A brief review of recent developments in the designs that prevent bio-fouling on silicon and silicon-based materials
© The Author(s) 2017
Received: 9 July 2016
Accepted: 14 February 2017
Published: 20 February 2017
KeywordsSilicon Silicon-based materials Antifouling Surface modification Biomimetic
Silicon and silicon-based materials are integral parts of our daily life. Silicon has widespread applications in healthcare and manufacturing due to its unique material properties, including high flexibility, low biological activity, ease of fabrication, and chemical and thermal stability [1–4]. In addition, silicone based materials, such as silicone elastomer, is also the basic constituent of tubing, microfluidic system, catheters, drains, shunts, joint implants, silastic mammary prostheses, and contact lenses . Silicon-based materials, such as SixN4, have excellent fracture toughness and are chemically inert. Therefore, silicon is often used as an insulator and chemical barrier in manufacturing integrated circuits .
Unfortunately, silicon and silicon-based materials are susceptible to bio-fouling, which is the tendency of microbes, cells, and bacteria to physically adsorb to surfaces. This leads to deterioration of surface engineering in addition to infectious contamination , which are significant concerned . For example, in the USA, about 40% of all bacterial infections occurring in hospitals are found to be catheter-associated urinary tract infection (CAUTI), which considerably increases the healthcare costs, the length of stay in the hospital and the antibiotic use [9–11].
Bio-fouling can also result in the growth of marine organisms on ship hulls, which is a major expense factor in naval industries. Based on the World Shipping Council’s report, fuel can represent as much as 50% of a ship’s total operating costs. Because the fouling causes a drag force on the ship and subsequent decreased fuel efficiency, hull fouling can increase fuel consumption, cost, and carbon dioxide emissions by as much as 40% . In addition, the metabolic activity of the attached organisms can cause localized corrosion . In one solution to this problem, polydimethylsiloxane (PDMS), a low energy silicone material, was used as a nontoxic alternative to conventional biocide paints.
Significant efforts have been dedicated to modifying silicon and silicon-based materials to improve their anti-fouling performance. The objective was to change the properties of the materials or the immobilized molecules in ways that either limit foulant accumulation, or provide ways to remove attached foulants after adsorption saturation, such that the fouled materials can be regenerated. However, reviews of surface modification of silicon and silicon-based materials for their antifouling and antibacterial properties are lacking. Therefore, in this article, an overview of the recent work in silicon and silicon-based materials modification for antifouling purposes will be presented. We are interested in silicon-based materials such as silicone elastomer because they are appropriate to be used for medical applications.
Functionalization of silicon and silicon-based substrates with antifouling molecules
Poly (ethylene glycol) and its derivatives
As the most commonly-used materials for fouling resistance, poly (ethylene glycol) (PEG) and its derivatives are widely used to engineer the surface of silicon [15–17]. Their modification enables silicon to be hydrophilic, nontoxic, and biocompatible. The hydration layer surrounding the ethylene oxide chain is the reason PEG has demonstrated the ability to repel fouling materials . However, the ethylene oxide chains are, over time, auto-oxidized in aqueous solutions, resulting in cleavage of ethylene oxide units and formation of aldehyde-terminated chains. Therefore, there are limits to its long-term application (more than 14 days). In addition, the formed aldehyde moieties may react with fouling materials, such as protein, resulting in a declination of the repellent nature of the PEG coatings . Furthermore, PEG loses its protein resistance at 37 °C and above, while 37 °C is a critical temperature for many biomedical applications. It is known that repulsive ethylene oxide (EO)-protein interactions are essential to the anti-fouling efficiency of PEG. Higher temperatures (37 °C and above) can cause EO monomers to alternate their configurations and affect EO-protein interactions, resulting in more protein adsorption on the surface .
In a report published in Langmuir , the copolymer, poly(TMSMA-r-PEGMA), which is comprised of an “anchor part” (trimethoxysilane) and a “function part” (PEG), was synthesized by a radical polymerization reaction. Then polymeric self-assembled monolayers (PSAMS) of poly(TMSMA-PEGMA) on Si/SiO2 or glass substrates were prepared by immersing the substrate in a methanol solution of poly(TMSMA-PEGMA) at ambient temperature. Then the polymer-coated Si/SiO2 or glass substrates were immersed in insulin, lysozyme, and fibrinogen solution to evaluate their protein resistance characteristics. The results demonstrated that the polymer-coated Si/SiO2 or glass substrates have a great reduction in nonspecific protein adsorption compared to the unmodified substrates.
In another study, Voo and co-workers coated thiol-functionalized silicone rubber, which is a commonly used catheter material, with modified PEG molecules through a Michael addition reaction. The antibacterial and antifouling properties of the polymer-modified surface against both Gram-positive Staphylococcus aureus, which is methicillin-resistant and a major cause of the infection, and Gram-negative Escherichia coli were examined. Their results shown that the coating can prevent S. aureus and E. coli biofilm formation over 14 days incubation. Comparing to a high number of S. aureus and E. coli adhered onto the pristine surface after one day incubation, this coating demonstrates potential for use as antifouling coating to prevent catheter-associated infections .
Yang’s team created PEG nonfouling anti-microbiao hydrogels, which can be applied onto catheters or other implants as a coating to prevent infections. This PEG hydrogel was fabricated via Michael addition chemistry that incorporated an antimicrobial cationic block copolymer of PEG and polycarbonate. The antimicrobial mechanism of the cationic hydrogels is proposed that the anionic cell wall/membrane of bacteria was first attracted and interacted with the cationic hydrogel surface at many fixed points via electrostatic interaction, followed by the insertion of the hydrophobic segments of hydrogel into the hydrophobic regions of the lipid membrane, inducing the leakage of the membrane and eventually resulted in cell lysis. These hydrogels were then grafted onto silicone rubber, a material used to manufacture catheters. The antimicrobial activity of hydrogel-coated rubber was investigated by exposing itself to S. aureus for 1 day. There were numerous viable S. aureus cells found on the rubber surface without coating, but no cells on the gel coated rubber surface were detected by confocal. No adverse effect of the gel was observed on the toxicity, skin sensitization and skin irritation .
Stimuli-responsive, or “smart” polymers, have the extraordinary ability to change their physical and chemical state after they “detect” a change in their environments; their responses depend dramatically on their chemical composition . In addition, due to the ease of modification with specific chemical functionalities, stimuli-responsive polymers have attracted additional attention for use as antifouling coatings [43–46]. Some researchers have used the properties of stimuli-responsive conformational changes to develop antifouling coating materials with self-cleaning properties [47, 48]. Compared to traditional antifouling surfaces, which are often associated with the accumulation of dead bacteria and other debris that degrade biocidal activity and provide nutrients for other colonizers , the stimuli-responsive polymer-modified surface is desirable for foulants to be removed or released to maintain long-term anti-fouling properties.
We found that few research papers have reported on the use of stimuli-responsive polymers modified silicon and silicon-based materials for marine applications. Therefore, more research in this area is expected in the near future. An intrinsic difficulty of these stimuli-responsive polymers-coatings is the trade-off between the ability to switch and the mechanical stability of the system. At low crosslink densities, the switching process works well, but the coatings are quite fragile. At high crosslink densities, the coatings are more robust, but switching becomes increasingly difficult .
Incorporation of biocidal agents, such as synthetic biocides and enzymatic biocides, on surfaces is an effective approach to kill or degrade attached bacteria, and therefore inhibit their proliferation and formation of biofilms. For example, quaternary ammonium salt (QAS), one type of synthetic biocide, can provide effective protection against bacterial colonization by disrupting the cell membrane through the binding of their ammonium cations to anionic sites in the outer layer tissue of bacteria . It was reported that the QAS-modified substrate can resist the bacterial adhesion with water-repelling hydrophobicity and eradicate the contacted bacteria with biocidal capability .
Zwitterionic polymers are polymers that have moieties possessing both cationic and anionic groups. These materials are characterized by high dipole moments and highly charged groups but are charge neutral . The strongly bound hydration layer, induced by electrostatically ionic solvation in addition to hydrogen-bonding interactions, is considered to be the reason for the efficient repulsion of fouling materials—the electrostatic interactions between water molecules and dipoles present in the zwitterionic polymer chains make these polymers better “water-bears” [18, 64, 65]. For example, Huang’s group recently modified the silicon-based materials, PDMS, with sulfobetaine silane (SBSi) with covalent silanization. This superhydrophilic zwitterionic interface presents its antibacterial adhesion property to resist nonspecific adsorption of bacteria (S. epidermidis and P. aeruginosa), protein (bovine serum albumin, lysozyme, and mucin), and lipids. Moreover, because the cellular liability experiment demonstrated that SBSi had negligible cytotoxicity in vivo application, the applicability of SBSi modification was applied to silicone hydrogel contact lenses by following the same procedure as that for PDMS. The SBSi-modified contact lens was kept under the P. aeruginosa solution in a physiological condition. The experimental results demonstrated that the number of adherent bacteria on SBSi-modified contact lens is much less than unmodified one .
Most zwitterionic polymers with antifouling functionality are attached to the surface through Si–O–Si–C [66–68] and Si–O–C linkages [69, 70]. A major disadvantage of these approaches is the limited hydrolytic stability. This may result in the detachment of the zwitterionic polymers and may consequently keep long-term application out of reach. To increase the stability of the attachment, researchers from Netherlands deposited the Si substrates with SixN4 (x > 3) by low-pressure chemical vapor deposition (LPCVD) with a thickness of 150 nm first. The sulfobetaine methacrylate (SBMA) zwitterionic polymer brushes were then grafted from SixN4 surfaces by controlled surface-initiated atom-transfer radical polymerization (ATRP) through more stable Si–C linkage as compared to less stable Si–O–Si–C and Si–O–C linkages. As a result, the long-term protein-repellent properties of the zwitterionic polymer (polySBMA) remain largely unaffected .
Fabrication of surfaces with nano- or micro- topographical features
It is well-known that the surface microstructure influences cell behavior or tissue formation , and certain topography features may contribute to a fouling-free surface. In Carman’s study, the designated surface microstructures, including ridges and channels, were induced on a silicone elastomer based cross-linked PDMS films by adopting microfabrication techniques. Their results demonstrated that the settlement of Ulva linza zoospores related to the ridge topographies, and is inversely proportional to the width (between 5 and 20 μm) of the channels .
Because the special surface topography of skin or shells includes micro- and nanostructure, many marine organisms do not have biofouling [78, 79]; therefore, artificial surfaces with biomimicking natural microtextures have been fabricated and studied. In a recent work, researchers designed PDMS hierarchical surface microtopographies that mimic the critical features observed on the M. hardwickii surface. This micropatterned surface was subject to fouling tests, including laboratory assays against algae adhesion and was also exposed to marine environments during field testing. Their results demonstrated that the settlement of organism on the patterned PDMS was lower than that on the smooth PDMS, indicating that the designed micrographic surface features associate with antifouling. The micropatterned PDMS samples were further modified with zwitterionic polymer brushes, and it was reported that the use of microtopography enhances the antifouling performance of zwitterionic polymer brushes to a greater extent .
Another pioneering report of biomimicry focused on the surface of the Trifolium leaf, which has a self-cleaning property. In this work, silicone elastomer was used to fabricate biomimetic surfaces using the Trifolium leaf as a template. The surface of the replica displays a remarkable amount of microspines with a size similar to that of the original Trifolium leaf, and is effective in resisting the settlement of microalgae. The antifouling property of the replica was improved by modification with poly(3-sulfopropyl methacrylate) (PSPMA), a kind of hydrophilic acrylate polymers .
Conclusion and perspectives
We have reviewed strategies for designing effective antifouling approaches for silicon and silicon-based materials, although several of them have associated shortcomings. In addition, by providing a surface topography that is unfavorable for biofoulant attachment, it can also repel the attached biofoulant from the silicon and silicon-based material surface. Although many works claim their antifouling coatings or surface modifications have long-term stability, it is our understanding that an antifouling coating doesn’t last forever; as it becomes aged, it becomes less effective. It also has been brought to our attention that once the deposition of foulants has taken place, the surface modification is no longer effective at preventing fouling, which is understandable in light of the fact that the effect of solute/coating interaction is severely reduced once a layer of deposited foulants is formed . In other words, the development of an absolutely nonfouling surface is extremely difficult. The old antifouling coating needs to be removed, and a new antifouling coating needs to be applied once the fouling layer is formed. One of the approaches to remove antifouling paint is by scraping, which is a time consuming process. In addition, one might damage the surface during this coating removal process. We must therefore explore methods by which to restore the permanently fouled surface and maximize the effective use of the modified materials. We expect that these methods can be described in near future and become solutions to reduce the cost associated with fouling for industry, and can prevent long-term bio-fouling for those biomedical devices which are fouled over quickly, such as the colonization of bacteria on catheters, contact lenses, and surgical tools, so that the healthcare costs can be decreased. Besides, we expect more studies testing the cost-effectiveness, durability, and stability of those designs in real situations, such as the prevention of marine fouling and fouling on medical implants/devices. However, in those cases, the challenge would be developing a coating or an approach of modification that will resist adhesion of all forms of biofouling.
Catheter-associated urinary tract infection
poly (ethylene glycol)
ethylene oxide (EO)
human serum albumin (HSA)
bovine serum albumin
quaternary ammonium salt
Atomic Force Microscopy
low-pressure chemical vapor deposition
Scanning Electron Microscopy
All authors carried out the literature research and the writing of the manuscript. All authors read and approved the manuscript.
The authors gratefully acknowledge the financial support from the National Science Foundation (HRD-1505197). H. H. is grateful for support from the Science and Technology Project of Zhejiang Province (2017F50021) and the Science and Technology Project of Zhoushan City (2016C31055).
The authors declare that they have no competing interests.
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