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David G. Wildgoose, MPhil,a Anthony Johnson, PhD, MmedSci,b and Raymond B. Winstanley, MDS, BDSc School of Clinical Dentistry, University of Shefeld, Shefeld, United Kingdom
This review considered the development of glass, ceramic, refractory materials, and techniques over a period of 25,000 years, from the time of stone-age man to their introduction into dentistry. Currently a wide variety of all-ceramic dental restorations are provided using alumina-reinforced, leucite-forming, and novel glass and ceramic materials along with a range of refractory materials and associated techniques. However, some of the problems of dimensional and thermal change experienced by early craftsmen still persist during current laboratory fabrication techniques. Early English archaeological and dental publications were obtained through the Archaeology Education Department of the British Museum in London and the Archives of the British Dental Association Library. More recent peer-reviewed articles published from 1966 to the present were obtained through MEDLINE. (J Prosthet Dent 2004;91:136-43.)
t is difcult to consider the development of refractory mold materials without considering the glass or ceramic which would be formed within or around their surfaces. Glass has its history at the beginning of time, with naturally occurring volcanic glasses such as obsidian being fashioned into implements, tools, and jewelry as early as stone-age man1 (Fig. 1). Pliny is said to have suggested that man rst produced glass accidentally when a wood re was made on a bed of silica sand.2 It is possible that this method may have produced temperatures in the range of 560-900C, which would have been sufcient for an initial fusion of the 2 predominant elements of sand and soda ash to form a crude glass.3 However, it is more probable that the rst deliberate attempts to manufacture glass were the consequence of the potter, whose ancient art was dependent on re,1 with some of the earliest burnt clay objects recorded in areas of Czechoslovakia approximately 23,000 BC4,5 and Russia approximately 16,000 6 BC. This review of the literature describes the development of glass, ceramic, refractory materials, and techniques over a period of 25,000 years, from the time of stone-age man to their more recent introduction into dentistry. A time line (Table I) illustrates some of the more signicant development trends, which were sourced through the Archaeology Education Department of the British Museum, London, the Archives of the British Dental Association Library, and through MEDLINE from 1966 to the present.
Dental Instructor, Department of Adult Dental Care. Dental Instructor, Department of Adult Dental Care. c Reader, Department of Adult Dental Care.
b
Evidence of rst burnt clay artifacts Pre-Neolithic period mans rst use of naturally occurring glass (obsidian) Ancient Egyptians use molds of Steatite to pour or press glass Egyptians form glass vessels around a refractory core of mud, sand, and animal dung Evidence of lost wax technique for metal and possibly glass casting Phidias casts glass into a variety of shapes using clay molds
Introduction of glass and refractory materials and techniques into dentistry Mayan civilization Alexis Ducha teau Murphy Various researchers Charles Henry Land Charles Henry Land Legro Brodsky Moore and Watt Buonocore Morrison and Warnick McLean and Hughes MacCullock Francois Duret Horn Calamia Mo rmann and Brandestini Adair and Grossman Sadoun Wohlwend and Scharer Techceram 400900 1774 AD 1833 AD 187099 1895 1901 1931 1933 1949 1955 1959 1965 1968 1971 1983 1983 1980 1985 1985 1990 1996
AD AD AD AD AD AD AD AD AD AD AD AD AD AD AD AD AD AD
AD
First evidence of milled plugs (inlays) of jade or obsidian for esthetic purposes Developed technique for red porcelain dentures Fabricated glass inlays using a platinum foil matrix Continued to develop glass/porcelain inlays, using gold/platinum foil matrix and/or refractory die support Developed platinum foil matrix for fabricating porcelain crowns Fabricated and tted the rst porcelain laminate veneers Described use of acid to etch porcelain Reported rst manufactured refractory material for dental use (German-Brillat) Developed phosphate-bonded refractory material Reported method of chemically etching enamel Reported ndings of ethyl silicate refractory material for dental use Developed alumina core material to strengthen dental porcelain First reported the use of glass casting for dental purposes First to consider the automatic production for dental restorations (CAD-CAM technique) Combined etched enamel/porcelain technique to resin bonded restoration Re-introduced the method of etching porcelain, for resin-bonded restorations Developed chairside CAD-CAM system for machining dental porcelain (CEREC) Developed the rst commercial castable glass (Dicor) First developed the alumina-inltrated glass technique (In-Ceram) Reported on a technique for pressed glass restorations (Empress) Commercial introduction of thermal spray technique into dentistry
1527-1475 BC, hollow glass vessels were formed around refractory cores.1,7,8,10 Although some uncertainty exists, it has been suggested that these cores may have been dipped into a glass previously heated in clay crucibles until molten, or, alternatively, colored rods of softened glass may have been wound around the core before being rolled to obtain the desired shape (Fig. 2). Further evidence suggests that the lost wax casting process (cire perdue), used by the Al Ubaid culture of Ur around 3500 BC11 for casting metals into enclosed molds,12 was being adopted by these 14th-century Egyptian artisans for the forming of glass ornaments2,9 (Fig. 3). However, by the 5th century BC, glass was being cast into a variety of shapes by the Greek sculptor, Phidias, using clay molds2 (Fig. 4). It is probable that these soft clay molds improved the speed of manufacture of hollow vessels, lessening the possibility of damage during the divesting of the surrounding mold material.9 By the rst century BC, glass blowing techniques appeared in areas around Phoenicia.2,8 However, it was later refractory mold blown glass that heralded a complete change in glass manufacturing techniques that would not be matched until the introduction of mechanized methods in approximately 1820 AD.2
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Fig. 2. Core formed glass vessel of bulti-sh, designed to hold scented oil, circa 1350 BC. Copyright The British Museum.
Fig. 5. Mayan tooth with jade inlay, circa 800 AD. Image courtesy of British Dental Association Museum Collection (LDBDA 7688). Fig. 3. Intact refractory mold for early gold casting found in Columbia. Image from Bray12 reprinted with permission from World Gold Council.
binders of animal dung was used.2,4,14 It may be that early glass manufacturers modied the compositions of their refractories in order to achieve the particular refractory property required, as these molds would have to demonstrate good dimensional stability,4 have a coefcient of expansion slightly greater than that of the glass in order to prevent cracking,14 and be sufciently soft to scrape out.13 Archaeologists Bimson and Werner reported in 1968 at the International Congress on Glass, London, that additions of calcite, lime wash, or clay were applied to the surface of a wax pattern prior to molding the bulk of the refractory, in order for ne surface detail to be reproduced by both the mold materials and subsequent cast glass.
Fig. 4. Sculpture of ram, cast in glass using closed mold technique, circa 600 BC. Copyright The British Museum.
reported about the diversity of manufactured refractory mold materials. This may be due in part to the disposable nature of the mold, and that on decomposition it would be difcult to differentiate the individual materials from the natural surroundings from which they were developed. Evidence shows that where hollow glass vessels were fabricated, a manufactured refractory core of mud, sand, and highly ferruginous clay with organic
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Fig. 6. Set of porcelain dentures made in style of Nicholas de Che mant, late 18th century. Original held by Odontological Museum, Royal College of Surgeons of England, RSCOM K1.1. Image courtesy of British Dental Association Museum.
rials. This may have been due in part to volumetric shrinkage occurring within the porcelain paste materials during the continued ring processes. A report by Moft (1887)20 recognized that the warpage and cracking of the porcelain body may be minimized by dispensing with investments of plaster and pumice in favor of int sand when fabricating continuous gums, thereby encouraging a variety of materials and techniques to be developed.
warpage of the foil and ring shrinkage of the powdered ceramic.22-25 Land (1889)26 describes a method of improving the t of porcelain llings by burnishing platinum foil directly into the preparation. Simonis (1890)27 cites Richter as developing a technique whereby a colored glass was fused within a matrix of platinum or gold previously formed by burnishing it into the preparation. However, Darby (1899)28 described a method of using pulverized asbestos to support a foil matrix while fusing occurred. By the late 19th century, various attempts were being made to use foil matrices, either independently or in conjunction with what may loosely be termed an investment mold, during the construction of porcelain and glass restorations. Simonis, in 1890,27 recommended using pulverized asbestos or a mixture of plaster and pumice to support the foil matrix during ring, but failed to provide any reason why this mixture was preferred. An undisclosed investment was described by Nyman (1905)29 to support the platinum or gold matrix in order to prevent warpage due to annealing of the foil matrix and shrinkage of the porcelain during ring. However, Jenkins (1913)30 observed that whether a matrix was adapted directly intraorally or indirectly on a cast, a noticeably disguring cement lute, due to defective edges, was more prevalent with porcelain restorations fabricated on a platinum matrix than those on gold foil. During the early part of the twentieth century, numerous authors19,31,32 cited Lands successful development (1886) and subsequent patent (1889) of the platinum foil matrix when fabricating ceramic crowns. This technique provided restorations with both a clinically acceptable t and esthetic quality. The same technique was again described by Land (1903)33 and much later by Pincus (1937)34 for the fabrication of articial ceramic veneers. However, it was to be much later in the century before this technique became popular.
Fig. 7. A, Gypsum bound refractory after ring at 690C. B, Gypsum bound refractory after ring at 950C.
mold in order to fabricate restorations from a variety of materials. Unfortunately, the author provides no indication as to the effect of plumbago on the color of the resultant porcelain or glass restoration. A considerable shrinkage of the red glass was observed by Ernsmere,35 who suggested that even when a second refractory transfer mold was made, the resultant t was less than satisfactory. These early twentieth century researchers continued to experiment with a variety of refractory materials in an endeavor to overcome persistent problems with shrinkage of the refractory, and cracking of the porcelain or glass during ring.
It is important to recognize that, as dental porcelains and glasses are red more than once at temperatures of approximately 950C, the observed contraction and roughness may in part be attributed to a continued decomposition of the gypsum binder of the refractory investment (Fig. 7), which may have contributed to the inaccuracy identied by previous workers.38,43
Fig. 8. Mismatched ceramic and metal thermal expansion coefcients resulting in ceramic failure.
Fig. 9. Thermal expansion coefcient mismatch of ceramic and refractory resulting in ceramic failure.
Table II. Mean dimensional change after ring for 7 selected refractory materials
Material Results % CeramiteH CeramiteV Corum Flexo-Ceram Hi-Ceram Vitadurvest Whipmix VHT
1st ring 2nd ring 3rd ring 4th ring 5th ring 6th ring
1.18 0.07* 1.24 0.08 1.23 0.08 1.24 0.07 1.25 0.08 1.24 0.07
0.45 0.08 0.51 0.08 0.50 0.08 0.51 0.08 0.53 0.09 0.51 0.08
0.34 0.04 0.32 0.03 0.32 0.04 0.28 0.04 0.29 0.03 0.27 0.04
0.90 0.02 0.91 0.02 0.94 0.02 0.95 0.02 0.96 0.01 0.94 0.01
0.08 0.02 0.08 0.04 0.09 0.02 0.10 0.02 0.11 0.02 0.11 0.02
0.00 0.05 0.03 0.05 0.03 0.06 0.02 0.07 0.05 0.07 0.04 0.07
0.12 0.04 0.08 0.02 0.09 0.03 0.08 0.05 0.07 0.03 0.07 0.03
Refractory die materials for the fabrication of conventional all-ceramic restorations and laminate veneers
More recently, a variety of phosphate-bonded refractory materials have been described in the literature when fabricating a range of all-ceramic restorations.51-56 In 1985, Calamia57 suggested the use of phosphatebonded refractory materials when fabricating all-ceramic laminate veneers using conventional dental ceramic materials and techniques. However, problems of t58-61 along with cracking59,60 and adherence of the ceramic to the refractory material were again recognized.60 For these reasons, some workers62-64 continued to advocate using the platinum foil technique to avoid an interaction of the porcelain with the refractory, while recognizing the benet from the support offered by an underlying refractory cast. However, Hunt65 suggested that all-ceramic veneers made on refractory dies are less susceptible to warping, and that thermal contraction may be controlled by reducing the size of the refractory die. The marginal integrity of ceramic veneers fabricated on matched and unmatched refractory dies was compared by McIntyre et al in 1993,66 who concluded that a sigFEBRUARY 2004
nicant improvement in marginal accuracy was evident where the ceramic and refractory were matched. Many researchers have considered the residual stress in a number of alloy-porcelain combinations,67-70 concluding that to minimize stress levels in the veneering porcelain, the thermal expansion/contraction of the porcelain must be matched to the alloy between its glass transition and room temperature (Fig 8). Conversely, little has been reported regarding the consequence of mismatch for current dental refractory and ceramic combinations71 (Fig. 9). Only recently (2000) has an International Standard (ISO 11245)72 for phosphate-bonded refractory die materials been introduced. A recent study by Wildgoose and Winstanley73 showed that a wide range of dimensional change occurred during setting, varying between 1.8% 0.05% and 0.11% 0.02% at 24 hours for 7 phosphate refractory materials identied in a survey.71 When further investigation was conducted, a nal dimensional change of between 1.24% 0.07% and 0.27% 0.04% was evident upon completion of 6 identied ring cycles (Table II). 73
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systems continue to improve, their capital costs are considerable, requiring a high production turnover in order to achieve nancial viability.
SUMMARY
There have been many novel refractory and/or ceramic developments. However, many have not been sustainable over time. This may be due to the initial capital outlay, technique sensitivity, or a need to continually develop the product in reaction to market forces. Many conventional ceramic and refractory materials are currently available, although problems encountered by the early artisans and technologists relating to ceramic fracture and dimensional change (warpage) still persist. To date, little has been reported regarding the selection of refractory materials and laboratory techniques when fabricating all-ceramic restorations on refractory dies. Information about the dimensional change after multiple ring and thermal expansion coefcients of refractories may enable the laboratory to select a compatible refractory and ceramic combination.
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