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NIOM Scandinavian Institute of Dental Materials, Forskningsveien (Received 20 November 1984; revised 14 February 1985) 1, 037 1 Oslo 3, Norway
The release rate of mercury from a conventional, under static conditions in stimulated exponentially artificial
a dispersed phase or a spherical high copper content amalgam saliva than in
or artificial saliva has been measured and found to decrease approximately
with time. A higher initial release rate was observed for mercury in stimulated
saliva during the in vitro experiments. exponentially with time. After brushing the surface of the amalgam during two an increase in corrosion current was measured surface has been proposed.
In a pilot study corrosion current was recorded from an amalgam specimen immersed in saliva, and was found to decrease approximately subsequent periods, in a manner similar to toothbrushing,
indicating the removal of loosely bound corrosion products. A model describing the periodical mercury release from an amalgam
Keywords: Dental materials. mercury release, amalgam corrosion, saliva
During exposure of an amalgam restoration to chewing forces mercury might be released’. The levels of mercury in the mouth air and blood before and after chewing have been measured in a group of individuals with amalgam restorations as well as in a control group without such restorations’. Significantly higher air mercury levels were demonstrated after chewing than before chewing. The blood mercury concentrations were found to be positively correlated with the surface area of the amalgam restorations. An in vitro approach to simulate the mechanical interactions involved in chewing is accomplished by so-called cyclic loading. During such interactions considerably higher release rates of mercury were registered in artificial saliva3 than under static conditions4f5. A substantial part of the mercury released from the amalgam surface is present in amalgam particles3* 5. It is known that various types of corrosion products of tin are deposited on amalgam surfaces”,’ and may possibly act as a semi-protective layer, reducing the corrosion rate. According to ESCA-measurements (electron spectroscopy for chemical analysis) such corrosion products have been found to be loosely bound to the surface and may be removed from the surface by a brushing procedure similar to toothbrushing in vitro8. After brushing a clean surface is obtained. Exposing such a surface to an electrolyte, electrochemical corrosion could be expected to be pronounced, resulting in the release of Hg2+(Hg2”) ions. In addition, unreacted mercury, i.e. Hg’, could be released from the surface. Presently, the static release pattern of mercury in at-tifical and natural saliva was studied in vitro in order to obtain knowledge about the release rate versus time, as well as about possible migration of mercury corrosion products
through the pellicle which is deposited on a restorative material like amalgamg. Furthermore, the effect of brushing an amalgam surface on corrosion current was studied. MATERIALS AND METHODS
Amalgams. The release of mercury in both natural and artificial saliva was studied on 4 freshly prepared cylindrical specimens of the product Dispersallo\$, 8 mm high and 3 mm in diam. (Table 1). The alloy powder was triturated with radioactive mercury (“‘Hg, 203Hg). The radioactive specimens were exposed to natural or artificial saliva, about 10 min after mixing, for a period up to about 13 h. The samples were not polished. During these initial release measurements cylindrical specimens were considered in view of rapid preparation of such samples allowing measurements to be conducted soon after trituration. For the same reason the samples were not polished. Also the release of mercury from old amalgam specimens, i.e. about 1 mnth old, was studied on 4 specimens each of a conventional, a dispersed phase and
Table 1 Amalgams studied Type Conventional Name Revalloy@ Manufacturer S.S. White Ltd. Middlesex. England Batch no. 117234
Johnson b Johnson, 8L 713 Dental Products Co., E. Windsor, NJ, USA Kerr Mfg Co., Rochester, NY, USA 1027752289
Spherical high copper content
Butterworth Et Co (Publishers) Ltd. 0142-9612/85/050357-03$03.00 Biomaterials 1985, Vol 6 September 357
i. The saliva comprised either natural saliva collected under stimulated conditions by chewing parafilm.e.5 and 7. 358 Biomaterials 1985. During the 10 to 30 min time periods proteins in the natural saliva samples were not observed to precipitate. A higher release rate was indicated in the stimulated saliva than in the artificial saliva in the initial release phase.3 mm. Elemental mercury (Hg’) is also released during the action of forces’. in this case. measuring 5 X 10 mm with a thickness of about 0. In this case corrosion products of tin deposited on the amalgam surface seems to have been removed by brushing as indicated by ESCA-measurements’. once for 10 s and again for 20s. it has been shown that the elements carbon. The nuclear technique used has been described previously5* lo.01 0 Dispersalloy 0 Revalloy Ei Sybralay ‘. while stirred under aerated conditions. or artificial saliva of the modified Fusayama type” containing no proteins. The release rate refers to 4 freshly prepared specimens of a dispersed phase type amalgam. i. Figure 3 Corrosion current from 1 amalgam specimen measured against a Pt-electrode versus time.001 o.e. Toothpaste was not used during these measurements. The total corrosion current from 1 specimen of dispersed phase amalgam was measured against a Pt-electrode by means of a galvanometer with an inner resistance of 10 kn while the amalgam specimen was immersed in stimulated saliva at 23°C. while Figure 2 concerns the release from old samples. &me a spherical high copper content amalgam type immersed in artificial saliva (see Table 7). Figure 2 presents static release rates for 3 types of amalgams immersed in artificial saliva.1 N E 0 . The release rates in both cases decline approximately exponentially with time. Currents were registered during a period up to about 36 h. Corrosion current following this procedure was measured. Vol6 September .5 ml of the saliva solutions. be ascribed to corrosion of zinc and tin5-7.5 rT 0. The amalgam surface has been brushed in 2 periods. Saliva. Current measurement.e. mercury in all chemical forms occurs during cyclic loading in stimulated saliva13 analogous to the conditions in artificial saliva3.oooe 5’0 Time(h) Id0 Figure 2 Release rare understatic conditions for totalmercury from 3 types of amalgams of age about 1 mnth deposited quickly in a l-2 nm thick surface layer (ESCA-information depth) of an amalgam immersed in vitro in natural saliva’. 0. during cyclic loading13.A model for periodical mercury release: 0. The amalgam specimens were immersed in 7. Release under dynamic conditions. Corrosion current measurement. Ionic mercury may be released through RESULTS AND DISCUSSION Static release measurements. at 37°C.005 * 0. i. The decline in the release rate was especially pronounced for the freshly prepared specimens (Figures 1 and 2). while the rapid deposition of these elements indicate the fast deposition of the pellicle. These specimens consisted of rectangular sheets. oxygen and nitrogen are Total electrochemical release Me”*Me2*+ 2e- 0 Natural saliva a Artificial saliva 50 aI '0 : 30 N E 4 a IO c 0 2 Time (h) 3 10s brushing it 2 bruz Time (h) )S 36 + Figure 1 Static relese rate of total mercury versus time in stimulated and artificial saliva.05 0. Amalgam particles are mainly released. These elements are the main constituents of the saliva proteins’*. According to ESCA-measurements. After cleaning the amalgam surface by brushing a strong increase in the current was observed. Each bar with standard deviations represents the mean value of 4 measurements. and the pH remained between 6.: 0. The samples had been ground with 1000 grit paper. from freshly prepared samples. replaced at intervals between 10 and 30 min. Figure 1 pertains to an initial release period shortly after trituration. This seems also to occur under dynamic conditions. An approximate exponential decline was observed in this pilot study. Figure I represents the static release rates of total mercury (all forms) in natural or artificial saliva. Mercury seems to have migrated through such layers under the present static release conditions (Figure I). The samples were about 1 mnth old. A substantial fraction of the current could probably. The amalgam specimen was brushed in 2 periods on one side with a toothbrush to simulate toothbrushing. A high release rate of total mercury. 0. Figure 3 illustrates the total corrosion current versus time for the amalgam sample exposed to the saliva.
J.W. Initial Suppl.. In Katayori.. 855-859 D. Man’s Sci. through brushing. (Eds R.g. Dent.G.. Res. exponenng 30 Nov-2 T. Evje. levels.. mercury Dent. The model involves high mercury release rates (mercury in all forms included) during loading13. rn Proceedings: Stiles. and T. Stockholm. Eye. amalgam. saliva Res. D. (abstract) Microbial Aspects of Dental Caries. 2 Abraham. D.. 239-242 Dent. S. Cox. Dent.. 15 Marek. on blood 1. 59.. J. 198 1. application of various mastical forces and brushing the amalgam restorations etc. Royal Institute of Technology. Corros&on other. Nilsson.e. First. Based on another study13 and present findings a model describing the mercury release pattern during dynamic and static conditions is proposed. Svare. Marshall. Brune. and Reinhardt.J. 42. 165-l T. 1984. Res. Marshall. i. London.J. Fusayama. 985-986 Frank. of dental 820-823 products amalgam. A substantial effect of corrosion occurred even at low pressure. followed by decreasing release rates under the subsequent static conditions. S. Hultquist. rn Surface and Colloid Phenomena in the Oral Cavity: pp 227-237 mercury loadrng from a dental amalgam. 506-514 FL. Surface 3 Her0. NIOM. should be considered in detail. Deposits on the amalgam surface may be removed by mechanical interactions inherent with the chewing processes..W. Interaction between human and various hydroxy- The periodical release model.M.. 1984. Res. 1985. whereby corrosion products may be removed through scratches in the pellicle film... (Eds H. H.. REFERENCES electrochemical corrosion. C. 1984.. Leach)..M. Loesche 1976. MethodologicalAspecfs.. Clinically. Brune.5 MPa’a. and schematically outlined in Figure 4. Acceleratron 63. e. comprising mainly tin compound8 7. Frank and S. H. van Quecksrlber aus Amalgamfullungen Otsch Zahnaerztl Z 1976.. B.. 0 $ Ii Time (h) 7 I 18 24 Figure 4 Scheme of model for mercury release (all chemical forms) from an amalgam surface under dynamic and static conditions..D. 1983.. 1010-1013 of cormsron J. and Stockholmsmassan. The effect J of dental amalgam 63. Sweden for kindly conducting the corrosion current measurements and to D. J.T. II1 . R. Stand. between meals. Lakaresallskapets Alvsjb. 44. This situation corresponds to the clinical condition of rest.. Chewrng releases mercury fillrngs. on composrtron amalgam colomzation composite in vitro. Under static release conditions mercury ions.A. chewing time. Diehl.. high initial corrosion currents were registered after accomplishing abrasion of the amalgam surface with soft pads in an electrolyte. fran Dec. Calif. A decrease in current then followed consistent with the present findings (Figure 13). static release conditions may exist during rest periods e. restorations 71-73 J. Dent. Res.J.M... frequency of meals. Dent. Dent.W.g. unreacted mercury (Hg’) as well as particles are expected to be released. Nordberg. contact 92. D. D. Clinically such release mechanisms occur during the normal wear and deterioration of an amalgam restoration14. D.g. Pellicle and 9 S0nju. corrosion of amalgams. 1982. In order to predict mercury release in the oral cavity under different clinical conditions various parameters inherent with masticatory functions (chewing habits) e. 1982. Vol 6 September 359 . Electrochemicalcorrosion during static conditions.. R. Corrosion of amalgams.M. G. Nomoto.. After exposing such a surface to the electrolyte under static conditions. From the unprotected amalgam surface the initial corrosion rate would gradually decrease (Figures 7-3) as a consequence of the formation of a semi-protective surface layer of corrosion products.. G.B. Ahgabe and cyclrc loading.. from D. J of gold and amalgam Dent. G. Kwcksrlver Rrksstamma p 217 rnrtral bactenal Res. corrosron Microb!ol. J. Ass. ACKNOWLEDGEMENTS The author wishes to express his gratitude to Dr G. degradation of amalgams in vitro during 91.. static Eye. Removal of corrosion products from the amalgam surface. Res. at 0. for skilful technical assistance in the various experimental procedures. Jwgensen. Biomaterials 1985. Stand. of amalgams pp 133-141 10 11 Brune.M. Eye. 1981. Corrosion 90. Dent. Skjrarland. each with 71 S. 31. Information Retrieval. Stand. J.. 51-63 The toxicity of mercury rn dental amalgam. reveal a nonprotected amalgam surface. dentala 1983. D.A. J.. apatite K. III III I II I iI I II I II I : iii II II II II I Static ii i I I I I I I I I II II II II II II II i II II II II I Static iii I II I II I I.W.E.. 47-61 of dental amalgams by abrasron.H. In den Brune.G. Mayer. products Jensen. 1982. 1 Gay.. in vitro. J. 13 Brune. O’Brien) Spec. Sn4(OH)sC12 and SnO 89. J.488-495 W. C. Hultquist. placed 1183-1197 12 Eggen. Brune Dynamic Dynamic : I Dynamic : I II II II ii . Stand. According to a recent investigation by Marek’“. Res. 6.D..A model for periodical mercwy release: 0. 1963. Lancet 1979. Speichel. I II I II I II I II ’ : Static Adaption of the model to clinical conditions...M. electrochemical corrosion is expected to prevail. M. 14 Bauer. surfaces. W. D. Total Environ. K.
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