Hostname: page-component-cd9895bd7-dzt6s Total loading time: 0 Render date: 2024-12-25T08:48:39.718Z Has data issue: false hasContentIssue false

DO WEAK OR STRONG ACIDS REMOVE CARBONATE CONTAMINATION FROM ANCIENT TOOTH ENAMEL MORE EFFECTIVELY? THE EFFECT OF ACID PRETREATMENT ON RADIOCARBON AND δ13C ANALYSES

Published online by Cambridge University Press:  13 May 2021

Rachel Wood*
Affiliation:
Research School of Earth Sciences, Australian National University, Acton, 2601, Australia School of Archaeology and Anthropology, Australian National University, Acton, 2601, Australia
Andre Barros Curado Fleury
Affiliation:
School of Archaeology and Anthropology, Australian National University, Acton, 2601, Australia
Stewart Fallon
Affiliation:
Research School of Earth Sciences, Australian National University, Acton, 2601, Australia
Thi Mai Huong Nguyen
Affiliation:
Anthropological and Palaeoenvironmental Department, The Institute of Archaeology of Vietnam, Hanoi, Vietnam
Anh Tuan Nguyen
Affiliation:
Anthropological and Palaeoenvironmental Department, The Institute of Archaeology of Vietnam, Hanoi, Vietnam
*
*Corresponding author. Email: [email protected]

Abstract

In hot environments, collagen, which is normally targeted when radiocarbon (14C) dating bone, rapidly degrades. With little other skeletal material suitable for 14C dating, it can be impossible to obtain dates directly on skeletal materials. A small amount of carbonate occurs in hydroxyapatite, the mineral phase of bone and tooth enamel, and has been used as an alternative to collagen. Unfortunately, the mineral phase is often heavily contaminated with exogenous carbonate causing 14C dates to underestimate the true age of a sample. Although tooth enamel, with its larger, more stable crystals and lower porosity, is likely to be more robust to diagenesis than bone, little work has been undertaken to investigate how exogenous carbonate can be effectively removed prior to 14C dating. Typically, acid is used to dissolve calcite and etch the surface of the enamel, but it is unclear which acid is most effective. This study repeats and extends earlier work using a wider range of samples and acids and chelating agents (hydrochloric, lactic, acetic and propionic acids, and EDTA). We find that weaker acids remove carbonate contaminants more effectively than stronger acids, and acetic acid is the most effective. However, accurate dates cannot always be obtained.

Type
Research Article
Copyright
© The Author(s), 2021. Published by Cambridge University Press for the Arizona Board of Regents on behalf of the University of Arizona

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

Asscher, Y, Regev, L, Weiner, S, Boaretto, E. 2011. Atomic disorder in fossil tooth and bone mineral: an FTIR study using the grinding curve method. ArchéoSciences 35.CrossRefGoogle Scholar
August, S, Fleury, A, Fallon, S, Wood, R. in prep. The use of radiocarbon to assess the effeciency of pretreatment protocols on d13C analyses of tooth enamel.Google Scholar
Bacon, AM, Demeter, F, Duringer, P, Helm, C, Bano, M, Vu, TL, Nguyen, TKT, Antoine, PO, Bui, TM, Nguyen, TMH, et al. 2008. The late pleistocene duoi u’oi cave in northern vietnam: Palaeontology, sedimentology, taphonomy and palaeoenvironments. Quaternary Science Reviews 27(15–16):16271654.CrossRefGoogle Scholar
Bacon, AM, Westaway, K, Antoine, PO, Duringer, P, Blin, A, Demeter, F, Ponche, JL, Zhao, JX, Barnes, LM, Sayavonkhamdy, T, et al. 2015. Late Pleistocene mammalian assemblages of southeast Asia: new dating, mortality profiles and evolution of the predator-prey relationships in an environmental context. Palaeogeography, Palaeoclimatology, Palaeoecology 422:101127.CrossRefGoogle Scholar
Balter, V, Saliège, JF, Bocherens, H, Person, A. 2002. Evidence of physico-chemical and isotopic modifications in archaeological bones during controlled acid etching. Archaeometry 44(3):329336.CrossRefGoogle Scholar
Berry, EE, Baddiel, CB. 1967. The infra-red spectrum of dicalcium phosphate dihydrate (brushite). Spectrochimica Acta Part A: Molecular Spectroscopy 23(7):20892097.CrossRefGoogle Scholar
Bottero, MJ, Yvon, J, Vadot, J. 1992. Multimethod analysis of apatites in sound human tooth enamel. Eur J Mineral 4:13471357.CrossRefGoogle Scholar
Brock, F, Wood, R, Higham, TFG, Ditchfield, P, Bayliss, A, Ramsey, CB. 2012. Reliability of nitrogen content (%n) and carbon: Nitrogen atomic ratios (c:N) as indicators of collagen preservation suitable for radiocarbon dating. Radiocarbon 54(3–4):879886.CrossRefGoogle Scholar
Calo, A, Prasetyo, B, Bellwood, P, Lankton, JW, Gratuze, B, Pryce, TO, Reinecke, A, Leusch, V, Schenk, H, Wood, R, et al. 2015. Sembiran and pacung on the north coast of Bali: a strategic crossroads for early trans-asiatic exchange. Antiquity 89:378396.CrossRefGoogle Scholar
Castillo, CC. 2019. Preservation bias: Is rice overrepresented in the archaeological record? Archaeological and Anthropological Sciences 11(12):64516471.CrossRefGoogle Scholar
Cerling, TE. 1984. The stable isotopic composition of modern soil carbonate and its relationship to climate. Earth and Planetary Science Letters 71(2):229240.CrossRefGoogle Scholar
Cherkinsky, A. 2009. Can we get a good radiocarbon age from “bad bone”? Determining the reliability of radiocarbon age from bioapatite. Radiocarbon 51(2):647655.CrossRefGoogle Scholar
Corrêa de Araujo, A, Wesley Poling, G, de Magalhães Viana, PR. 2010. Apatite dispersants. In: Zhang, P, editor. Beneficiation of phosphates—technology advance and adoption. Littleton: Society for Mining, Metallurgy, and Exploration. p. 161167.Google Scholar
Cui, FZ, Ge, J. 2007. New observations of the hierarchical structure of human enamel, from nanoscale to microscale. Journal of Tissue Engineering and Regenerative Medicine 1(3):185191.CrossRefGoogle Scholar
Elliott, JC. 2002. Calcium phosphate biominerals. Reviews in Mineralogy and Geochemistry.CrossRefGoogle Scholar
Fallon, SJ, Fifield, LK, Chappell, JM. 2010. The next chapter in radiocarbon dating at the australian national university: status report on the single stage ams. Nuclear Instruments and Methods in Physics Research, Section B: Beam Interactions with Materials and Atoms 268(7–8):898901.CrossRefGoogle Scholar
Featherstone, JDB, Lussi, A. 2006. Undertanding the chemistry of dental erosion. In: Lussi, A, editor. Dental erosion. Basel: Karger. p. 6676.CrossRefGoogle ScholarPubMed
Fohlmeister, J, Voarintsoa, NRG, Lechleitner, FA, Boyd, M, Brandtstätter, S, Jacobson, MJ, Oster, L. J. 2020. Main controls on the stable carbon isotope composition of speleothems. Geochimica et Cosmochimica Acta 279:6787.CrossRefGoogle Scholar
Gordon, LM, Cohen, MJ, MacRenaris, KW, Pasteris, JD, Seda, T, Joester, D. 2015. Amorphous intergranular phases control the properties of rodent tooth enamel. Science 347(6223):746750.CrossRefGoogle ScholarPubMed
Haynes, V. 1968. Radiocarbon: analysis of inorganic carbon of fossil bone and enamel. Science 161(3842):687688.CrossRefGoogle ScholarPubMed
Hedges, R, Lee-Thorpe, JA, Tuross, NC. 1995. Is tooth enamel carbonate a suitable material for radiocarbon dating. Radiocarbon 37(2):285290.CrossRefGoogle Scholar
Hopkins, RJA, Snoeck, C, Higham, TFG. 2016. When dental enamel is put to the acid test: Pretreatment effects and radiocarbon dating. Radiocarbon 58(4):893904.CrossRefGoogle Scholar
Jacob, E, Querci, D, Caparros, M, Barroso Ruiz, C, Higham, T, Devièse, T. 2018. Nitrogen content variation in archaeological bone and its implications for stable isotope analysis and radiocarbon dating. Journal of Archaeological Science 93:6873.CrossRefGoogle Scholar
Koch, PL, Tuross, N, Fogel, ML. 1997. The effects of sample treatment and diagenesis on the isotopic integrity of carbonate in biogenic hydroxylapatite. Journal of Archaeological Science 24(5):417429.CrossRefGoogle Scholar
Korlević, P, Talamo, S, Meyer, M. 2018. A combined method for DNA analysis and radiocarbon dating from a single sample. Scientific Reports 8(1):41274127.CrossRefGoogle ScholarPubMed
La Fontaine, A, Zavgorodniy, A, Liu, H, Zheng, R, Swain, M, Cairney, J. 2016. Atomic-scale compositional mapping reveals mg-rich amorphous calcium phosphate in human dental enamel. Science Advances 2(9):e1601145.CrossRefGoogle ScholarPubMed
Lee-Thorp, J, Manning, L, Sponheimer, M. 1997. Problems and prospects for carbon isotope analysis of very small samples of fossil tooth enamel. Bulletin de la Societe Geologique de France 168(6):767773.Google Scholar
Lee-Thorp, JA. 1989. Stable carbon isotopes in deep time: the diets of fossil fauna and hominids [PhD thesis]. University of Capetown.Google Scholar
Lee-Thorp, JA, van der Merwe, NJ. 1991. Aspects of the chemistry of modern and fossil biological apatites. Journal of Archaeological Science 18(3):343354.CrossRefGoogle Scholar
Lee-Thorp, JA, van der Merwe, NJ, Brain, CK. 1989. Isotopic evidence for dietary differences between two extinct baboon species from Swartkrans. Journal of Human Evolution 18(3):183189.CrossRefGoogle Scholar
Makarewicz, CA, Sealy, J. 2015. Dietary reconstruction, mobility, and the analysis of ancient skeletal tissues: Expanding the prospects of stable isotope research in archaeology. Journal of Archaeological Science 56:146158.CrossRefGoogle Scholar
Millard, AR, Hedges, REM. 1996. A diffusion-adsorption model of uranium uptake by archaeological bone. Geochimica et Cosmochimica Acta 60(12):21392152.CrossRefGoogle Scholar
Naysmith, P, Scott, EM, Cook, GT, Heinemeier, J, van der Plicht, J, van Strydonck, M, Ramsey, CB, Grootes, PM, Freeman, SPHT. 2007. A cremated bone intercomparison study. Radiocarbon 49(2):403408.CrossRefGoogle Scholar
Pellegrini, M, Snoeck, C. 2016. Comparing bioapatite carbonate pre-treatments for isotopic measurements: Part 2—impact on carbon and oxygen isotope compositions. Chemical Geology 420:8896.CrossRefGoogle Scholar
Petrov, I, Šoptrajanov, B, Fuson, N, Lawson, JR. 1967. Infra-red investigation of dicalcium phosphates. Spectrochimica Acta Part A: Molecular Spectroscopy 23(10):26372646.CrossRefGoogle Scholar
Rey, C, Collins, B, Goehl, T, Dickson, IR, Glimcher, MJ. 1989. The carbonate environment in bone mineral: a resolution-enhanced fourier transform infrared spectroscopy study. Calcified Tissue International 45(3):157164.CrossRefGoogle ScholarPubMed
Rey, C, Renugopalakrishnan, V, Shimizu, M, Collins, B, Glimcher, MJ. 1991. A resolution-enhanced fourier transform infrared spectroscopic study of the environment of the CO3 2− ion in the mineral phase of enamel during its formation and maturation. Calcified Tissue International 49(4):259268.CrossRefGoogle ScholarPubMed
Roberts, P, Perera, N, Wedage, O, Deraniyagala, S, Perera, J, Eregama, S, Petraglia, MD, Lee-Thorp, JA. 2017. Fruits of the forest: human stable isotope ecology and rainforest adaptations in late Pleistocene and Holocene (∼36 to 3 ka) Sri Lanka. Journal of Human Evolution 106:102118.CrossRefGoogle ScholarPubMed
Roberts, P, Stewart, M, Alagaili, AN, Breeze, P, Candy, I, Drake, N, Groucutt, HS, Scerri, EML, Lee-Thorp, J, Louys, J et al. 2018. Fossil herbivore stable isotopes reveal Middle Pleistocene hominin palaeoenvironment in “Green Arabia”. Nature Ecology & Evolution 2(12):18711878.CrossRefGoogle Scholar
Roche, D, Ségalen, L, Balan, E, Delattre, S. 2010. Preservation assessment of miocene–pliocene tooth enamel from tugen hills (Kenyan Rift Valley) through FTIR, chemical and stable-isotope analyses. Journal of Archaeological Science 37(7):16901699.CrossRefGoogle Scholar
Ruppin, R, Englman, R. 1970. Optical phonons of small crystals. Reports on Progress in Physics 33(1):149196.CrossRefGoogle Scholar
Simmelink, J, Piesco, NP. 2001. Histology of enamel. In: Avery, JK, editor. Oral development and histology. New York: Thieme.Google Scholar
Simmelink, JW, Nygaard, VK, Scott, DB. 1974. Theory for the sequence of human and rat enamel dissolution by acid and by EDTA: a correlated scanning and transmission electron microscope study. Archives of Oral Biology 19(2):183197.CrossRefGoogle ScholarPubMed
Sønju Clasen, AB, Ruyter, IE. 1997. Quantitative determination of type a and type b carbonate in human deciduous and permanent enamel by means of fourier transform infrared spectrometry. Advances in Dental Research 11(4):523527.CrossRefGoogle ScholarPubMed
Storm, P, Wood, R, Stringer, C, Bartsiokas, A, De Vos, J, Aubert, M, Kinsley, L, Grün, R. 2013. U-series and radiocarbon analyses of human and faunal remains from Wajak, Indonesia. Journal of Human Evolution 64(5):356365.CrossRefGoogle ScholarPubMed
Stuiver, M, Polach, HA. 1977. Reporting of 14C data. Radiocarbon 19(3):355363.CrossRefGoogle Scholar
Surovell, TA. 2000. Radiocarbon dating of bone apatite by step heating. Geoarchaeology—An International Journal 15(6):591608.3.0.CO;2-K>CrossRefGoogle Scholar
Surovell, TA, Stiner, MC. 2001. Standardizing infra-red measures of bone mineral crystallinity: an experimental approach. Journal of Archaeological Science 28(6):633642.CrossRefGoogle Scholar
Sydney-Zax, M, Mayer, I, Deutsch, D. 1991. Carbonate content in developing human and bovine enamel. Journal of Dental Research 70(5):913916.CrossRefGoogle ScholarPubMed
Tuross, N, Fogel, ML, Hare, PE. 1988. Variability in the preservation of the isotopic composition of collagen from fossil bone. Geochimica et Cosmochimica Acta 52(4):929935.CrossRefGoogle Scholar
Ventresca Miller, A, Fernandes, R, Janzen, A, Nayak, A, Swift, J, Zech, J, Boivin, N, Roberts, P. 2018. Sampling and pretreatment of tooth enamel carbonate for stable carbon and oxygen isotope analysis. JoVE (138):e58002.CrossRefGoogle Scholar
Wood, R, Duval, M, Mai Huong, NT, Tuan, NA, Bacon, AM, Demeter, F, Duringer, P, Oxenham, M, Piper, P. 2016. The effect of grain size on carbonate contaminant removal from tooth enamel: towards an improved pretreatment for radiocarbon dating. Quaternary Geochronology 36:174187.CrossRefGoogle Scholar
Wood, RE, Barroso-Ruíz, C, Caparrós, M, Jordá Pardo, JF, Santos, BG, Higham, TFG. 2013. Radiocarbon dating casts doubt on the late chronology of the middle to upper palaeolithic transition in southern Iberia. Proceedings of the National Academy of Sciences of the United States of America 110(8):27812786.CrossRefGoogle ScholarPubMed
Xu, C, Reed, R, Gorski, JP, Wang, Y, Walker, MP. 2012. The distribution of carbonate in enamel and its correlation with structure and mechanical properties. Journal of Materials Science 47(23):80358043.CrossRefGoogle ScholarPubMed
Zazzo, A. 2014. Bone and enamel carbonate diagenesis: a radiocarbon prospective. Palaeogeography, Palaeoclimatology, Palaeoecology 416:168178.CrossRefGoogle Scholar
Zazzo, A, Lécuyer, C, Mariotti, A. 2004. Experimentally-controlled carbon and oxygen isotope exchange between bioapatites and water under inorganic and microbially-mediated conditions. Geochimica et Cosmochimica Acta 68(1):112.CrossRefGoogle Scholar
Zazzo, A, Saliège, JF. 2011. Radiocarbon dating of biological apatites: a review. Palaeogeography, Palaeoclimatology, Palaeoecology 310(1–2):5261.CrossRefGoogle Scholar
Supplementary material: File

Wood et al. supplementary material

Wood et al. supplementary material

Download Wood et al. supplementary material(File)
File 668.4 KB