Arrest and Control of Carious Lesions: A Study Based on

Preliminary Experiments with Resorcinol-Formaldehyde Resin

C. ROBINSON, A. S. HALLSWORTH, J. A. WEATHERELL, and W. KUNZEL

Department of Oral Biology, Dental School, Leeds University, Leeds LS2 9NZ, England,
and Department of Preventive Dentistry, Medical Academy, Erfurt, G. D. R.

An experimental investigation has been made to introduce material with certain se-
made into the possibilities of retarding the lected properties into enamel lesions both in
progress of carious attack by infiltrating car- vitro and in vivo.
iostatic material into enamel lesions. The The different approaches to caries inhibi-
problems associated with this kind of proce- tion just mentioned are not, of course, mu-
dure are discussed against the background of tually exclusive. Any substance that will
experimental observations made using a for- penetrate the porous enamel of a lesion, for
mulation based on a resorcinol-formaldehyde instance, would enter fissures and by adher-
resin. ing to the enamel surface might also protect
the sound enamel.
Many attempts have been made to reduce CRITERIA AND CHOICE OF AN IDEAL TOPICAL
the incidence of dental caries by treating AGENT.-In an attempt to define the func-
tooth surfaces after eruption. One approach, tions and properties of an ideal topical pro-
using varnishes1 or polymerizing methacry. phylactic material, we considered the follow-
late and other sealants,2,3 aims to place a ing points were important.
physical barrier between the sound enamel 1. Carious lesions tend to develop in fis-
and potentially cariogenic bacteria in the sures, proximal surfaces and other relatively
most susceptible region of the dentition, the inaccessible parts of the dentition. These
enamel fissure. Other treatments, involving regions and the porous enamel of the lesion
solutions,4 pastes,5,6 or gels containing flu- itself are usually wet. Therefore, the cario-
orides,7 long-chain amines,8 and other agents, static material should be hydrophilic when
aim to enhance the natural resistance of applied, which would also permit the inclu-
sound enamel by reacting with the tooth sion of other cariostatic ions such as flu-
surface. oride.2 Since an incipient lesion is often
However, the impervious nature of sound undetected by normal clinical procedures,
enamel compared to the greater accessibility the material should also be strongly surface-
and perhaps reactivity of the porous carious active and have a low viscosity, so that it
tissue suggests that the principal means by will spread rapidly over the tooth surface,
which many topical applications exert their penetrate inaccessible areas, and enter the
effect may be by their penetrating into and pores of lesions.
accumulating in the porous enamel of the le- 2. Bacteria can never be completely ex-
sion itself where they retard, arrest, or even cluded and so the material should have bac-
reverse the process of lesion formation. Flu- teriocidal or at least bacteriostatic properties.
oride, for example, although perhaps not 3. The material must, however, be toler-
retained by sound enamel seems to accumu- ated by the pulp and other oral tissues.
late in the enamel of carious lesions.9-11 4. Because the lesion consists of porous,
From this point of view, we believe that physically weakened enamel, in its final
more deliberate attempts should be made to state, the material should offer some me-
treat the porous enamel directly. In the pres- chanical support.
ent study, an attempt has therefore been 5. The material should be cosmetically ac-
ceptable.
Received for publication June 2, 1975. Material that when introduced into the
Accepted for publication March 11, 1976. lesion in an aqueous phase would subse-
812
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Vol 55 No. S ARREST & CONTROL OF CARIOUS LESIONS 813

quently polymerize to a solid would be suit- more brittle and highly colored material
able. Such a polymer might with advantage tended to form. This property was, however,
also cross-link with the enamel mineral or potentially useful; when treated teeth were
the organic material in the lesion or both. brushed lightly with alkali, the resin surface
From a survey of currently available poly- polymerized almost instantly to form a seal
merizing materials, none completely fulfilled over the polymerizing resin.
the aforementioned criteria. The methacry- RESIN INFILTRATION OF NATURAL CARIOUS
lates, cyanoacrylates, and polyurethanes al- LESIONS OF ENAMEL, IN vITRo.-Extracted hu-
ready used as fissure sealants had too high a man permanent teeth with small white- or
viscosity even to penetrate deep or narrow brown-spot lesions were painted with the
fissures, would not polymerize in very moist resin solution which polymerized when the
conditions, and had limited bacteriostatic tooth was warmed to 50 C for about one
properties. minute with a warm-air blower. In later ex.
Resorcinol-formaldehyde resins seemed to periments, penetration was greatly improved
match the criteria most closely. They poly- by first etching the teeth for five to ten
merized from aqueous solutions at temper- seconds using a fine spray of 1 N HCI. The
atures low enough to be tolerated in the sprayer delivered less than 2 ml acid/min so
mouth (about 50 C). They could be intro- that, in the human mouth, the amount of
duced at a pH (about 8) that would not acid used would be tolerably low. The teeth
damage enamel and that would neutralize were subsequently sectioned using a diamond
any residual acid. Surface-active agents, disk and the sections examined in trans-
charged molecules, and water-soluble ions mitted and reflected light.
could be included. The resins also possessed RESIN INFILTRATION OF NATURAL CARIOUS
considerable antibacterial activity. LESIONS OF ENAMEL, IN vITRO.-Extracted hu-
The application of resorcinol-formalde- man permanent teeth with small white- oT
hyde resins in clinical dentistry is not new. brown-spot lesions were painted with the
Since they were introduced to endodontic resin solution which polymerized when the
therapy.'2, their use has been investigated tooth was warmed to 50 C for about one min-
by several workers.13,14 Their tendency to ute with a warm-air blower. In later experi.
shrink during polymerization, their irritant ments, penetration was greatly improved by
effect around the root apex,15.168 and their first etching the teeth for five to ten seconds
cosmetically objectionable red color result- using a fine spray of 1 N HCI. The sprayer
ing from oxidation'7 finally discouraged their delivered less than 2 ml acid/min so that, in
use. Resorcinol-formaldehyde formulations the human mouth, the amount of acid used
nevertheless corresponded most closely to the would be tolerably low. The teeth were sub-
criteria already described and they were sequently sectioned using a diamond disk
therefore used in the present experimental and the sections examined in transmitted
study. and reflected light.
PENETRATION INTO CARIOUS LESIONS IN
Materials and Methods vIVO.-A monkey (Macaca irus) was main-
PREPARATION OF RESIN.-The resin was pre- tained on a cariogenic diet'8 until identifiable
pared by dissolving 1.3 gm of resorcinol in carious lesions developed. After fasting for
2 ml 40% formaldehyde solution, 0.1 ml con- 17 hours, the monkey was sedated with an
centrated detergent (Teepol) a being in- intramuscular injection of metahexitoneb (20
cluded as a surface-active agent and the pH mg/kg body weight). The vocal chords were
adjusted to 8.2 with saturated aqueous KOH sprayed with 2% lignocaine HCI. A 2.5-mm
immediately before use. Care was necessary endotracheal tube was placed intranasally
at this stage to prevent overheating and pre- and anesthesia was maintained with 1%
mature polymerization. Polymerization oc- halothane + N20 at 2 to 3 liters/min and
curred at room temperature in about one oxygen, I liter/min. The airway was pro-
h-our. At 50 C, the resin polymerized in tected with cotton-wool rolls. After removing
about one minute. At a pH of more than 8, plaque and soft debris, the teeth were
the rate of polymerization increased, but a sprayed with I N HCI as previously de-

a Shell Chemicals U.K. Ltd., Manchester, Eng. b Brietal, Lilly & Co., Basingstoke, Hants, U.K.

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814 ROBINSON ET AL J Dent Res September-October 1976

A B D
100 FE

060f
4 F L

cr I
o.20

VO VI VO VI VO VI VO0VI,V,V3
BEFORE RESIN AFTER RESIN
APPt ICAtIO0N 11 A lCATfON

FIG 2.-Histograms, illustrating effect of resin

treatment on accessibility of lesion pores to
chloronaphthalene. V,, initial untreated pore
volume; V, pore volume after one treatment;
V,, pore volume after two treatments; and Vs,
pore volume after three treatments.

Results
A methlod was devised for determining the
FIG 1.-Buccolingual section of premolar ex- volume of space within these artificial le-
posed to acid-gelatin gel at pH of 4.5 for two sions before and after resin treatment. On
to four weeks. Demineralized porous enamel can removal from the gel, the teeth were thor-
be seen as white opaque band. E, enamel; D, oughly washed with hot water and allowed
dentin; N, nail varnish; and P, porous enamel. to dry in air. A drop of 3-clhloronaphthalene
(Refractive Index 1.63) was applied to the
scribed and dried thoroughly with a warm surface of the lesion where it gradually pen-
stream of air. Freshly prepared resin solu- etrated and "cleared" the porous enamel.
tion was applied to selected teeth with the When imbibition was complete, the enamel
use of a small brush, keeping the material surface was wiped with paper tissue and im-
as far away possible from the soft tissues.
as mediately immersed in 10 ml of spectro-
The resin was polymerized in about one min- ph-otometric grade hexane. After one hour,
ute using a warm-air blower. Finally, the the chloronaplhthalene had diffused from the
monkey's mouth was thoroughly rinsed with lesion into the hexane and was determined
water and 5%; sodium bicarbonate solution. spectroplhotometrically at its absorption max-
DETERMINATION OF PORE SPACE WITHIN imum (285 nm), and the volume of space
ENAMEL LESIONS.-During polymerization, the imbibed by the chloronaphthalene calcu-
resorcinol-formaldehyde resin preparation lated.
contracted by 30 to 40% and an attempt was The mass of clhloronaphthalene leached
made to determine what volume of the le- from the pores of the lesion was calculated
sion had been occluded by the resin. To do from the extinction value of the hexane so-
this, efforts were made to produce a "stan- lution at 285 nm and the molar extinction
dard" lesion in vitro. Porous enamel was coefficient at 285 nm, that is, 7,490 absorp-
prepared by placing sound premolars in a tion units. The volume of chloronaphthalene
10% w/v gelatin gel acidified to a pH of washed from the lesion was calculated from
4.5 with 1 M lactic acid. Most of the tooth its mass and density at room temperature.
was protected with nail varnish, leaving a Repeated determinations on natural as well
panel of enamel exposed. After two to four as artificial lesions indicate that the tech-
weeks at 16 C, the exposed panel of enamel nique gives a coefficient of vari ation of
was white, chalky, and partially demineral- 8%.
ized to a uniform depth of about 100 micro- The demineralized panels were then
meters (Fig 1) with an apparently intact treated with resin and the volume deter-
surface (judging from the presence of per- mined. The difference between the two de-
ikymata) terminations was presumed to represent the

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Vol 55 No. 5 ARREST & CONTROL OF CARIOUS LESIONS 815

280 r

260

240

220

200

180F
0

160

3 140
0

120
0
11'

80 _

60 F FIG 4.-Vertical section of natural approximal

carious lesion in human molar tooth, showing
40 _ extent of in vitro resin infiltration. Visible limit
of resin penetration is indicated by dotted line.
20
witli resin and the chloronaplhthalene-acces-
sible space redetermined. This indicated
that about 60% + 10% of the lesion's pore
Vo V1 Vo V1
volume hiad been occupied by resin. Figure
BEFORE ACID-GEL 2 shows four representative lesions treated in
TREATMENT this way.
The hiistological demonstration that the
AFTER ACID-GEL
resin was well distributed throughout the
TREATMENT porous enamel suggested that it had com
FiG 3.-Histograms, illustrating effect of resin pletely occluded 60% of the internal spaces
treatment on increase in porosity of prepared de- andl not meiely blocked access to them. That
mineralized enamel exposed to acid gel. V0, the space was only 60%o occluded was prob-
initial pore volume; V1, pore volume after an ably dtLe to tthe 30 to 40(% slhrinkage in the
exposure to gel for two days without (E) and iesitn that occui-s during polymerization. This
with (F) resin treatment. is supported by the fact that second and
thiird suiccessive resin treatments reduiced the
volume of space occupied by the resin. clhloronaphtllalene-accessible space by a pre-
VOLUME OF SPACE OCCLUDED BY THE RESIN.- dictable 80 and 99%, respectively (Fig 2,D).
The pore volume of lesions (namely the EFFECT OF RESIN ON SUBSEQUENT DEMINER-
space accessible to chloronaplhthialene) was ALIZATION OF TIlE LESION IN vITRo.-After de-
determined for lesions as previously de- termining their pore volume with chloro-
scribed. The lesions were then infiltrated naphithalene, tlhe artificial lesions were

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816 ROBINSON ET AL J Dent Res September-October 1976

.. .< 1.

II
I

FIG 5.-Vertical section of narrow human

molar fissutres sbowinig cxtent of in vitro resin 02 .. (
penetration. Some peneti ation into porous 1IG 6.-Longitudinal sectioni of monkey pre-
enamel oni fissLire walls is also visible. Visible niolar, resirn treated in N-ivo. Visible limit of
limit of penietlationi is in-idicated by dotted lines. lesini penetlation is iiidicatedi by dotted line.
treated withi resin, their pore volume was the material removed could be dletected aftet-
i-edetermined, antI the tectlh replaced in acidi otie hour.
gel (pH, 4.5). After two to thlree days in The total aniount of material leachled from
th-e gel, the pore volume of the lesionis was in locks of 1C.sin1 wotdldl correspond to
2-gm
again measuredl. It was fotind that the pore about 200 nig of i-esoi-cinol. In the ai-tificial
voliuine for conti ol paniels, that is, panels enamel lesions, a total of about 250o ig resin
not ti-eated witlh resin, increaseti by 300 %0 wotuld be )1resent and, assuming a similai-
moie tlian the pote volume fo- those gixNen degree of leacling, oilsv alout 25 ng of re-
at single i-esirn treatment and ain example is sorcinol wsould be t-eleasedl. 1 his estimate
slhown in Fligtire 3. miglht be low if tIre sinrface ai-ea of r-esin in
IISSOuIUTION OF NTAIFRIAI, FROM FRESHLY the enamel wais lhighl ant, in any instance,
POLYMERIZED RESINS.-To oltain some meas- the release of even siclc small amounts of
tire of the soluhility of r-esin components, )otentially toxic miaterials into the motuth
2-gm blocks of resin were freshlly preparedl in wouldk hase 10 be tlhorouglhly investigated b)e-
small plastic molds. These were suspended fore clinical utse of this tyl)e of material could
in 5 ml of molar soluitionis of soditum bicar- be contemplated.
Iconate (buffered to a pH of 6, 8, andl 9). PFNF1RATION OF RESIN IN-lO NATURAL LE-
Aliquots of soluition withidrawn at intervals SIONS IN VITRG . Ieeti Uisith whlite-spot lesions
of 1, 5, 10, 20, 60, and 120 minutes were ex- were sprayed witlh I N HCl for five to ten
aiminedl for (lissolved resin components. Al- seconds and tr-eated( wvith resin. After poly-
sorption peaks at 210 and 280 nm suggestedl nieriziiig the resin witlh warm air for one
that resorcinol, or some low molectular weighit minuite, the teetlh were sectioned and left
p)olymer intermetliates, were being leached expose(l to air ovei-niglrt. The p)resence of
from the iesin blocks. The rate of removal tde red coloration, a resuilt of the oxidlation
of mateiial from the resin blocks dleci-eased of resin, indicated that the bodies of the
logarithmically, lowever, and no increase in lesions were extensively infiltrated (Fig 4).

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Vlzo 55 No. 5 ARREST & CONTROL OF CARIOUS LESIONS 817

Penetration into the base of deep and very the mucosa with the air blower during resin
narrow fissures was also routinely observed polymerization.
(Fig 5). Perhaps the most serious objection to this
PENETRATION OF RESIN INTO LESIONS IN material is the possible effect of resin on
vivo.-The teeth of a monkey (Macaca irus) vital dentin or pulp should the lesion extend
in which carious lesions were induced18 were so far. With regard to the cosmetically ac-
treated with resin as previously described. ceptable criterion, the dark-red color pro-
Two years after treatment, several teeth were duced by oxidation could be cosmetically
extracted and sectioned. Some resin was still objectionable although the resin would not
in place even on the tooth surface. On ex- necessarily be visible in fissures and inter-
posure to air for about 24 hours, the red proximal regions.
color, characteristic of oxidized resin, was The suitability of the resin as a caries pro-
visible throughout most of the depth of the phylactic is therefore questionable. How-
treated lesions (Fig 6). ever, the concept of such a treatment and
the techniques developed for its use seem to
Discussion and Conclusions point to a feasible line of approach for the
treatment of dental caries.
One of the primary aims of this study was In view of the recent great advances in
to set out the requirements of a material polymer science, it seems likely that other
suitable for treating noncavitated carious potentially useful materials may soon come
enamel lesions. An attempt was made to to light.
find such a material, to introduce it into
porous enamel and natural carious lesions, The authors thank Dr. W. H. Bowen and Mr. M.
to assess the likely effect of such treatment Cole of the Royal College of Surgeons, England, for
their facilities and help with the monkey investigation,
on the progress of lesion development, and and Mr. G. Moore for his technical assistance.
to determine whether such material would
be retained in the mouth. It was thought References
that the ideal material should be (1) water- 1. MAIWALD, H.J., and GEIGER, L.: Lokalappli-
based or, at least, hydrophilic; (2) highly kation von Fluorshutzlack zur Karies Pro-
surface-active withi a low viscosity; (3) anti- phylaxie in Kallekriven, Dtsch Stomat 23:
microbial; (4) nontoxic to the oral soft tis- 56-63, 1973.
sues; (5) capable of polymerization into a 2. BUONOCORE, M.G.: Adhesives for Pit and
solid plhase under physiologically tolerable Fissure Caries Control, Dent Clin North Am
conditions; and (6) cosmetically acceptable. 16: 693-708, 1972.
Experiments have shown that a resorcinol- 3. SILVERSTONE, L.M.: Fissure Sealants: Labora-
formaldehyde formulation goes some way to- tory Studies, Caries Res 8: 2-26, 1974.
4. MELLBERG, J.R., and NICHOLSON, C.R.: Flu-
ward fulfilling these criteria, particularly the oride Uptake In Vivo by Deciduous Enamel
first tlhree and the fifth. This material could of Children from Neutral Fluoride and APF
be introduced into lesions in vitro and in Mouthrinses, Caries Res 8: 148-154, 1974.
vivo, and it possessed antimicrobial activity. 5. BUONOCORE, M.G., and GWINNET, J.A.: Chem-
Treatment of porous enamel reduced the ical, Polarized Light, and Microradiographic
rate of demineralization in acidified gelatin Study of the Effects of Various Toothpastes
in vitro; in addition, the resin was retained on "White Spot" Formation In Vitro, J Oral
in vivo. A more comprehensive study, prob- Ther 3: 321-329, 1967.
6. VRBIC, V., and BRUDEVOLD, F.: Fluoride Up-
ably with a large number of monkeys, would take from Treatment with Different Fluoride
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since this treatment had certain unsatisfac- Pastes Containing a Soluble Aluminum Salt
tory features. With regard to the nontoxic Followed by Topical Application, Caries Res
to oral soft tissue criterion, local ulceration 4: 158-167, 1970.
of the oral mucosa occurred in the vicinity 7. RIETHE, P., and WEINMANN, K.: Caries In-
of the monkey's treated teeth, which might hibition with Fluoride Gel and Fluoride
have been due to a rapid loss of unpolymer-
Varnish in Rats, Caries Res, 4: 63-68, 1970.
8. LEAVER, A.G.: Long-Chain Aliphatic Amines
ized resin components after initial polymer- as Potential Caries-Preventing Agents, NZ
ization. Alternatively, the ulceration, which Dent J 67: 99-106, 1971.
disappeared within 24 to 48 hours, might 9. DowsE, C.M., and JENKINS, G.N.: Fluoride
merely have been due to heating and drying Uptake In Vivo in Enamel Defects and Its

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Significance, J Dent Res 36: 816, 1957. 14. MULLER, 0.: Pulpa-und Wurzelbehandlung,
10. JOHANSEN, E., and NORDBACK, L.G.: Ultra- Berlin: 1948, pp 110-111.
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Dental Caries, in SOGNNAES, R.F. (ed): wendung der Albrechtschen Wurzelfullung,
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Washington, D.C.: American Association for 16. PLACKOVA, A., and SICHA, V.: Eine Klinisch-
the Advancement of Science, 1963, p 199. experimentelle Studie uiber Wuzelfiullmittel
11. HALLSWORTH, A.S.; ROBINSON, C.; and aus Resorzin-Formalin-Kunstharz, Dtsch
Stomat 10: 284, 1960.
WEATHERELL, J.A.: Chemical Pattern of 17. BERTRAM, E.: Zahnverfarbung nach Anwen-
Carious Attack, J Dent Res 50: 664, 1971. dung der Resorzin-Formalin-Alkali-Wurzel-
12. ALBRECHT, J.: Verfarbung durch Resorzin- ffillung nach Albrecht, Dtsch Zahnaertzl
Formalin-Alkali-Wurzelfullung, Dtsch Zahn- Wochenschr 18: 357-358, 1915.
iiertzl Wochenschr 18: 577-582, 1915. 18. BOWEN, W.H.: The Induction of Rampant
13. REBEL, H.H.: Konservierende Zahnheilkunde, Dlental Caries in Monkeys (Macaca irus),
2nd ed, Munich 1947, p 413. Caries Res 3: 227-237, 1969.

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