首页|仿DNase酶的双金属分级多孔MOFs:制备与抗细菌生物膜应用

仿DNase酶的双金属分级多孔MOFs:制备与抗细菌生物膜应用

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本研究成功构建了具有切割DNA能力的双金属枝状大孔金属有机框架(MOFs;HMUiO-66(Zr/Ce)),并将其用于高效破坏生物膜并抑制细菌生长.通过改变Zr/Ce的投料比,可在0-69％的范围内精确调控Zr/Ce的引入量,并控制其粒径在1 μm-150 nm之间.HMUiO-66(Zr/Ce)具有独特的化学和热稳定性,开放的大孔结构和可接近的Lewis酸活性位点,表现出模拟DNA酶活性.双金属MOFs中丰富的Zr-OH位点能有效地捕获核酸,而相邻的Ce-OH基团对磷氧键形成亲核攻击,协同放大DNA的水解速率,使得开发的HMUiO-66(Zr/Ce)能够作为切割细胞外DNA和清除细菌生物膜的纳米药物.在此基础上,我们设计了一种仿生HMUiO-66(Zr/Ce)/PVDF膜,该生物膜可抑制细菌粘附和定植,在抗菌治疗和医疗器械中具有广阔的应用前景.
DNase-mimetics based on bimetallic hierarchically macroporous MOFs for the efficient inhibition of bacterial biofilm
The accumulation of pathogenic biofilms poses a serious threat to human health,making their effective de-struction and eradication significant,yet greatly challenging.Herein,the bimetallic hierarchically macroporous metal-or-ganic frameworks(MOFs)(HMUiO-66(Zr/Ce))with ability to cleave DNA were successfully constructed for the efficient destruction of biofilm and thus inhibition of bacterial growth.By systematically adjusting the feed ratios of Zr/Ce,their particle size could be minimized to approximately 150 nm and the amount of Zr introduced into HMUiO-66(Zr/Ce)could be precisely tailored over a broad molar range from 0 to 69％.The developed HMUiO-66(Zr/Ce)feature unique chemical and thermal stabilities as well as abundant exposed Lewis acid sites.Benefitting from their open macroporous structure and accessible active sites,they exhibit exceptional DNase-mimetic activities.The abundant Zr-OH sites present in bimetallic MOFs could effectively sequester nucleic acids,while adjacent Ce-OH moieties form nucleophilic attacks toward phos-phorus-oxygen bonds,synergistically amplifying the hydro-lysis rate of DNA.Such a unique DNA cleavage ability makes the developed HMUiO-66(Zr/Ce)competent to serve as na-nomedicines for cleaving cross-linked extracellular DNA and eradicating bacterial biofilms.On this basis,we designed a biomimetic HMUiO-66(Zr/Ce)/polyvinylidene difluoride(PVDF)film which could discernibly suppress bacterial ad-herence and colonization,prefiguring their broad application potentials in antimicrobial therapy and medical devices.

hierarchically porous MOFsmacro-microporous UiO-66DNasebacteriabiofilms

夏凡、李可、杨健、陈婧雯、刘熙濛、龚鸣、顾金楼

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Key Laboratory for Ultrafine Materials of Ministry of Education,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China

hierarchically porous MOFs macro-microporous UiO-66 DNase bacteria biofilms

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaChenguang Plan of Shanghai Education Development FoundationProgram of Shanghai Academic/Technology Research Leader

2227505452103314219750725190210621CGA3823XD1401000

2024

10.1007/s40843-023-2687-7

中国科学:材料科学(英文)

中国科学:材料科学(英文)

CSTPCD
ISSN：
年,卷(期)：2024.67(1)
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