Polydopamine/silver hybrid coatings on soda-lime glass spheres with controllable release ability for inhibiting biofilm formation

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  • ReceivedNov 15, 2019
  • AcceptedJan 13, 2020
  • PublishedMar 4, 2020


Funded by

the Longshan Academic Talent Research Supporting Program of SWUST(18LZX447)

and the Biofilm Research & Innovation Consortium from the College of Science and Engineering

Flinders University.


Zhang H and Tang Y are grateful to the Longshan Academic Talent Research Supporting Program of SWUST (18LZX447) and the biofilm research & innovation consortium from the College of Science and Engineering, Flinders University for supporting this research, respectively.

Interest statement

The authors declare that they have no conflict of interest.

Contributions statement

Zhang HW and Tang Y designed the research. Shi Q fabricated the materials, did the characterizations, analyzed the results and drafted the manuscript with support from Zhang HP, Zhao P and Zhang Y. Zhang HP and Tang Y revised the manuscript. All authors contributed to the general discussion.

Author information

Quanbin Shi received his master’s degree from Southwest University of Science and Technology in 2013. During this period, he mainly studied the degradation characteristics of degradable mulch under natural composting conditions. He entered the School of Environmental Science and Engineering, Tianjin University for PhD study in 2013. During his PhD, his main research direction is the preparation of surface modified glass spheres and the study of their adsorption properties.

Hongwei Zhang is the Director of the Institute of Sustainable Development of Resources, Environment, Ecology and Society of Tianjin University. He graduated from Tianjin University with a major in water supply and drainage in 1982 and obtained a doctorate degree in engineering in 2002 in Tianjin University. For many years, he has been engaged in scientific research and teaching in the application of membrane technology in water treatment processes, mathematical simulation and optimal operation of urban water supply systems.

Youhong Tang obtained his PhD degree in the Hong Kong University of Science and Technology in 2007. He moved to Flinders University with an ARC-DECRA in 2012 from the Centre for Advanced Materials Technology, the University of Sydney. Prof. Tang is a material science and engineering researcher with research interests mainly focused on the structure-process-property relations of polymeric materials and nanocomposites, especially on multifunctional and value-added nanocomposites and bioresources, biomaterials and biosensors, especially incorporating novel aggregation-induced emission materials.


[1] Adeleye AS, Conway JR, Garner K, et al. Engineered nanomaterials for water treatment and remediation: Costs, benefits, and applicability. Chem Eng J, 2016, 286: 640-662 CrossRef Google Scholar

[2] Bolto B, Gregory J. Organic polyelectrolytes in water treatment. Water Res, 2007, 41: 2301-2324 CrossRef PubMed Google Scholar

[3] Srivastava NK, Majumder CB. Novel biofiltration methods for the treatment of heavy metals from industrial wastewater. J Hazard Mater, 2008, 151: 1-8 CrossRef PubMed Google Scholar

[4] Herrmann S, De Matteis L, de la Fuente JM, et al. Removal of multiple contaminants from water by polyoxometalate supported ionic liquid phases (POM-SILPs). Angew Chem Int Ed, 2017, 56: 1667-1670 CrossRef PubMed Google Scholar

[5] Di Cesare A, Eckert EM, D’Urso S, et al. Co-occurrence of integrase 1, antibiotic and heavy metal resistance genes in municipal wastewater treatment plants. Water Res, 2016, 94: 208-214 CrossRef PubMed Google Scholar

[6] Huang X, Jiao T, Liu Q, et al. Hierarchical electrospun nanofibers treated by solvent vapor annealing as air filtration mat for high-efficiency PM2.5 capture. Sci China Mater, 2019, 62: 423-436 CrossRef Google Scholar

[7] Aslan S, Cakici H. Biological denitrification of drinking water in a slow sand filter. J Hazard Mater, 2007, 148: 253-258 CrossRef PubMed Google Scholar

[8] Lim HS, Lim W, Hu JY, et al. Comparison of filter media materials for heavy metal removal from urban stormwater runoff using biofiltration systems. J Environ Manage, 2015, 147: 24-33 CrossRef PubMed Google Scholar

[9] Cheng Y, Huang T, Cheng L, et al. Structural characteristic and ammonium and manganese catalytic activity of two types of filter media in groundwater treatment. J Environ Sci, 2018, 72: 89-97 CrossRef PubMed Google Scholar

[10] Freitas de Oliveira F, Schneider RP. Slow sand filtration for biofouling reduction in seawater desalination by reverse osmosis. Water Res, 2019, 155: 474-486 CrossRef Google Scholar

[11] Bar-Zeev E, Passow U, Romero-Vargas Castrillón S, et al. Transparent exopolymer particles: From aquatic environments and engineered systems to membrane biofouling. Environ Sci Technol, 2015, 49: 691-707 CrossRef PubMed Google Scholar

[12] Mansouri J, Charlton T, Chen V, et al. Biofouling performance of silver-based PES ultrafiltration membranes. Desalin Water Treat, 2016, 57: 28100-28114 CrossRef Google Scholar

[13] Park JA, Lee SC, Kim SB. Synthesis of dual-functionalized poly(vinyl alcohol)/poly(acrylic acid) electrospun nanofibers with enzyme and copper ion for enhancing anti-biofouling activities. J Mater Sci, 2019, 54: 9969-9982 CrossRef Google Scholar

[14] Yin J, Deng B. Polymer-matrix nanocomposite membranes for water treatment. J Membrane Sci, 2015, 479: 256-275 CrossRef Google Scholar

[15] Souza LRR, da Silva VS, Franchi LP, et al. Toxic and beneficial potential of silver nanoparticles: The two sides of the same coin. Adv Exp Med Biol, 2018, 1048: 251–262. Google Scholar

[16] Baruah S, Najam Khan M, Dutta J. Perspectives and applications of nanotechnology in water treatment. Environ Chem Lett, 2016, 14: 1-14 CrossRef Google Scholar

[17] Lee H, Dellatore SM, Miller WM, et al. Mussel-inspired surface chemistry for multifunctional coatings. Science, 2007, 318: 426-430 CrossRef PubMed Google Scholar

[18] Liu Y, Ai K, Lu L. Polydopamine and its derivative materials: Synthesis and promising applications in energy, environmental, and biomedical fields. Chem Rev, 2014, 114: 5057-5115 CrossRef PubMed Google Scholar

[19] Ryu JH, Messersmith PB, Lee H. Polydopamine surface chemistry: A decade of discovery. ACS Appl Mater Interfaces, 2018, 10: 7523-7540 CrossRef Google Scholar

[20] Lee HA, Ma Y, Zhou F, et al. Material-independent surface chemistry beyond polydopamine coating. Acc Chem Res, 2019, 52: 704-713 CrossRef PubMed Google Scholar

[21] Hebbar RS, Isloor AM, Ananda K, et al. Fabrication of polydopamine functionalized halloysite nanotube/polyetherimide membranes for heavy metal removal. J Mater Chem A, 2016, 4: 764-774 CrossRef Google Scholar

[22] Fu J, Chen Z, Wang M, et al. Adsorption of methylene blue by a high-efficiency adsorbent (polydopamine microspheres): Kinetics, isotherm, thermodynamics and mechanism analysis. Chem Eng J, 2015, 259: 53-61 CrossRef Google Scholar

[23] Lu Z, Xiao J, Wang Y, et al. In situ synthesis of silver nanoparticles uniformly distributed on polydopamine-coated silk fibers for antibacterial application. J Colloid Interface Sci, 2015, 452: 8-14 CrossRef PubMed Google Scholar

[24] Tang P, Han L, Li P, et al. Mussel-inspired electroactive and antioxidative scaffolds with incorporation of polydopamine-reduced graphene oxide for enhancing skin wound healing. ACS Appl Mater Interfaces, 2019, 11: 7703-7714 CrossRef Google Scholar

[25] LaMarche CQ, Leadley S, Liu P, et al. Method of quantifying surface roughness for accurate adhesive force predictions. Chem Eng Sci, 2017, 158: 140-153 CrossRef Google Scholar

[26] Ge L, Han C, Liu J, et al. Enhanced visible light photocatalytic activity of novel polymeric g-C3N4 loaded with Ag nanoparticles. Appl Catal A-General, 2011, 409: 215-222 CrossRef Google Scholar

[27] Zhang P, Shao C, Zhang Z, et al. In situ assembly of well-dispersed Ag nanoparticles (AgNPs) on electrospun carbon nanofibers (CNFs) for catalytic reduction of 4-nitrophenol. Nanoscale, 2011, 3: 3357-3363 CrossRef PubMed Google Scholar

[28] Spori DM, Drobek T, Zürcher S, et al. Beyond the lotus effect: Roughness influences on wetting over a wide surface-energy range. Langmuir, 2008, 24: 5411-5417 CrossRef PubMed Google Scholar

[29] Drelich J, Chibowski E. Superhydrophilic and superwetting surfaces: Definition and mechanisms of control. Langmuir, 2010, 26: 18621-18623 CrossRef PubMed Google Scholar

[30] Guldiren D, Aydın S. Antimicrobial property of silver, silver-zinc and silver-copper incorporated soda lime glass prepared by ion exchange. Mater Sci Eng-C, 2017, 78: 826-832 CrossRef PubMed Google Scholar

[31] Ma Y, Niu H, Zhang X, et al. Colorimetric detection of copper ions in tap water during the synthesis of silver/dopamine nanoparticles. Chem Commun, 2011, 47: 12643-12645 CrossRef PubMed Google Scholar

[32] Ma S, Ye Q, Pei X, et al. Antifouling on Gecko’s feet inspired fibrillar surfaces: Evolving from land to marine and from liquid repellency to algae resistance. Adv Mater Interfaces, 2015, 2: 1500257 CrossRef Google Scholar

[33] Sirmerova M, Prochazkova G, Siristova L, et al. Adhesion of Chlorella vulgaris to solid surfaces, as mediated by physicochemical interactions. J Appl Phycol, 2013, 25: 1687-1695 CrossRef Google Scholar

[34] Sekar R, Venugopalan VP, Satpathy KK, et al. Laboratory studies on adhesion of microalgae to hard substrates. Hydrobiologia, 2004, 512: 109-116 CrossRef Google Scholar

[35] Zhou K, Hu Y, Zhang L, et al. The role of exopolymeric substances in the bioaccumulation and toxicity of Ag nanoparticles to algae. Sci Rep, 2016, 6: 32998 CrossRef PubMed Google Scholar

[36] Hazeem LJ, Kuku G, Dewailly E, et al. Toxicity effect of silver nanoparticles on photosynthetic pigment content, growth, ROS production and ultrastructural changes of microalgae Chlorella vulgaris. Nanomaterials, 2019, 9: 914 CrossRef PubMed Google Scholar

[37] Xie C, Lu X, Han L, et al. Biomimetic mineralized hierarchical graphene oxide/chitosan scaffolds with adsorbability for immobilization of nanoparticles for biomedical applications. ACS Appl Mater Interfaces, 2016, 8: 1707-1717 CrossRef Google Scholar

[38] Rizzello L, Pompa PP. Nanosilver-based antibacterial drugs and devices: Mechanisms, methodological drawbacks, and guidelines. Chem Soc Rev, 2014, 43: 1501-1518 CrossRef PubMed Google Scholar

[39] Mirzajani F, Ghassempour A, Aliahmadi A, et al. Antibacterial effect of silver nanoparticles on Staphylococcus aureus. Res MicroBiol, 2011, 162: 542-549 CrossRef PubMed Google Scholar

[40] Li WR, Xie XB, Shi QS, et al. Antibacterial activity and mechanism of silver nanoparticles on Escherichia coli. Appl Microbiol Biotechnol, 2010, 85: 1115-1122 CrossRef PubMed Google Scholar

[41] Le Ouay B, Stellacci F. Antibacterial activity of silver nanoparticles: A surface science insight. Nano Today, 2015, 10: 339-354 CrossRef Google Scholar

  • Figure 1

    (a) Surface modification processes of glass sphere (GS) and (b) anti-biofilm and controlled release properties of PDA-Ag-HF/GS.

  • Figure 2

    The microstructure of GSs. (a–d) are SEM images of GS, HF/GS, Ag-HF/GS and PDA-Ag-HF/GS, respectively. (e) and (f) are Ag element mapping of Ag-HF/GS and PDA-Ag-HF/GS, and (g) is N element mapping of PDA-Ag-HF/GS.

  • Figure 3

    Chemical compositions of the GS surface. (a) XRD spectra of GSs. (b) XPS of GSs. High-resolution O 1s spectra of (c) GSs and (d) HF/GSs. (e) High-resolution Ag 3d spectra of Ag-HF/GSs. (f–h) are the high-resolution C 1s, N 1s, and O 1s spectra of PDA-Ag-HF/GSs, respectively.

  • Figure 4

    (a) Photo images and (b) water contact angle for 5 μL droplet on the surfaces of GS, HF/GS, Ag-HF/GS and PDA-Ag-HF/GS, respectively.

  • Figure 5

    Cumulative release of Ag+.

  • Figure 6

    Adhesion of Chlorella on the surfaces of (a) GS, (b) HF/GS, (c) Ag-HF/GS, and (d) PDA-Ag-HF/GS.

  • Figure 7

    Adhesion of bacteria on the surface of GSs. SEM images of E. coli adhesion on the surfaces of (a) GSs, (b) HF/GSs, (c) Ag-HF/GSs and (d) PDA-Ag-HF/GSs. SEM images of Bacillus adhesion on the surfaces of (e) GSs, (f) HF/GSs, (g) Ag-HF/GSs and (h) PDA-Ag-HF/GSs. (i) and (j) are photographs of different GSs co-cultured with E. coli and Bacillus. (k) and (l) are the antibacterial ratios of different GSs against E. coli and Bacillus.

  • Table 1   Curve fitting results for the O 1s spectra of GSs and HF/GSs

    Function group

    Binding energy (eV)

    GS (%)

    HF/GS (%)










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