis, full characterization, and structural features of two new silver-based bioactive coordination polymers (CPs) and their immobilization into acrylated epoxidized soybean oil (ESOA) biopolymer films for antimicrobial applications. The 3D silver(I) CPs [Ag(μ-Hpma)]·4HO () and [Ag(μ-Htma)(HO)]·2HO () were generated from AgNO and pyromellitic (Hpma) or trimesic (Htma) acid, also using ,'-dimethylethanolamine (Hdmea) as a template. Both and feature the intricate 3D layer-pillared structures driven by distinct polycarboxylate blocks. Topological analysis revealed binodal nets with the and /hc topology in and , respectively. These CPs were used for fabricating new hybrid materials, namely, by doping the [ESOA] biopolymer films with very low amounts of and (0.05, 0.1, and 0.5%). Their antimicrobial activity and ability to impair bacterial biofilm formation were investigated in detail against both Gram-positive ( and ) and Gram-negative ( and ) bacteria. Both silver(I) CPs and derived biopolymer films showed activity against all the tested bacteria in a concentration-dependent manner. Compound exhibited a more pronounced activity, especially in preventing biofilm growth, with mean bacterial load reductions ranging from 3.7 to 4.3 log against the four bacteria (99.99% bacterial eradication). The present work thus opens up antibiofilm applications of CP-doped biopolymers, providing new perspectives and very promising results for the design of functional biomaterials.
本研究描述了一种模板介导的自组装合成方法,对两种新的基于银的生物活性配位聚合物(CPs)进行了全面表征和结构分析,并将其固定在丙烯酰化氧化大豆油(ESOA)生物聚合物薄膜中,用于抗菌应用。通过 AgNO 和均苯三甲酸(Hpma)或均苯三甲酸(Htma),以及使用,'-二甲乙醇胺(Hdmea)作为模板,生成了 3D 银(I)CPs [Ag(μ-Hpma)]·4HO () 和 [Ag(μ-Htma)(HO)]·2HO ()。这两个 CP 都具有由不同多羧酸基块驱动的复杂的 3D 层-支柱结构。拓扑分析表明,在 中具有 /hc 拓扑结构,而在 中具有 binodal 网络。这些 CP 被用于制造新的杂化材料,即通过用非常低的量的 和 (0.05、0.1 和 0.5%)掺杂 [ESOA] 生物聚合物薄膜。详细研究了它们对革兰氏阳性菌( 和 )和革兰氏阴性菌( 和 )的抗菌活性和抑制细菌生物膜形成的能力。两种银(I)CP 和衍生的生物聚合物薄膜都表现出浓度依赖性的抗菌活性。化合物 表现出更明显的活性,特别是在防止生物膜生长方面,对四种细菌的平均细菌负载减少了 3.7 至 4.3 个对数(99.99%的细菌根除)。因此,本研究为 CP 掺杂生物聚合物的抗生物膜应用开辟了新的途径,为设计功能性生物材料提供了新的视角和非常有前景的结果。