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Future perspectives of resin-based dental materials

Klaus D. Jandt a,c, , Bernd W. Sigusch b,c
a b c

Institute of Materials Science and Technology (IMT), Chair in Materials Science, 07743 Jena, Germany Department of Conservative Dentistry, Germany Friedrich-Schiller-University, D-07743 Jena, Germany

a r t i c l e
Article history:

i n f o

a b s t r a c t
Objective. This concise review and outlook paper gives a view of selected potential future developments in the area of resin-based biomaterials with an emphasis on dental composites. Methods. A selection of key publications (1 book, 35 scientic original publications and 1 website source) covering the areas nanotechnology, antimicrobial materials, stimuli respon-

Received 9 February 2009 Accepted 23 February 2009

Keywords: Resin-based dental materials Nanotechnology Antimicrobial Stimuli responsive Self-repair Tissue regeneration

sive materials, self-repairing materials and materials for tissue engineering with direct or indirect relations and/or implications to resin-based dental materials is critically reviewed and discussed. Connections between these elds and their potential for resin-based dental materials are highlighted and put in perspective. Results. The need to improve shrinkage properties and wear resistance is obvious for dental composites, and a vast number of attempts have been made to accomplish these aims. Future resin-based materials may be further improved in this respect if, for example nanotechnology is applied. Dental composites may, however, reach a completely new quality by utilizing new trends from materials science, such as introducing nanostructures, antimicrobial properties, stimuli responsive capabilities, the ability to promote tissue regeneration or repair of dental tissues if the composites were able to repair themselves. Signicance. This paper shows selected potential future developments in the area of resinbased dental materials, gives basic and industrial researchers in dental materials science, and dental practitioners a glance into the potential future of these materials, and should stimulate discussion about needs and future developments in the area. 2009 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.

1.

Introduction

The introduction of resin-based dental materials around the mid of the last century was a revolution in restorative dentistry. Dental composites are esthetically pleasing since they possess tooth like appearance, are stable within the oral environment, are relatively easy to handle and do set on demand via LED or other blue light curing.

Dental composites, however, still have several drawbacks. These include their polymerization shrinkage, potential failure of the resindentin interface leading to secondary caries, a relatively high coefcient of thermal expansion and a relatively low wear resistance compared to metal-based restorations. Leaching of uncured monomers from the composite may lead to cytotoxic effects in the surrounding gum tissues. Much of recent research on resin-based dental

Corresponding author at: Institute of Materials Science and Technology (IMT), Chair in Materials Science, 07743 Jena, Germany. Tel.: +49 3641 94 77 30. E-mail address: K.Jandt@uni-jena.de (K.D. Jandt). 0109-5641/$ see front matter 2009 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.dental.2009.02.009

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materials focused on these challenges and signicant progress was made, although the basic principles of composition and effects of dental composites remained unchanged during the last decades. Beyond the recent improvements of dental composites, it is well worth to have a look at the potential future of this class of materials. The author of this article is no clairvoyant and can therefore not know for sure what the future holds for resin-based dental materials. There are, however, a number of interesting developments and strong trends in the broader eld of materials science and biomaterials, which may inspire future developments of dental composites to some extent. These developments include nanotechnology and nanostructuring, materials that actively ght microbes, stimuli responsive materials, materials that promote tissue regeneration or self-repairing materials. In this article, some of these future perspectives are surveyed with respect to a potential use in resin-based dental materials. Some principles of these new approaches are explained and the potential of application for resin-based dental materials is discussed concisely.

2.

Nanotechnology

Nanotechnology is an applied science, which deals with the control of structure and properties on an atomic or molecular scale. It is, however, generally accepted that nanomaterials are 100 nm (1 107 m) or smaller in size. A human hair has a diameter of approximately 50 m, i.e. it has a diameter, which is 50,000 times larger than 1 nm. The denition given above means also, that a roughly cubic iron particle of a side length of 100 nm contains approximately 80 million (8 107 ) atoms. This means that nanotechnology often deals with a relative small number of atoms or molecules. On the other hand, nanomaterials have been dened as materials with morphological features smaller than a micrometer in at least one dimension [1]. What makes nanomaterials work is their extremely large surface free energy. For an iron cube of 100 nm edge length, approximately 10% of the atoms are surface atoms and the part of surface atoms increases to 100%, if the cube has an edge length on 1 nm. Since the bonds at the surface of these nanoparticles are not saturated, these particles possess a large surface free energy, which leads to a drastic change of the physical and chemical properties compared to the bulk of condensed matter. Legend has it that this effect inspired Wolfgang Pauli, the discoverer of Paulis exclusion principle that to state God created the bulk of condensed matter but the devil created the matters surface. Because of the huge surface free energy, nanoparticles bond strongly to other materials or to each other (agglomeration). These effects may be exploited in bulk applications of nanoparticles, such as in composites with enhanced physical properties, for example in resin-based dental composites. On the other hand, the production of such composites goes hand in hand with technological challenges due to the nanoparticle agglomeration. Functionalization of the nanoparticles may introduce a surface charge to the nanoparticles, which reduces agglomeration since similar charges repel each other. A sec-

ond strategy to break up nanoparticles before introduction into a resin is to use a so-called pearl mill. In a pearl mill, small ceramic or metal particles crash with the suspended agglomerates of nanoparticles and break the former up. In addition, nanoparticles tend to be difcult to wet with bifunctional primers, which is necessary to bond them to the resin matrix in dental composites. The use of nanoparticles in dental composites is not new. Colloidal silica particles of a diameter of approximately 40 nm have been in use in dental microlled and hybrid composites for more than 10 years. Nanoparticle lled composites exhibit outstanding esthetics, are easy to polish and posses an enhanced wear resistance. Nanoparticle llers may include colloidal silica or Ormocers, such as in Ceram X from Dentsply. Similar particles may be used in resin-based bonding systems. Nanoparticle lled dental composites may show an enhanced fracture toughness [2] and adhesion to tooth tissue [3]. In some cases the wear and fatigue properties of composites containing nanoparticles were similar or worse than a microlled composite [4]. Other studies report that dental nanocomposites showed a high translucency, high polish and polish retention similar to those of microlled composites while maintaining physical properties and wear resistance equivalent to those of several hybrid composites [5]. It was further concluded, that the strength and esthetic properties of the resin-based nanocomposites tested should allow the clinician to use them for both anterior and posterior restorations. The exural strength of resin-based dental composites can be improved if single-walled carbon nanotubes (SWCNT) are added as llers [6]. These true nanollers, however, may negatively inuence the esthetics of dental composites since SWCNT are of a blackish color. Another study found that composites containing TiO2 nanoparticles treated with the organosilane allyltriethoxysilane improve the microhardness and exural strength of resin-based dental composites [7]. Improvements of mechanical properties of resin-based dental cements lled with nanosized Al2 O3 have been reported furthermore [8]. Overall, it seems that the majority of studies about resinbased dental materials lled with different nanollers report improvements in some properties compared to composites without nanoller. A clear comparison of performance, however, is challenging since often, more than one parameter was varied in the studies or only one or two physical properties were measured. An overall superiority of nanolled composite can, therefore, hardly be claimed in general. A second serious problem is the unknown risks connected with nanoparticles. In composites, the nanoparticles are rmly bound and embedded and should therefore pose no threat to human health. As the composites wear over the years, nanoparticles are released from the composite. In the light of an intense public debate about dental amalgam in the last two decades, the potential health risk [9] of nanolled resin-based dental materials needs to be explored and assessed in more detail.

3.

Antimicrobial materials

Antimicrobial materials ght bacteria and delay, reduce or avoid the formation of biolms on the materials. There are dif-

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ferent strategies to accomplish this. Generally, antimicrobial properties of (bio) materials may be accomplished by introducing agents such as sliver [10] or one or more antibiotics [11] into the material. Microbes are subsequently killed on contact with the materials or through leaching of the antimicrobial agents into the body environment. There are several examples of antimicrobial biomaterials used as implants [12] or in pure research [13] and the number of studies, addressing antimicrobial biomaterials outside the eld of dental materials has recently increased rapidly. In the oral cavity, important examples of microbes present are acid producing bacteria, such as Streptococcus mutans or anaerobic bacteria. A common problem with composites is the failure of the resin dentin interface, although new and improved bonding systems have helped to reduce the problem. If the interface fails, bacteria as mentioned above are able to penetrate the gap, which may result in secondary caries. Therefore, a need exists to have dental composites with antimicrobial properties. Several attempts have been made to produce antimicrobial resin-based dental composites. Silver and titanium particles were introduced into dental composites, respectively, to introduce antimicrobial properties and enhance biocompatibility of the composites [14]. In another study two types of silver-supported antibacterial materials, Novaron (N-5) and Amenitop (AM) were incorporated into dental composites [15]. These composites inhibited the growth of Streptococcus mutans during and after 6 months. This indicated a relatively long lasting antimicrobial effect of these composites. No or extremely little release of silver ions was observed for the composites. Compressive strength and exural strength were not negatively affected by N-5 after storage in water, whereas there was a signicant difference in both mechanical parameters for the AM containing composites. Dental composites containing 1% (w/w) quaternary ammonium polyethylenimine (PEI) nanoparticles were tested for their antimicrobial activity [16]. The antibacterial properties of these composites were based on contact mechanism rather than on leaching. The mechanical properties of the composites were not signicantly affected by introducing the PEI nanoparticles. The antimicrobial effect lasted for at least 1 month. Alkylated ammonium chloride derivatives have been introduced to dental composites and an enhancement of the antimicrobial properties was reported for these composites [17]. Nevertheless, it was also found in the same study that alkylated ammonium chloride derivatives with a greater chain length between the ammonium and the acryl (or methacryl) functional groups reduced some of the mechanical properties of the composites. Chlorhexidine diacetate (CHXA) was introduced as antimicrobial agent into dental composites [18]. When raising the hydroxyethylmethacrylate (HEMA) content of these composites, the light cure polymerization rates decreased. On the other hand, water sorption induced swelling and rates of diffusion controlled CHXA release from the set materials increased. These composites showed a delay in biolm formation compared to conventional composites but some compositions showed polymer leakage.

Since microbe induced problems are important in connection with dental composites, it is surprising how few current dental composites actually possess proven antimicrobial properties. The antimicrobial properties of its corrosion products and the silver content of dental amalgam are almost legendary [19] and that leaves much to be accomplished in this respect for dental composites. There are sometimes problems with introducing antimicrobial agents into composites, such as decrease of the antimicrobial properties with time or reduced ability of the composites to light cure. Nevertheless, antimicrobial composites would help to solve or alleviate some of the major clinical problems connected to these resinbased restorative materials. One can, therefore, expect that future composites will address this issue and will possess some antimicrobial properties and that this will be an issue of intensive research.

4.

Stimuli responsive materials

Stimuli responsive materials, also called smart materials, possess properties that may be considerably changed in a controlled fashion by external stimuli. Such stimuli may be for example changes of temperature, mechanical stress, pH, moisture, or electric or magnetic elds. There is a strong trend in materials science [20,21] and biomaterials [22,23] science to develop and apply these intelligent materials. Developing stimuli responsive materials is often inspired by nature where living systems use macromolecules, such as proteins, polysaccharides and nucleic acids, both to build structural materials or as major components in cell regulation and function [24]. These systems show a strong non-linear behavior and signicantly change structure and properties at a certain point of external stimuli, such as a critical temperature. The material behavior is often based on a drastic change of the conformation of the macromolecules involved. It is, therefore, no surprise that many of the reports about stimuli responsive synthetic materials address polymeric materials as well. For example, stimuli responsive porous poly(N-isopropylacrylamide) hydrogels with superfast shrinkage kinetics as a function of temperature have been created recently for drug or protein release [24]. The process of photopolymerization by blue light may be considered a stimuli response of the dental composite. Since this well-known process only takes place once at the beginning of a duty cycle of a dental composite, it will not be further considered here. Other than that, resin-based dental materials such as dental composites are per se not stimuli responsive and a literature search with the respective keywords results in no hits. On the other hand, stimuli responsive dental composites may be quite useful for example for release-oncommand of antimicrobial compounds (see above) or uoride to ght microbes or secondary caries, respectively. In addition, self-repair mechanisms of composites (see below) may be triggered some day by external processes, which damage the composites. These properties would potentially allow new and groundbreaking dental therapies and a signicantly enhanced clinical outcome of treatments with smart dental composites. It is clear that such smart dental composites would require much more sophisticated materials than currently used in

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dental composites but it seems that these efforts promise great rewards. As mentioned above, many stimuli responsive (non-dental) materials are based on polymers. Normally the macromolecules in these systems possess degrees of freedom, which allow them to change their conformation to some degree. The high degree of chemical crosslinking in current dental composites does not allow for these degrees of freedom, which means the resin composition would have to be changed profoundly to accomplish smart properties.

The self-repairing mechanism based on microcapsules may be more promising, and composites repaired in that way may perform better than those repaired with macroscopic repair approaches, some of which [29] have been shown not to lead to satisfactory mechanical properties of the repaired composite.

6. Materials for bone and dental hard tissue regeneration

Materials for tissue regeneration allow the partial or complete regeneration of tissues in the human body. Examples for this are bone replacement materials, which are used after part of the bone was destroyed by accident, necrosis or inammatory processes. So far, bone replacement materials based on ceramics, such as bioactive glass have been used. These materials, however, allow only partial tissue regeneration, if any. Recently, polymerceramic biomimetic composite bone replacement materials have been developed which are biodegradable [30,31] and may have much potential to be remodeled by the body, thus allowing more or less complete tissue regeneration. The main purpose of resin-based restorative materials, such as composites, is to replace lost tooth structure and function with an esthetically pleasing result. These conventional composites, however, have little in common with natural tooth structure and do not support any kind of tissue regeneration. Nevertheless, natural dental tissues possess much better properties and more suitable structures to full their tasks, than the best restorative composite. It is, therefore, interesting to incorporate tissue regenerative properties in dental composites. Dental tissues of the oral cavity, which exhibit a need to be regenerated, are dental enamel and dentin. For dentin regeneration, modied polymerceramic biomimetic composites may have a potential, but further tests are required to judge the potential of this new material fully. During the last few years, a number of interesting attempts have been reported to create synthetic dental enamel [32] or repair dental enamel. Lippert et al. demonstrated that a hydroxyapatite layer can be deposited from solution in vitro onto enamel [33]. Other studies have shown that crystalline uoroapatite with a structure very similar to human dental enamel may be created articially [34]. This is accomplished, however, under conditions far from those present in the oral cavity, at temperatures between 200 C and 600 C. The same research group synthesized uorapatite nanorods of different size, shape, and composition for incorporation in dental materials or in the treatment and prevention of caries [35]. An enamel-inspired nanocomposite fabricated through amelogenin supramolcular assembly for incorporation into dental materials has been developed recently [36]. Many of the articially created hydroxyapatites have not been extremely effective in enamel repair and remineralization [37]. Recently, Tang and co-workers found a potential explanation for this [37]. In their work, they used much smaller (20 nm) hydroxyapatite particles, which correspond in size much better to natural hydroxyapatite, found in dental

5.

Self-repairing materials

Materials have usually a limited lifetime and degrade due to different physical, chemical and/or biological stimuli. These may include external static (creep) or dynamic (fatigue) forces, internal stress states, corrosion, dissolution, erosion or biodegradation. This generally leads to a decay of the materials structure and, hence the materials properties degrade. As a result, the material fails at some stage of these processes, for example, it fractures. Examples for this are the failure of the resindentin interface [25] or the fracture of the dental composite. The latter is caused often by the breakdown of the resin matrix and/or the interface between the ller and the resin matrix [26]. It appears that the clinical failure in the rst 5 years is a restoration issue (technique or material selection); after that time period, failure most often results from secondary decay [26]. In addition, wear of dental composites is a major issue. While dental and engineering materials generally fail after some time of use, nature manages to renew many of the biological materials it utilizes. An example for this is natural bone which is permanently remodeled and which can self-repair (heal) even after a major fracture has occurred. These principles inspired materials scientists and engineers worldwide to develop synthetic so-called self-healing or self-repairing materials. One of the rst self-repairing synthetic materials reported, interestingly shows some similarities to resin-based dental materials, since it is resin-based. This was an epoxy system [27] which contained resin lled microcapsules. If a crack occurs in the epoxy composite material, some of the microcapsules are destroyed near the creak and release the resin. The resin subsequently lls the crack and reacts with a Grubbs catalyst dispersed in the epoxy composite, resulting in a polymerization of the resin and a repair of the crack. Similar systems were demonstrated to have a signicantly longer duty cycle under mechanical stress in situ compared to similar systems with the self-repair [28]. It is self-evident how attractive such an approach is for application in dental composites. It can be expected that dental composites using this technology would have a significantly longer duty cycle and enhanced clinical performance. Problems may arise from the potential toxicity of the resins in the microcapsules and from the catalyst, which needs to be present in the composite. The amounts of these agents necessary to repair microcracks in the dental composite, however, seem to be rather small, and may well be below the toxicity threshold.

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enamel. These studies show much promise, especially if one thinks to combine this approach with a resin-based restorative dental material. In the future, it will be especially important to demonstrate the enamel repair potential in vivo and that the repaired enamel is mechanically stable.

7.

Summary

There is much room for the improvement and further development of resin-based dental materials, such as composites. A new quality of dental composites may, however, be created if nanotechnology is used and other new developments in material science and biomaterials are considered in composites in the future. These developments include antimicrobial properties, introducing stimuli responsive or self-repairing materials and materials for dental hard tissue regeneration. These approaches require much more complex dental composites and sophisticated technologies than currently used. The benet for the patient and the quality of the dental therapy, if such new materials are developed and introduced, however, are self-evident.

Acknowledgments
This paper was presented at the 2008 Annual Academy of Dental Materials Meeting in Wrzburg, Germany. K.D.J. is grateful to Karin Jandt for proofreading this manuscript.

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