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. 2022 Aug 9;27(16):5059.
doi: 10.3390/molecules27165059.

A Multiple-Stimuli-Responsive Amphiphilic Copolymer for Antifouling and Antibacterial Functionality via a "Resistance-Kill-Release" Mechanism

Xiaohan Liao  1 , Kai Niu  1 , Feng Liu  1 , Yongming Zhang  1
Affiliations

A Multiple-Stimuli-Responsive Amphiphilic Copolymer for Antifouling and Antibacterial Functionality via a "Resistance-Kill-Release" Mechanism

Xiaohan Liao et al. Molecules. .

Abstract

In recent years, polymers with stimuli-responsive properties have been increasingly reported on due to their diverse applications. However, most of the studies have only focused on the performance of polymers under specific scenarios. The laws of changes in the properties in response to various external stimuli have been less systematically and quantitatively studied. In this paper, we prepared an amphiphilic polymer (PadaMX and PAdaM3QA-X) with temperature-, pH-, ion-, and β-cyclodextrin (β-CD)-responsive properties. According to the cloud point tested by the UV-Vis method, the lower critical soluble temperature (LCST) of PAdaM3QA-10% was more sensitive to a change in pH and less sensitive to a change in ions compared with PadaM3 due to quaternized side chains with a stronger intramolecular mutual repulsion. We then fabricated the coatings with responsive properties by immobilizing the adamantyl groups on β-CD-modified surfaces. The hydrophilicity of the coatings was improved after quaternization, as proven by the water contact angle (WCA) measurement. The antifouling and antibacterial performance was further evaluated via the fluorescence intensity of bovine serum albumin (BSA) adsorbed on the surfaces and the spread plate method. A 78.4% BSA desorption rate and a 96.8% sterilization rate were achieved by the PAdaM3QA-10% coating. In summary, this work prepared a multiple-stimuli-responsive amphiphilic copolymer for antifouling and antibacterial functionality via a "resistance-kill-release" mechanism.

Keywords: amphiphilic polymers; antibacterial; antifouling; host–guest interactions; stimuli-responsive.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
(a) The schematic illustration of the synthesis of AdaMMA; (b) 1H-NMR spectra of AdaMMA (in deuterochloroform).
Figure 2
Figure 2
(a) The schematic illustration of the synthesis of PAdaMX; (b) 1H-NMR spectra of PAdaMX (in deuterochloroform).
Figure 3
Figure 3
(a) The schematic illustration of the synthesis of PAdaM3QA with different degrees of quaternization; (b) 1H-NMR spectra of PAdaM3QA−X (in deuteroxide).
Figure 4
Figure 4
(a) The transmittance of 0.25 wt% PAdaMX solution; (b) the effect of AdaMMA addition on LCST of PAdaMX solution; (c) the transmittance of PAdaM3QA−X solution; (d) the zeta potential of PAdaM3QA−X solution with different degrees of quaternization.
Figure 5
Figure 5
(a) The transmittance of PAdaM3 solution at different pHs; (b) the transmittance of PAdaM3QA−10% solution at different pHs; (c) the zeta potential of PAdaM3QA−10%, PAdaM3, and PAdaM0 solutions at different pHs.
Figure 5
Figure 5
(a) The transmittance of PAdaM3 solution at different pHs; (b) the transmittance of PAdaM3QA−10% solution at different pHs; (c) the zeta potential of PAdaM3QA−10%, PAdaM3, and PAdaM0 solutions at different pHs.
Figure 6
Figure 6
The effect of salt addition on the transmittance of PAdaM3 solution: (a1) NaCl; (a2) NaBr; (a3) KI; (a4) NH4Cl. The effect of salt addition on the transmittance of PAdaM3QA−10% solution: (b1) NaCl; (b2) NaBr; (b3) KI; (b4) NH4Cl.
Figure 7
Figure 7
The effect of different ions on the LCST of (a1) PAdaM3 and (a2) PAdaM3QA−10% solutions; the fitting curve between the ion concentration and the LCST of (b1) PAdaM3 and (b2) PAdaM3QA−10% solutions.
Figure 8
Figure 8
The effect of β-CD on the LCST of (a1) PAdaM3QA−10%, (a2) PadaM3, and (a3) PAdaM0 solutions; partial 2D NMR NOESY spectra of the mixture of β-CD and (b1) PAdaM3QA−10%, (b2) PAdaM3, and (b3) PAdaM0 in water at 30 °C.
Figure 8
Figure 8
The effect of β-CD on the LCST of (a1) PAdaM3QA−10%, (a2) PadaM3, and (a3) PAdaM0 solutions; partial 2D NMR NOESY spectra of the mixture of β-CD and (b1) PAdaM3QA−10%, (b2) PAdaM3, and (b3) PAdaM0 in water at 30 °C.
Figure 9
Figure 9
(a) The images and curves of WCA of PAdaM3 coating; (b) the images and curves of WCA of PAdaM3QA−10% coating.
Figure 10
Figure 10
Fluorescent images of BSA adhered on (a) 37 °C and (b) 4 °C PBS-washed bare silicon wafers, (c) 37 °C and (d) 4 °C PBS-washed PAdaM3QA−10% coatings, and (e) comparison of antifouling performances of bare silicon wafers and PAdaM3QA−10% coatings.
Figure 11
Figure 11
(a) Images of bacterial colonies of (a) bare, (b) PAdaM3, and (c) PAdaM3QA−10% coatings; (d) comparison of antifouling performances of bare, PAdaM3, and PAdaM3QA−10% coatings.
Figure 12
Figure 12
The mechanism of “resistance–kill–release” of PAdaM3QA coating.
Figure 13
Figure 13
The schematic illustration of PAdaM3/PAdaM3QA−10%-Si.
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