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通过血红素和儿茶酚功能化微凝胶的类芬顿反应产生羟基自由基

Hydroxyl Radical Generation Through the Fenton-Like Reaction of Hematin- and Catechol-Functionalized Microgels.

作者信息

Forooshani Pegah Kord, Pinnaratip Rattapol, Polega Elizabeth, Tyo Ariana G, Pearson Eric, Liu Bo, Folayan Tinu-Ololade, Pan Lei, Rajachar Rupak M, Heldt Caryn L, Lee Bruce P

机构信息

Department of Biomedical Engineering, Michigan Technological University, Houghton, MI 49931, USA.

Department of Chemical Engineering, Michigan Technological University, Houghton, MI 49931, USA.

出版信息

Chem Mater. 2020 Oct 13;32(19):8182-8194. doi: 10.1021/acs.chemmater.0c01551. Epub 2020 Sep 4.

Abstract

Hydroxyl radical (OH) is a potent reactive oxygen species with the ability to degrade hazardous organic compounds, kill bacteria, and inactivate viruses. However, an off-the-shelf, portable, and easily activated biomaterial for generating OH does not exist. Here, microgels were functionalized with catechol, an adhesive moiety found in mussel adhesive proteins, and hematin (HEM), a hydroxylated Fe ion-containing porphyrin derivative. When the microgel was hydrated in an aqueous solution with physiological pH, molecular oxygen in the solution oxidized catechol to generate HO, which was further converted to OH by HEM. The generated OH was able to degrade organic dyes, including orange II and malachite green. Additionally, the generated OH was antimicrobial against both gram-negative () and gram-positive () bacteria with the initial concentration of 10-10 CFU/mL. These microgels also reduced the infectivity of a non-enveloped porcine parvovirus and an enveloped bovine viral diarrhea virus by 3.5 and 4.5 log reduction values, respectively (99.97-99.997% reduction in infectivity). These microgels were also functionalized with positively charged [2-(methacryloyloxy)ethyl] trimethylammonium chloride (METAC), which significantly enhanced the antibacterial and antiviral activities through electrostatic interaction between the negatively charged pathogens and the microgel. These microgels can potentially serve as a lightweight and portable source of disinfectant, for an on-demand generation of OH with a wide range of applications.

摘要

羟基自由基(OH)是一种具有强氧化性的活性氧物种,能够降解有害有机化合物、杀灭细菌并使病毒失活。然而,目前尚不存在一种现成的、便携式且易于激活的用于产生OH的生物材料。在此,微凝胶用儿茶酚(贻贝粘附蛋白中的一种粘附部分)和血晶素(HEM,一种含羟基铁离子的卟啉衍生物)进行功能化修饰。当微凝胶在生理pH值的水溶液中水合时,溶液中的分子氧将儿茶酚氧化生成HO,HO再通过血晶素进一步转化为OH。生成的OH能够降解有机染料,包括橙黄II和孔雀石绿。此外,生成的OH对初始浓度为10-10 CFU/mL的革兰氏阴性菌和革兰氏阳性菌均具有抗菌活性。这些微凝胶还分别将非包膜猪细小病毒和包膜牛病毒性腹泻病毒的感染性降低了3.5和4.5个对数减少值(感染性降低99.97 - 99.997%)。这些微凝胶还用带正电荷的[2-(甲基丙烯酰氧基)乙基]三甲基氯化铵(METAC)进行了功能化修饰,通过带负电荷的病原体与微凝胶之间的静电相互作用显著增强了抗菌和抗病毒活性。这些微凝胶有望作为一种轻便的便携式消毒剂来源,用于按需产生OH并具有广泛的应用。

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