Construction of an Antibacterial Membrane Based on Dopamine and

Article Cite This: ACS Biomater. Sci. Eng. XXXX, XXX, XXX−XXX

pubs.acs.org/journal/abseba

Construction of an Antibacterial Membrane Based on Dopamine and Polyethylenimine Cross-Linked Graphene Oxide Yongxin Zhang, Shuai Chen, Jinxia An, Hao Fu, Xinshi Wu, Chengcai Pang,* and Hui Gao* School of Chemistry and Chemical Engineering, Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion, Tianjin University of Technology, No. 391, West Binshui Road, Tianjin 300384, P. R. China

ACS Biomater. Sci. Eng. Downloaded from pubs.acs.org by UNIV OF SOUTHERN INDIANA on 05/19/19. For personal use only.

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ABSTRACT: Bacterial infections have been considered to be one of the greatest threats to human health. In this study, a covalently cross-linked GO membrane was fabricated through vacuum-assisted filtration self-assembly after being consequentially functionalized with dopamine (GO-PDA) and branched polyethylenimine (GO-PDA-PEI). The characteristics of GO, GO-PDA, and GO-PDA-PEI membranes were confirmed by Xray diffraction, Fourier transform infrared measurements, scanning electron microscopy images, static water contact angle measurements, etc. The GO-PDA-PEI membrane showed extraordinary stability, compared with GO and GO-PDA, confirmed by ultrasonication treatment. Notably, the GO-PDA-PEI membrane exhibited excellent antibacterial efficiency for both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli (more than 99%) upon irradiation by a 795 nm near-infrared (NIR) laser. Interestingly, the GO-PDA-PEI membrane can be recycled, that is, the photothermal effect, as well as the antibacterial activity of the GO-PDA-PEI membrane, remained the same after 5-time recycling. Hence, the proposed system has great potential for future design of recyclable, highly stable, superior bacteriostatic membrane materials. KEYWORDS: efficient antibacterial, cross-linked graphene oxide membrane, stability, photothermal effect, reusable

1. INTRODUCTION Bacterial infections have been considered to be one of the greatest threats to human health, which can lead to a variety of acute or chronic diseases (e.g., inflammation, sepsis, etc.).1 In recent years, graphene oxide (GO) has become a novel type of green broad-spectrum antibacterial material that can exert its antibacterial effect by directly contacting bacterial cell membranes and destructively extracting lipid molecules through sharp edges. These injuries include encapsulation and photothermal ablation mechanisms.2−4 GO can cause bacterial death by cutting, wrapping, and trapping bacteria. The sharp edges of the GO can mechanically destroy the bacterial membrane, causing leakage of intracellular cytoplasm, and the GO sheets can be softened around the bacteria to wrap the bacteria, thereby preventing the bacteria from coming into contact with the external environment. In addition, the flaky GO aggregates can form a network to trap bacteria to inhibit their growth.5 Photothermal antibacterial (PTA) therapy is an effective way to kill bacteria, and many biomaterials have a photothermal effect that produces a large amount of heat under near-infrared (NIR) laser illumination.6,7 The surface of the strain is heated by the photothermal material to denature the protein, which can lead to the death of the strain and avoid drug resistance. PTA is a promising therapeutic strategy, and many research groups have successfully applied some photopolymeric materials to cancer treatment,8 inhibition of bacterial infection,9,10 and accelerated wound healing.11 Moreover, due to the limitations of existing bacteriostatic methods, PTA treatment with few side effects is © XXXX American Chemical Society

worthy of promotion. Because of the efficient photothermal properties of GO, it can generate a large amount of heat in a short time under the illumination of an NIR laser (795 nm), which can enhance the antibacterial property of the composite.11−15 In addition, GO has been used as a carrier for cross-linking various materials such as metal oxides and high molecular polymers due to the superiority of surface structure and functional groups and synergistic effects combined with other compounds, thereby improving the bacteriostatic efficiency.15,16 Based on antimicrobial properties and brilliant biocompatibility, graphene oxide based composites have a wide range of applications in biomedical materials such as antimicrobial film materials, wound dressings, and water disinfection.17−20 GO has become an outstanding carbon material with high specific surface area and rich surface functional groups, which has attracted wide attention in various fields.2,3,20 In particular, GO has been recognized as a very promising candidate for membrane materials, being modified and reacted with various polymer compounds by virtue of the superior specificity of the surface structure to enhance important membrane properties such as selectivity and antibacterial activity and so on.21−24 However, it is worth noting that the toxicity of GO as a liquid form of antibacterial in vitro and in vivo may threaten the Received: January 15, 2019 Accepted: May 13, 2019 Published: May 13, 2019 A

DOI: 10.1021/acsbiomaterials.9b00061 ACS Biomater. Sci. Eng. XXXX, XXX, XXX−XXX

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ACS Biomaterials Science & Engineering

Scheme 1. (a) Preparation Process of the GO-PDA-PEI Membranea and (b) Schematic Diagram of the Bacteriostatic Process of the GO-PDA-PEI Membrane Irradiated by a 795 nm NIR Laser and Recycling Processb

After reacting GO and PDA for 24 h, PEI was added in Tris-HCl buffer for cross-linking. Then, the mixture was vacuum filtered with a 0.22 μm cellulose acetate (CA) membrane filter, and the GO-PDA-PEI membrane was peeled off from the CA support. bAfter incubation with the GOPDA-PEI membrane for 16 h, some of the bacteria died with damaged membranes. Next, after 3 min of laser irradiation at 795 nm, almost all bacteria were killed because of the photothermal effect. The recovered GO-PDA-PEI membrane was further used for the second bacteriostatic experiment. a

environment and human health.25 In addition, the liquid form of GO may pose a risk of microbial growth enhancement effects.26 Therefore, in this study, the solid form of GO was selected as the antibacterial membrane material to further explore the antibacterial activity. Due to the deficient structural stability of the simple GO membrane in aqueous conditions and the insufficient antibacterial properties, the practical application of the GO membrane in applications such as antibacterial dressings is still limited.1,20 Moreover, the GO membrane is easily decomposed in an aqueous solution due to the structural limitations of its surface. Therefore, it is highly appropriate to modify GO with other stable polymers with bacteriostatic properties to prepare a stable and antibacterial polymer material membrane.27−29 Polydopamine (PDA), possessing high concentrations of catecholamine functional groups, with similar structure to the binding proteins of natural mussels, exhibits terrific biocompatibility on various solid material surfaces.29−32 Morover, PDA has excellent bonding ability to various nanomaterials. Because of its biological characteristics, PDA has become a universal coating for a variety of materials and has been used in some biomedical applications.30,33,34 Particularly, the PDA housing can be further surface modified to improve material stability and functionality.32,35

Due to the high reactivity of the amine groups and excellent antibacterial effect, the branched polyethylenimine (PEI) with high density amine groups can also be selected to reduce and modify GO, thereby increasing the antibacterial properties and stability in an aqueous solution.36 In addition, the catechol functional groups in the PDA can react with the amine and imino groups of PEI by Michael addition and Schiff base reaction under weakly basic conditions to form a highly stable cross-linked layer.37 Thus, the resulting membrane manufactured from dopamine functionalized GO and PEI is expected to exhibit exceptional stability in aqueous solution environments.38,39 Moreover, PEI can enhance the antibacterial properties of the GO-PDA-PEI membrane due to its antibacterial activity and excellent binding ability on the membrane surface.38 Herein, dopamine functionalized GO (GO-PDA) and PEI were used for the cross-linking process, and then a covalently cross-linked GO-PDA-PEI membrane was produced by vacuum-assisted filtration self-assembly to obtain a bacteriostatic membrane with favorable stability and excellent antibacterial properties. Its photothermal effect further enhanced the antibacterial activity. Specifically, the produced GO-PDA-PEI membrane could be reused because of its excellent water stability and the stable photothermal effect (Scheme 1). This study set up a foundation for the future study B


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Figure 1. (a) Synthesis process of graphene oxide (GO) and dopamine (DA) under alkaline conditions. (b) Covalent cross-linking reaction between PEI and catechol functional groups in GO-PDA. test tube and cultured in the incubator for 16 h (37 °C, 170 rpm). After shaking for 16 h, the mixture in each tube was serially diluted to the appropriate concentration with PBS buffer solution, and the 0.1 mL of diluted bacteria suspension was transferred to the solid LB agar plate and then incubated at 37 °C for 16−18 h. The number of colony forming units (CFU) was calculated, and the bacterial survival rate was determined. The same method was used for control groups. The antibacterial activity of the membrane after laser irradiation was evaluated using a similar procedure as above. The GO-PDA-PEI membrane was added to a glass test tube containing 1 mL of the diluted bacterial suspension, and the membrane was irradiated with a 795 nm laser (1.5 W cm−2) for 3 min. The tube was then shaken at 170 rpm in the incubator at 37 °C. The subsequent steps were the same as above. 2.3.2. Antibacterial Activity of the Recovered GO-PDA-PEI Membrane. After the GO-PDA-PEI membrane was sterilized, recovered, and then washed three times with ethanol and sterilized by ultraviolet irradiation for 30 min, the recycled membrane was used to evaluate the antibacterial activity of the recycled membrane. The recycled membrane was put into the 1 mL diluted bacterial suspension again and irradiated for 3 min, and colony analysis after 16 h of culture was performed as described above. This recycling cycle was repeated 5 times. The CFU ratio was calculated on the basis of the following equation: CFU ratio = C/C0 × 100%. C and C0 represented the CFU of the experimental group treated with the membrane and the control group without any treatment, respectively. The average and standard deviations obtained from three parallel groups were the final result. 2.4. Statistics Analysis. Significant differences in antibacterial activity assay were evaluated using Student’s t-test.

of recyclable, highly stable, durable, and bacteriostatic membrane materials as dressings and other applications.

2. EXPERIMENTAL SECTION 2.1. Synthesis of the GO-PDA-PEI Membrane. PEI aqueous solution (2 mg mL−1) dispersed in the Tris-HCl buffer solution (20 mL, 10 mM, pH = 8.5) was added into the GO-PDA solution, followed by 1 h of sonication for cross-linking. Then, the mixture of them was vacuum-filtered with a 0.22 μm CA membrane filter and washed with distilled water three times in order to remove unreacted PEI and the remaining buffer solution. After having been peeled off from the CA membrane and dried, the GO-PDA-PEI membrane was obtained. For comparison, a GO membrane was prepared using the same method. 2.2. Photothermal Effect. The GO, GO-PDA, and GO-PDA-PEI membranes were cut into small pieces (4 cm2) of the same proportion and placed in a test tube containing 1 mL of PBS buffer solution (pH = 7.4). Then, these samples were laser-irradiated (795 nm, 1.5 W cm−2) for 5 min. The temperature changes were recorded every 30 s. 2.3. Antibacterial Activity. 2.3.1. Antibacterial Activity of GO, GO-PDA and GO-PDA-PEI Membranes. The antibacterial activity of GO, GO-PDA, and GO-PDA-PEI membranes was investigated using the shake flask method with Staphylococcus aureus (S. aureus, Grampositive) and Escherichia coli (E. coli, Gram-negative). First of all, S. aureus and E. coli were incubated in 5 mL of liquid Luria−Bertani (LB) culture medium at 37 °C for 16−18 h while shaking at 170 rpm in the incubator. After incubation overnight, the bacteria was diluted to a concentration of approximately 107 CFU mL−1 with PBS buffer solution (pH = 7.4). In detail, GO, GO-PDA, and GO-PDA-PEI membrane coupons (4 cm2) were sterilized by ultraviolet irradiation for 30 min and added into 1 mL of the diluted bacterial suspension in the C


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Figure 2. XRD patterns of (a) graphite and GO sheets and (b) GO, GO-PDA, and GO-PDA-PEI membranes. (c) FT-IR spectrum characterization of GO, GO-PDA, and GO-PDA-PEI membranes.

CC bond at 1625 cm−1, CO stretching vibrations at 1725 cm−1, and O−H stretching vibration around 3420 cm−1, respectively.22,24,42 As for GO-PDAs, the absorption peak of the CO bond appeared at 1735 cm−1, attributing to the formation of an ester bond, and an absorption peak of the amide groups was shown in the vicinity of 1600 cm−1 due to the formation of an amide bond. Upon further modication with PEI, the catechol groups of the PDA interacted with the amine groups of PEI, thus new absorption peaks at around 1440 and 1629 cm−1 corresponding to C−N and CN stretching were clearly observed. The surface and side edges morphology of GO, GO-PDA, and GO-PDA-PEI membranes was evaluated by SEM imaging (Figure 3). In addition to the wrinkles on the surface of the

3. RESULTS AND DISCUSSION 3.1. Fabrication and Characterization of Membranes. The GO sheets were fabricated from natural flake graphite by utilizing the ameliorative Hummer’s method.40 The characteristics of GO were further gathered and affirmed by X-ray diffraction (XRD), Fourier transform infrared (FT-IR) measurements, scanning electron microscopy (SEM) images, and static water contact angle measurements. As shown in Figure S1, the morphology of GO was in accord with the previous report,41 and the thickness of the monolithic GO material was approximately 25 nm. To obtain GO-PDA, the mixture of GO and dopamine was dispersed in Tris-HCl buffer (pH = 8.5) and stirred for 24 h (Figure 1a).24,42 Then, GO-PDA and PEI in Tris-HCl buffer were mixed in equal volume and ultrasonicated for another 1 h. Subsequently, the mixture was vacuum filtered with a 0.22 μm CA membrane filter, followed by being washed with distilled water three times to remove the unreacted raw materials, buffer solution, and impurities (Figure 1b). Since the amine groups of PEI and the catechol groups of PDA were covalently crosslinked under alkaline conditions in addition to the electrostatic interaction between them, it is reasonable to suppose that the resulting GO-PDA-PEI membrane was very stable under aqueous conditions. XRD spectral analysis of graphite, GO, GO-PDA, and GOPDA-PEI membranes is shown in Figure 2a,b. The diffraction peak of graphite demonstrated 2θ = 26.4°, revealing that the corresponding interlayer distance was 0.34 nm. For GO, a narrow and high diffraction peak at 2θ of 10.3° appeared after the oxidation reaction (with a corresponding interlayer distance of 0.86 nm), which contributed to the oxygen-containing functional groups formed on the GO surface (Figure 2a).24,37,39 With reduction of dopamine, a new absorption peak of 2θ of 8.2° in the XRD spectrum of the GO-PDA membrane appeared, demonstrating that GO was successfully reduced by dopamine and the interlayer spacing increased (1.08 nm). Subsequently, after cross-linking with PEI, a new diffraction peak (2θ = 6.1°) appeared, corresponding to the interlayer distance of 1.45 nm, a larger interlayer distance compared with GO-PDA, which was probably due to the electrostatic interactions, as well as the formation of the chemical bonds between the functional groups on the surface of the GO-PDA membrane and the amino groups of the PEI (Figure 2b). FT-IR spectra of GO, GO-PDA, and GO-PDA-PEI membranes are shown in Figure 2c. The spectrum of GO exhibited C−O−C stretching vibrations around 1259 cm−1,

Figure 3. SEM imaging of GO, GO-PDA, and GO-PDA-PEI membranes. Scale bars: 1 μm.

membranes, all of the membranes showed a good stacking structure. Consistent with the XRD characterization results, after PEI was embedded, a larger interlayer spacing was formed, which made the GO-PDA-PEI membrane thicker and looser. As shown in Figure S2, the surface hydrophilicity of GO, GOPDA, and GO-PDA-PEI membranes was evaluated by static water contact angle. The water contact angle of GO-PDA (55.5°) and GO-PDA-PEI (63.8°) membranes was successively increased, compared with that of the GO membrane (40.8°), which was probably due to the decreased hydrophilic oxygen D


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laser irradiation, and after 5 min of irradiation, the temperature also showed an upward trend, which proved its excellent photothermal performance (Figure 5a). The GO membrane shown in Figure 5a had better NIR absorption than other GO membranes (GO-PDA and GO-PDA-PEI). The photothermal effect of the membrane material was mainly caused by GO, and the photothermal experiment in this study was carried out with the membrane of the same volume. Thus, the GO content of the GO membrane was inevitably higher than that of the GO-PDA and GO-PDA-PEI membranes. As a consequence, the GO membrane had better NIR absorption than other membranes. To test the photothermal stability of the GO-PDA-PEI membrane, repeated on and off laser irradiation was performed. As shown in Figure 5b, the temperature of the PBS solution containing the GO-PDA-PEI membrane exhibited a distinguished on−off effect with or without 795 nm laser irradiation. The photothermal effect remained unchanged even after repeated treatments 5 times, indicating high photothermal stability of the GO-PDA-PEI membrane. Moreover, Figure S3 shows the photothermal statistics of the GO-PDA-PEI membrane recovered 5 times. The results further confirmed that the photothermal effect of the GO-PDA-PEI membrane of the three groups was not reduced after 5 times of recovery. It was considered whether there was a structural change after the GO-PDA-PEI membrane was irradiated with the NIR laser. Since the XRD and FT-IR characterizations of GO and reduced graphene oxide (rGO) are quite different,43 we performed XRD analysis and FT-IR measurement on the GO-PDA-PEI membrane before and after laser irradiation. The GO-PDAPEI membrane repeatedly irradiated with 795 nm laser 5 times (3 min × 5) was characterized by XRD and FT-IR measurements and then compared with the original GO-PDA-PEI membrane. As shown in Figure S4, the GO-PDA-PEI membrane treated with 795 nm laser irradiation or not exhibited the same XRD and FT-IR spectrum characterizations indicating that NIR laser irradiation did not induce the formation reduced GO. 3.4. Antibacterial Activity. The antibacterial property of GO, GO-PDA, and GO-PDA-PEI membranes and GO-PDAPEI membranes in combination with the photothermal effect was evaluated (Figure 6).44−47 GO and GO-PDA membranes had certain inhibitory effects on S. aureus (51.8%, 42.9% of CFU ratio) and E. coli (31.6%, 26.8% of CFU ratio). Compared to S. aureus, the inhibition of E. coli was slightly better. As expected, the GO-PDA-PEI membrane had better bacteriostatic effect than the former two with a CFU ratio of 9.47% and 3.92% for S. aureus and E. coli, respectively. Notably, after 3 min of 795 nm

functional groups on the GO surface upon the reduction of GO and the cross-linking of PEI.24,28 3.2. Stability of the Membranes in Aqueous Solution. Figure 4a displayed the optical photographs of GO, GO-PDA,

Figure 4. (a) Optical photographs of GO, GO-PDA, and GO-PDA-PEI membranes. (b) Evaluation of stability in water environments: GO, GO-PDA, and GO-PDA-PEI membranes were placed in an aqueous solution, ultrasonicated for 5 min, and redispersed in water, followed by being immersed in the water for a week.

and GO-PDA-PEI membranes created by the vacuum filtration assisted method. The individual GO membrane was brown, while the color of the GO-PDA composite membrane became black. After cross-linking with PEI, the membrane remained black and possessed a smooth and shiny surface. According to Figure 4b, after 5 min of ultrasonication, the GO and GO-PDA membranes began to redisperse in water. In contrast, the GOPDA-PEI membrane could not be broken by ultrasonication, and even after being left in water for 1 week, it did not disperse in water. The PEI chain further cross-linked with both composites of GO and PDA, showing better stability and water resistance. 3.3. Photothermal Properties. Under 795 nm NIR laser irradiation, GO had exceptional photothermal property. Notably, modification with PDA and PEI did not significantly bother the photothermal performance of GO. The GO-PDAPEI membrane can be heated to about 67 °C after 3 min of NIR

Figure 5. (a) Photothermal curves of PBS, GO, GO-PDA, and GO-PDA-PEI membranes under 5 min of 795 nm NIR laser irradiation. (b) The temperature rising and cooling curve of the GO-PDA-PEI membrane in the presence and absence of 795 nm NIR laser irradiation. E


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Figure 6. (a) Colony forming units (CFU) for S. aureus and E. coli of a control group without any treatment, PBS + laser, GO membrane, GO-PDA membrane, GO-PDA-PEI membrane, GO-PDA-PEI membrane + laser, and recycled GO-PDA-PEI membrane + laser (5 times). Quatitative results of CFU of (b) S. aureus and (c) E. coli. Note: The asterisk (*) indicates a significant difference between the two groups (p < 0.05). Results are mean ± standard deviation (n = 3).

Figure 7. SEM images of S. aureus and E. coli treated with PBS, GO membrane, GO-PDA membrane, GO-PDA-PEI membrane, and GO-PDA-PEI membrane + laser. Scale bars: 200 nm.

coli (Figure 7a,b).44,45 To visually observe the changes in bacterial morphology before and after the treatment, the bacteria without any treatment were designed as a negative control. Clear cell membrane margins and intact bacterial morphology were observed for S. aureus and E. coli in the control group. After the GO membrane treatment, the bacterial morphology changed slightly, and a few deformations occurred. After treatment with the GO-PDA membrane, the bacteria deformation and collapse were more serious, while the state of bacterial damage was further severe compared to the former two after treatment with the GO-PDA-PEI membrane. Finally, after the NIR laser irradiation, due to the synergistic photothermal effect, the bacterial cell membrane of both S. aureus and E. coli completely collapsed, split, and deformed. These results observed by SEM were consistent with the consequence of previous antimicrobial experiments. The antibacterial activity against S. aureus and E. coli was further explored by confocal microscopy (Figure S5a,b). Herein, live bacteria with intact cell membranes were stained green using acridine orange (AO), while dead bacteria with cell membrane damage were stained red by ethidium bromide (EB). After being

NIR laser irradiation, the GO-PDA-PEI membrane, combined with the photothermal effect, exhibited the best antibacterial activity (over 99%) for both S. aureus and E. coli. It is proved that the GO-PDA-PEI membrane itself had good antibacterial properties, and the antibacterial property of the composite membrane can be further improved by using its favorable photothermal effect. For microorganisms, the temperature can be locally raised by a photothermal agent (50 °C) so that the denaturation of the protein causes the death of the microorganisms.48 Thus, for the GO-PDA-PEI membrane, based on its effective antibacterial activity, the elevated temperature can be controlled by changing the time of laser irradiation, so that it can obtain better antibacterial efficiency at lower temperatures. Interestingly, the GO-PDA-PEI membrane can be recycled and reused. Based on its photothermal stability and its modality stability, the GO-PDA-PEI membrane was recycled and irradiated 5 times in bacteriostatic experiments, with every recycling showing excellent antibacterial activity (over 99%). To obtain further evidence of the proposed antimicrobial behavior of GO, GO-PDA, and GO-PDA-PEI membranes, SEM was used to observe morphological changes in S. aureus and E. F



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ACKNOWLEDGMENTS The authors thank the National Natural Science Foundation of China (21674080), 131 Talents Program of Tianjin, Distinguished Professor of Tianjin, the Leading Talents Program of the Tianjin Educational Committee, Key Program of Tianjin Municipal Natural Science Foundation (No. 18JCZDJC37700), and Training Project of Innovation Team of Colleges and Universities in Tianjin (TD13-5020) for financial support.

stained for 30 min, untreated bacterial cells (S. aureus and E. coli) showed uniform green fluorescence. On the contrary, the bacteria (S. aureus and E. coli) incubated with the GO-PDA-PEI membrane irradiated with 795 nm laser almost turned to the red fluorescence, indicating the potent antibacterial activity. The results confirmed that the bacteria treated by the laser irradiated GO-PDA-PEI membrane can induce the destruction of the bacterial membrane, which was favorable for the EB to enter the bacteria. Furthermore, Table S1 summarizes the bacteriostatic efficiency of some GO functionalized membranes. Compared with other antibacterial membranes, the proposed GO-PDAPEI membrane can achieve high antibacterial activity in combination with the photothermal effect, further demonstrating the great potential of the GO-PDA-PEI membrane as an antibacterial membrane for biomedical applications.

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ASSOCIATED CONTENT

S Supporting Information *

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsbiomaterials.9b00061.

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REFERENCES

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4. CONCLUSIONS In summary, we have designed a composite bacteriostatic membrane fabricated from covalently cross-linked dopaminefunctionalized graphene oxide (GO-PDA) and branched polyethylenimine (PEI), followed by vacuum-assisted filtration self-assembly. The GO-PDA-PEI membrane exhibited exceptional stability in aqueous solution. Simultaneously, on the basis of GO’s favorable photothermal effect, the composite membrane displayed an excellent photothermal effect under 795 nm NIR laser irradiation. It is worthy of consideration that we have synergistically combined antibacterial activity of the GO-PDA-PEI membrane and the photothermal effect, achieving a bacteriostatic efficiency of more than 99% for the GO-PDAPEI membrane. Interestingly, the GO-PDA-PEI membrane could be recycled because of its high stability, and the photothermal effect and bacteriostatic efficiency remained unchanged after 5 times of recovery. Therefore, an organic− inorganic hybridization membrane, with good stability, predominant photothermal effect, and improved antibacterial activity, was constructed and can serve as a highly stable bacteriostatic membrane material. Moreover, the proposed GOPDA-PEI membrane may be instructive for some environmental/sensing applications in the future, such as sewage treatment, water desalination, salt/dye/heavy metal separation, etc.

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Experimental sections including preparation of GO, GOPDA, bacterial culture, SEM and confocal microscopy imaging studies, XRD and FT-IR characterizations, and water contact angle measurement (PDF)

AUTHOR INFORMATION

Corresponding Authors

*E-mail: [email protected] (H.G.). *E-mail: [email protected] (C.C.P.). ORCID

Chengcai Pang: 0000-0003-0734-5290 Hui Gao: 0000-0002-5009-9999 Notes

The authors declare no competing financial interest. G


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Construction of an Antibacterial Membrane Based on Dopamine and

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