Jung Jooho, Eguchi Marin, Ida Shintaro, Kamada Kai
Graduate School of Engineering, Nagasaki University, 1-14 Bunkyo-machi, Nagasaki 852-8521, Japan.
Faculty of Advanced Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo-ku, Kumamoto 860-8555, Japan.
ACS Appl Bio Mater. 2024 Dec 16;7(12):8590-8598. doi: 10.1021/acsabm.4c01342. Epub 2024 Dec 5.
We fabricated composite membranes containing inorganic nanosheets (NSs) and polymers and demonstrated their outstanding antibacterial performance against several opportunistic pathogens. Layered α-zirconium phosphate [Zr(HPO), α-ZrP] as a pristine compound of NS was exfoliated by ion-exchanging protons in the interlayer space of α-ZrP with bulky tetraalkylammonium ions (TRA: R = butyl, hexyl, and octyl). During the exfoliation process, TRA was electrostatically adsorbed onto α-ZrP NS with a negative surface charge (ZrP-TRA-NS). The produced PMMA membrane including α-ZrP NS (PM-ZrP-TRA-NS) was optically transparent and prohibited bacterial growth, and the effect was stronger for Gram-positive than Gram-negative . The antibacterial activity of PM-ZrP-TRA-NS was based on physical damage induced by both 2D ceramic NSs and sharp alkyl chains of TRA. Despite the inherent flexibility of alkyl chains, when adsorbed onto the NSs, they can act in a manner that effectively pierces the bacterial cell wall. The piercing force of TRA was greater for the longer alkyl chains (TBA < THA < TOA). Focusing on the difference in the cell wall structure between these bacteria, the growth of Gram-positive with loose peptidoglycan layers as an outer membrane could be easily inhibited by contact with the composite film. In contrast, Gram-negative bacteria , surrounded by a relatively dense outer cell wall composed of peptidoglycan and lipopolysaccharide layers, could not be damaged easily. In this study, the antibacterial mechanism of PM-ZrP-TRA-NS membranes was elucidated, and their usefulness as antimicrobial coatings for existing solid surfaces was demonstrated.
我们制备了包含无机纳米片(NSs)和聚合物的复合膜,并证明了它们对几种机会性病原体具有出色的抗菌性能。层状磷酸锆[Zr(HPO),α-ZrP]作为NS的原始化合物,通过在α-ZrP的层间空间中用体积较大的四烷基铵离子(TRA:R = 丁基、己基和辛基)交换质子进行剥离。在剥离过程中,TRA通过静电吸附到具有负表面电荷的α-ZrP NS上(ZrP-TRA-NS)。制备的包含α-ZrP NS的聚甲基丙烯酸甲酯膜(PM-ZrP-TRA-NS)是光学透明的,并且能抑制细菌生长,对革兰氏阳性菌的效果比对革兰氏阴性菌更强。PM-ZrP-TRA-NS的抗菌活性基于二维陶瓷NSs和TRA的尖锐烷基链引起的物理损伤。尽管烷基链具有固有的柔韧性,但当吸附到NSs上时,它们可以以有效刺穿细菌细胞壁的方式起作用。TRA的刺穿力对于较长的烷基链更大(TBA < THA < TOA)。着眼于这些细菌细胞壁结构的差异,具有松散肽聚糖层作为外膜的革兰氏阳性菌的生长可以通过与复合膜接触而容易受到抑制。相比之下,被由肽聚糖和脂多糖层组成的相对致密的外细胞壁包围的革兰氏阴性菌不容易受到损伤。在本研究中,阐明了PM-ZrP-TRA-NS膜的抗菌机制,并证明了它们作为现有固体表面抗菌涂层的实用性。