MICROSCOPY RESEARCH AND TECHNIQUE 74:2327 (2011)

Nanohybrid Versus Nanoll Composite in Class I Cavities: Margin Analysis After 12 Months
NGELA MARQUES DUARTE,1 ANA KARINA MACIEL DE ANDRADE,1* ROSA RIO ANDRADE PASSOS,3 KENIO COSTA LIMA,4 SEVERINO JACKSON GUEDES LIMA,2 TIBE NIO JAPIASSU RESENDE MONTES5 AND MARCOS ANTO
1 2 3

baUFPB, Brazil Department of Restorative Dentistry, Federal University of Para baUFPB, Brazil Department of Mechanical Technology, Federal University of Para baUFPB, Brazil Department of Engineering Materials, Federal University of Para 4 Department of Dentistry, Federal University of Rio Grande do NorteUFRN, Brazil 5 Department of Restorative Dentistry, University of PernambucoUPE, Brazil

KEY WORDS

nanotechnology; nanoparticle; scanning electron microscopy

ABSTRACT This study evaluates the margin of a nanoll, a nanohybrid, and a conventional microhybrid composite in restorations in occlusal cavities of posterior teeth after 12 months. Fortyone patients, each with three molars affected by primary caries or the need to replace restorations, participated in this research. The teeth were restored with a nanoll (Filtek Z350), a nanohybrid (Esthet-X), and a microhybrid as a control (Filtek Z250). Ten patients were selected randomly, and the three restorations were molded with a low-viscosity polyvinyl siloxane material. The molds were poured with epoxy resin, gold-sputter coated, observed by scanning electron microscopy, and classied as: perfect margin, marginal irregularity, marginal gap, marginal fracture, or artifact. For statistical analysis, the Wilcoxon and Friedman nonparametric tests and pairedsamples t-test were used (signicance level of 5%). The performance of the three materials was compared after 1 week and 12 months. No statistically signicant differences were detected for all criteria (P > 0.05). When each composite was compared over time, statistically signicant differences were found for the criterion, perfect margins (Esthet-X and Filtek Z350, P < 0.05). The materials performed satisfactorily over the 12-month-observation period, but all composites under investigation showed a certain amount of deterioration relating to marginal quality over time. Microsc. Res. Tech. 74:2327, 2011. V 2010 Wiley-Liss, Inc.
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INTRODUCTION Anterior and posterior restorations are predomi mer nantly carried out using resin composites (Kra et al., 2009; Manhart et al., 1991), but a primary concern of composite restorations is the shrinkage that follows polymerization. This shrinkage can create forces that may disrupt the bond to the cavity walls and form marginal gaps, leaving the tooth more susceptible to postoperative sensitivity and recurrent caries. To restore a tooth in such a way that it is leak proof, there must be no dimensional mismatch at the tooth-restoration interface. Resin composites do not meet these requirements (Davidson and Feilzer, 1997). However, many changes have taken place in adhesive systems and restorative materials. One signicant change was the introduction of the rst restorative nanocomposite resin for dentistry. Nanotechnology, also known as molecular nanotechnology or molecular engineering, is the production of functional materials and structures in the range of 0.1100 nm (the nanoscale) by various physical or chemical methods (Kirk et al., 1991). Nanocomposites contain a unique combination of two types of nanollers (575 nm) and nanoclusters. Nanoparticles are discrete nonagglomerated and nonaggregated particles, 2075 nm in size. Nanocluster llers are loosely bound agglomerates of nanosized particles. The agglomerates act as a single unit enabling high-ller loading and high strength. As a
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result of the reduced dimension of the particles and wide-size distribution, increased ller load can be achieved with the consequence of reducing polymerization shrinkage and increasing the mechanical properties such as tensile strength, compressive strength to fracture. These properties of nanocomposites seem to be equivalent or sometimes even higher than hybrid composites and signicantly higher than microlled composites. As a consequence, manufacturers now recommend the use of nanocomposites for both anterior and posterior restorations (Beun et al., 2007; Condon and Ferracane, 2002; Mitra et al., 2003; Yap et al., 2004). In addition, there are composites on the market that combine nanoparticles with other micrometric particles, and these provide better performance. These materials are considered the precursors of nanoparticle composites and are sometimes referred to as nanohybrids (Beun et al., 2007). A prospective clinical trial remains the ultimate instrument to clarify the doubts that exist about the use of nanocomposites. Nevertheless, preclinical in
*Correspondence to: Ana Karina Maciel de Andrade, Universidade Federal da baUFPB, Departamento de Odontologia Restauradora, Cidade UniversiPara ria, Joa o PessoaPB, Brazil 58059-900. E-mail: kamandrade@hotmail.com ta Received 9 February 2009; accepted in revised form 12 March 2010 DOI 10.1002/jemt.20867 Published online 27 April 2010 in Wiley Online Library (wileyonlinelibrary.com).

2010 WILEY-LISS, INC.

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Brand name Filtek Filtek
TM TM

A.K.M. ANDRADE ET AL.

TABLE 1. The commercial brand name, composition, and manufacturer of the materials used in the study Composition Organic matrix: bis-GMA, UDMA, bis-EMA 6. Inorganic particle: zirconium/silica with 85% by weight (60% by volume). Size of particles: 0.013.5 lm (mean 0.6 lm) Organic matrix: bis-GMA, UDMA, bis-EMA 6, and small quantities of TEGDMA. Inorganic particle: nonagglomerated 20-nm nanoparticles of silica and nanoagglomerates formed of zirconium /silica particles ranging from 0.6 to 1.4 lm in size. 78.5% by weight (59.5% by volume) Organic matrix: bis-GMA urethane modied, bis-EMA, and TEGDMA. Inorganic particle: vitreous particles of aluminum borosilicate uoride and silanized barium, with mean size of less than 1 lm, colloidal silica 0.04 lm in size and nanometric silica. 77% by weight (60% by volume) Manufacturer 3M ESPE, St. Paul, MN, USA 3M ESPE, St. Paul, MN, USA

Z250 Z350

Esthet-X

Dentsply/Caulk, Milford, DE, USA

Bis-EMA 6, bisphenol A-polyethylene glycol diether dimethacrylate; bis-GMA, bisphenol A-diglycidyl ether dimethacrylate; TEGDMA, triethylene glycol dimethacrylate; UDMA, urethane dimethacrylate.

vitro investigations are still useful, especially when experimental questions or potential for optimizing proce mer et al., dures arise (Frankenberger et al., 2007; Kra 2009). SEM for micromorphologic evaluation of posterior composite restorations through replica epoxy resin was used as a research tool many years ago and is an effective tool used in several studies in the literature mer et al., 2009; Roulet (Gaengler et al., 2004; Kra et al., 1991). The opportunity to evaluate in vivo the marginal quality of the restorations through scanning electronic microscopy justies the conduction of this research. This study evaluates the margin of a nanoll, a nanohybrid, and as a control, a conventional microhybrid composite, in restorations in occlusal cavities of posterior teeth after 12 months. The null hypotheses to be tested are: (1) there is no difference in the marginal integrity among the three composites after 12 months and (2) there is no difference in the marginal integrity of each of the composites over time. MATERIALS AND METHODS This research was approved by the Research Ethics Committee of the Health Science Center of the Federal ba (Brazil). The volunteers and University of Para their guardians were consulted to obtain authorization for their participation in the research and for the researchers to use the results. All the volunteers signed a Term of Free and Informed Consent form and received complete dental treatment at the Integration ba. Clinic of the Federal University of Para This study represents a clinical, controlled, and randomized trial. The patients were selected from among students of either gender at public schools in ba (Brazil). The inclusion cri o PessoaPara city of Joa teria were as follows: presence of three molars requiring replacement of class I restorations or with primary caries on the occlusal surface; occlusal contact with the antagonist tooth; patient in good state of general health (Hickel et al., 2007; Spreaco et al., 2005). The following were excluded from the study: patients with intense bruxism; molars with a carious lesion on a surface other than the occlusal surface and in continuity with the occlusal cavity; pulp exposure during caries removal or cavities with imminent risk of pulp exposure; spontaneous pain or sensitivity to percussion. The sample involved in this research consisted of 123 permanent molars of 41 volunteers, who were divided into three groups. To ensure randomness, a draw was

held using sealed envelopes to establish the group for each tooth:  Group I: restorative composite Filtek Z250 (3M ESPE, Saint Paul, MN), as the control;  Group II: restorative composite Filtek Z350 (3M ESPE);  Group III: restorative composite Esthet-X (Dentsply/ Caulk, Milford, DE). The composition of the restorative materials used is shown in Table 1.

Preparation Initially, the occlusal contacts were recorded with Accu Film II articular paper (Parkell, Farmingdale, NY). The cavities were prepared, with absolute isolation of the operating eld, using 245 carbide burs (SS White, Rio de Janeiro, Rio de Janeiro, Brazil) at high speed, with intermittent movements; only carious tissue was removed. Any remaining caries was removed with a spherical bur at low speed. In the cases of unsatisfactory restorations, these and any remaining carious tissue were removed. Adper single bond two adhesive (3M ESPE, Saint Paul, MN) was used in accordance with the manufacturers instructions. The composite was inserted by the incremental technique with a maximum of 2 mm in each layer. Conventional photoactivation was carried out with LED light Optilight LD Max (Gnatus, o Preto, Sa o Paulo, Brazil) and irradiance of Ribeira 600 mW/cm2 gauged by a radiometer from the same company. The enamel colors were photoactivated for 20 s, each increment, but for the darker and more opaque colors, photoactivation was complemented with a further 1020-s exposure, depending on the manufacturers recommendations. Occlusion was adjusted with articular paper and a o Paulo, Sa o 12-bladed bur (FG7714F; KG Sorensen, Sa Paulo, Brazil) at high speed, and in a follow-up session, nal nishing and initial polishing was performed using the kit of abrasive rubbers (Flexicups and Flexipoints; Cosmedent, Chicago, IL) at low speed with intermittent movements. Final polishing was done with Enamelize paste (Cosmedent) and a diamond felt disk (FGM, Joinville, Santa Catarina, Brazil) also at low speed. All the procedures were performed by the same operator, and all the patients received individual oral
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Fig. 1. The replica in epoxy resin of a Filtek Z250 restoration after 1 week. Original magnication 243.

Fig. 3. A replica in epoxy resin illustrating a section of a Filtek Z350 restoration after 12 months, classied as marginal irregularity. Original magnication 1963.

Fig. 2. The replica in epoxy resin of a Filtek Z250 restoration after 12 months. Original magnication 243.

Fig. 4. A replica in epoxy resin illustrating a section of an EsthetX restoration after 12 months, classied as marginal gap. Original magnication 6323.

hygiene instructions. Each restoration was clinically evaluated after 1 week and 12 months. Margin Analysis Ten patients were randomly selected. The three restorations were molded with a low-viscosity polyvinyl siloxane material (Aquasil, Dentsply/Caulk, Milford, DE), and the molds were poured with epoxy resin o Paulo, SP, Brazil), gold-sputter coated (Maxepoxi, Sa (Emitech K550X, Kent, England), and observed by SEM (LEO 1430, Carl Zeiss, Jena, Germany) for evaluation, measurement, and classication of the cavity margins. Replicas were taken 1 week after placement of restorations and after 12 months (Figs. 1 and 2). A total of 60 replicas were made. The measurements and classications were made at 243 up to 4,0003 magnication (in doubtful cases); the entire perimeter of the cavity was examined (Montes et al., 2003). SEM examination was performed by one
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operator who was blinded to the restorative procedures. The Image J program (public domain, http:// rsb.info.nih.gov/ij/) was used for the margin analysis. The accessible marginal integrity between the resin composite and enamel was expressed as a percentage of the entire margin length that was available for eval mer et al., 2009). The measurements were uation (Kra recorded and classied, according to morphologically dened parameters, into the following types: perfect margin dened as a continuous, gap-free transition between restoration and dentin; marginal irregularity (Fig. 3), characterized as a noncontinuous but gapfree transition between restoration and dentin; marginal gap (Figs. 4 and 5), observed as gap formation and loss of interfacial adhesion, marginal fracture (Fig. 6), and artifact, when not conclusive (Frankenberger and Tay, 2005; Montes et al., 2003).

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A.K.M. ANDRADE ET AL.

TABLE 2. Results of the margin analysis for Filtek Z250, Filtek Z350, and Esthet-X (percentage and SD of entire evaluable margin length) Baseline (n 5 10) Filtek Z250 Perfect margin Marginal irregularity Marginal gap Marginal fracture Artifact Filtek Z350 Perfect margina Marginal irregularity Marginal gap Marginal fracture Artifact Esthet-X Perfect margina Marginal irregularity Marginal gap Marginal fracture Artifact 65.0 (7.8) 25.1 (5.2) 0.7 (0.4) 1.1 (0.8) 8.1 (5.9) 71.4 (7.4) 22.3 (7.2) 0.3 (0.2) 4.0 (1.1) 2.0 (1.2) 69.1 (6.2) 26.0 (4.3) 0.4 (0.3) 2.4 (0.8) 2.1 (1.1) 12 months (n 5 10) 50.3 (6.9) 39.4 (5.0) 1.5 (1.0) 4.8 (1.3) 4.0 (2.1) 46.7 (8.0) 43.8 (5.1) 0.0 (0.0) 9.1 (1.7) 0.4 (0.3) 34.2 (5.5) 54.8 (6.2) 0.3 (0.2) 4.6 (1.2) 6.1 (1.9)

Fig. 5. A replica in epoxy resin illustrating a section of a Filtek Z250 restoration after 12 months, classied as marginal gap. Original magnication 9283.

Indicate statistically signicant differences after 12 months.

Z350 composite was on the threshold of signicance (P 5 0.068). Comparison of the three materials after 1 week and 12 months showed no statistically signicant differences for all criteria (P > 0.05). The lengths evaluated were not statistically different between groups. DISCUSSION Resin composites are suitable materials for posterior cavities when a meticulous adhesive and layering technique is used (Dresch et al., 2006; Efes et al., 2006; mer et al., 2009). The major difErnst et al., 2006; Kra culty incurred in achieving a reliable technique for composite restorations is the rigid polymerization shrinkage of the restorative composites that challenges the bonded interface. Because of their inherent chemistry, current composites shrink on polymerization, thus introducing strain in the nal restorations. Unless the surrounding structures to which the composite is bonded have enough elastic compliance, something will fracture to compensate for the reduced volume and, consequently, create gaps, and leakage, which lead to recurrent caries and pulp irritation (Davidson and Feilzer, 1997; Frankenberger and Tay, 2005; Montes et al., 2003). In this study, margin analysis using a SEM served as an additional tool to clinical evaluation. SEM is more sensitive because of the increased evaluation. However, in vivo margin analyses has several shortcomings compared to in vitro research on marginal adaptation, which is routinely performed using thermomechanical loading and SEM analysis of epoxy replicas (Frankenberger and Tay, 2005; Frankenberger et al., 2007; mer et al., 2009). Even if the laboratory study tries Kra to simulate the real conditions in the mouth, only in the mouth, the restorations undergo all adverse conditions such as thermal and mechanical stresses associated with the role of the saliva. In this study, for the criteria perfect margin and marginal irregularity, deterioration after 12 months of clinical service was evident for three materials. Some studies have reported a high amount of marginal
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Fig. 6. Photomicrograph of a replica in epoxy resin illustrating a section of a Filtek Z350 restoration after 1 week classied as marginal fracture. Original magnication 4233.

Statistical Evaluation The Statistical Package for Social Science (SPSS) was used for the statistical analysis using the Wilcoxon and Friedman nonparametric tests and paired-samples t-test at a level of signicance of 5%. RESULTS The results of the SEM are shown in Table 2. For the criterion, perfect margin, between the two recall appointments, the Esthet-X and Filtek Z350 composites revealed statistically signicant differences (P 5 0.002 and P < 0.001, respectively) and Filtek Z250 was on the threshold of signicance (P 5 0.085); all decreased after 12 months. Marginal irregularity increased after 12 months; the Esthet-X composite was on the threshold of signicance (P 5 0.040). Marginal fracture increased that after 12 months; the Filtek

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mer et al., 2005, 2009; irregularity over time (Kra Spreaco et al., 2005). The three composites showed local marginal irregularities (of 2226%) at baseline despite the fact that the restorations were applied under a rubber dam by an experienced dentist. Within 1 year, the perfect margin decreased 1434% for all composites, in more evident way in the composites Esthet-X and Filtek Z350; marginal irregularities and marginal fracture increased. In agreement with Gaengler et al. (2004), this was mainly a result of excess material during application, later marginal fractures, and wear to a lesser extent. They afrmed that it is clearly impossible to avoid excess composite material especially next to ssures and pits, and, as a consequence, marginal fractures of the excessive material occurred. The consequent wear of composite and enamel surfaces contributed to a micromorphologically and clinically acceptable toothrestoration interface that was far from perfect. The evidence on clinical safety and longevity is supported by the micromorphologic assessment despite the obvious deterioration of marginal integrity. The myth of the need for perfect marginal integrity as the ultimate goal for composite restorations should be debated further. It is important to highlight the small amount of gaps found in this research, probably as a result of the restoration technique. Incremental lling techniques attempt to overcome the development of damaging polymerization shrinkage stresses and maintain a satisfactory restoration adaptation, mainly by optimizing the conguration factor and reducing the thickness of each increment (Spreaco et al., 2005). The prex nano has become fashionable in adhesive dentistry. The benets from incorporating only nanollers, as in Filtek Supreme and Filtek Z350 (3M ESPE, St. Paul, MN), are mainly related to translu mer et al., 2009; cency effects and polishability (Kra Mitra et al., 2003). However, clinical reports dealing with this class of materials show no signicant advantages in vivo (Dresch et al., 2006; Ernst et al., 2006; mer et al., 2009). In the classication used in this Kra study, Filtek Z250 was used as a microhybrid resin composite, and Esthet-X was used as a nanohybrid resin composites, incorporating nanollers other than conventional hybrid type llers. Margin analysis did not reveal any differences among the composites, and all restorations evaluated were clinically satisfactory, which indicates that even if some restorations have presented gaps, break-downs, and microscopic irregularities according to the clinical criteria outlined by the Modied USPHS (United States Public Health Service) guidelines, which is a long-established method used in clinical trials, these restorations have been classied as appropriate for clinical purposes. CONCLUSION The present investigation at the microscopic level conrmed the rst null hypothesis, because there were no differences in clinical behavior between Filtek Z250,

Filtek Z350, and Esthet-X as used for class I posterior restorations. However, the second null hypothesis was rejected, because there were differences in each composite over time. The materials performed satisfactorily over the 12-month observation period. ACKNOWLEDGMENTS The authors thank 3M ESPE and Dentsply/Caulk for the kind donation of materials for this investigation. REFERENCES
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