4.8 Article

Hydroxyl Radical Generation through the Fenton-like Reaction of Hematin- and Catechol-Functionalized Microgels

期刊

CHEMISTRY OF MATERIALS
卷 32, 期 19, 页码 8182-8194

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c01551

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资金

  1. National Institutes of Health [R15GM104846, R15GM135875, R15GM112082]
  2. Office of the Assistant Secretary of Defense for Health Affairs through the Defense Medical Research and Development Program [W81XWH1810610]
  3. Office of Naval Research [N00014-16-1-2463]
  4. National Science Foundation [DMR 2001076, CBET 1451959]
  5. Mack Chair in Bioengineering
  6. Portage Health Foundation
  7. King-Chavez-Parks Future faculty fellowship
  8. NSF [MRI 1429232]
  9. U.S. Department of Defense (DOD) [W81XWH1810610] Funding Source: U.S. Department of Defense (DOD)

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Hydroxyl radical ((OH)-O-center dot) 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)-O-center dot does not exist. Here, microgels were functionalized with catechol, an adhesive moiety found in mussel adhesive proteins, and hematin (HEM), a hydroxylated Fe3+ 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 H2O2, which was further converted to (OH)-O-center dot by HEM. The generated (OH)-O-center dot was able to degrade organic dyes, including orange II and malachite green. Additionally, the generated (OH)-O-center dot was antimicrobial against both Gram-negative (Escherichia coli) and Gram-positive (Staphylococcus epidermidis) bacteria with the initial concentration of 10(6) to 10(7) cfu/mL. These microgels also reduced the infectivity of a nonenveloped 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, 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( center dot)OH with a wide range of applications.

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