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From desert ores to Middle Kingdom copper: elemental and lead isotope data from the RMAH collection, Belgium

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Abstract

This paper presents the first combined elemental composition and lead isotope (LI) ratio data for Middle Kingdom Egyptian copper alloy artefacts and significantly extends our knowledge on copper smelting remains from the Sinai Peninsula. It further provides the first precise LI ratio and trace element data for two Classic Kerma daggers. Forty-one samples have been analysed from artefacts housed at the Royal Museums of Art and History, Brussels. An important part of this assemblage consists of ore, “slag” and raw metal from workshops associated with 12th Dynasty mining expeditions in the southern Sinai Peninsula. These offer a unique insight into Middle Kingdom copper production chains and the associated waste materials, and form an essential reference group for provenance studies. The other part of the assemblage encompasses finished artefacts from different sites in Egypt—the first ever to be characterised for LI ratios for this period—as well as two daggers from Kerma, Nubia. This study illustrates the need for a careful approach to provenance research of early Egyptian metals, tailored to the particular technologies attested there. Based on the wide range of artefact LI ratios overlapping with those of arsenic-poor Sinai ores on the one hand, and the discrepancy in arsenic content between these ores and artefacts on the other hand, a two-step process for the production of arsenical copper alloys is identified. This suggests some technological continuity with respect to earlier pharaonic periods. The sources for primary copper production, however, likely changed over time: a narrower range of Sinai mines appears to have been exploited compared to preceding periods, and the recycling of circulating metal gained importance in the overall provisioning system.

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Notes

  1. For the Middle Kingdom, Shortland (2006) provides LI ratio data for kohl (a cosmetic, mostly galena) only, which have no bearing on the copper alloy production chain discussed here. The only published lead isotope ratios for Kerma (modern day Sudan) copper alloys were acquired by Young (1996) for two daggers by Q-ICP-MS (Quadrupole-Inductively Coupled Plasma-Mass Spectrometry) and are insufficiently precise for provenance analysis.

  2. Furthermore, XRD results for six ore samples published by Rademakers et al. (2018b) are included, which were not previously published. Malachite is confirmed as the major copper ore mineral, alongside clinoatacamite. The sulphide ores are mainly galena, with cerussite and anglesite as well as sphalerite (in adherence with their elemental composition). No material was available for XRD analysis of sample EA-MR-101 (sulphide E.04269).

  3. Its LI ratios equally match an Umm Bogma ore sample (Southern Sinai, mining area 45: Abdel-Motelib et al. 2012). This has, however, far lower lead content, making an Eastern Desert origin more likely.

  4. Abdel-Motelib et al. (2012) list the ore as deriving “from archaeological contexts”, without further details.

  5. Cobalt, manganese, nickel and zinc concentrations are loosely correlated.

  6. Although percentage levels of manganese are encountered in slag from Wadi Homr (ET-50/1), Bir Nasib (ET-51/1, ET-53/1), Wadi Nasib (ET-52/1), Wadi Ba'Ba (ET-57/1) and Wadi Nefoukh (ET-72/1).

  7. In contrast with iron, which may be partly reduced to its metallic state, manganese requires far more reducing conditions and its reduction into the metal phase is expected to be negligible (Hauptmann 2007). The slightly elevated trace contents observed in the raw copper prills may thus be attributed to minor MnO and/or MnS inclusions (which may be accompanied, i.a., by iron oxides or sulphides). Manganese concentrations are obviously much lower in the finished artefacts, as would be expected after removal (as dross) during crucible melting (and alloying).

  8. The contextual information for these artefacts is not provided by Vandier d'Abbadie and Michel (1972).

  9. For all three samples, an elevated barium concentration is measured. Notable Ba (and Sr, Ca and Mn) was already detected by HH-XRF—on the metal parts as well as the ivory. This suggests a barium contamination of the entire object, rather than barium being present in the metal. Barium was likely a component of the plaster used in the consolidation of the ivory handle, but unfortunately, no documentation of the artefact’s conservation history exists. Barium hydroxide is most commonly used in the consolidation of plaster and stone (e.g., Sierra-Fernández et al. 2017 and references therein), and sometimes iron; its application to organics or copper alloys is uncommon.

  10. Vercoutter et al. (1960) report the results of (qualitative) spectroscopy and metallography of another Kerma dagger, revealing a similar distinction between an alloyed (tin bronze) blade and unalloyed rivet.

  11. Although exploited for its intrinsic value (Lucas 1962), the possible use of turquoise as a copper ore in antiquity remains poorly explored. Future smelting experiments of turquoise in Ayn Soukhna type furnaces (cfr. Verly 2017; Verly et al. 2021) may illuminate this possibility.

  12. Exploitation at other periods cannot be excluded, however, as later activities may have obliterated earlier mining evidence. Nonetheless, currently available evidence does not suggest this.

  13. In this manuscript, we have adopted the spelling “Wadi Tarr”, although it is most commonly referred to as “Wadi Tar” in archaeological literature (e.g., Abdel-Motelib et al. 2012, Ilani and Rosenfeld 1994, Pfeiffer 2013, Rademakers et al. 2018b). Wadi Tarr lies in the southeastern part of the Sinai Peninsula (cfr. Fig. 1), as does Gebel Tarr. Gebel Tar, however, is situated in the western part of Sinai. To avoid confusion, the spelling used in the topographical maps published by The Survey of Egypt (1935), upon which the maps presented in this paper are based, is followed here.

  14. More specifically samples 225 (Sheikh Awad), ET-1/6, ET-1/7, ET-1/8 (Sheikh Mukhsen), ET- 51/1, ET-53/1 (Bir Nasib I), ET-50/1 (Homr) and ET-59/3 (Serabit el-Khadim). Note that analysis methods vary and dating is not consistently specified for these samples, cfr. Pfeiffer 2013.

  15. With respect to the Kahun material, Gilmore (1986) notes that “If these particular ore samples are indeed representative of the local copper ores we would have to conclude either that the metals were not made from local ores or that arsenic was deliberately added in some way. Alternatively we can suggest that these items were indeed imported from areas where arsenic is a natural companion of copper”.

  16. For this Kerma blade, the lowest lead and sulphur contents are associated with the lowest arsenic content. This may suggest the use of the same copper for the different parts, but alloyed for specific parts, whereby the alloying introduced an important shift in LI ratios. On the other hand, the use of different copper sources may be attested, either in a single workshop or as a result of repair elsewhere, perhaps at a later time.

  17. Antimony contents exceeding 100 μg/g are not measured in pure copper, whereas elevated antimony contents (200 up to 1000 μg/g) are associated with percentage levels of arsenic (not all artefacts are well dated and trace elements are not reported for each artefact).

  18. Rademakers et al. (2018b) report silver levels mostly below 50 μg/g (with the exception of one Protodynastic artefact from Faras (55 μg/g) and two Old Kingdom artefacts from Qau el-Kebir (55–145 μg/g)), while Kmošek et al. (2018) report higher silver contents for these earlier periods (50–1200 μg/g). This may be due to minor silver loss during digestion (less than 20%, cfr. analytical procedure in Rademakers et al. (2020: Online Supplementary Materials)) for ICP-OES (vs. NAA) and, probably more importantly, variable silver concentrations in these early artefacts. In each dataset, a weak Ag-As-Sb correlation can be noted.

  19. It is not possible to exclude formally Anatolia as a potential source of imported metal for all samples, although the majority fall outside of the ranges defined for Anatolian ores (Hirao et al. 1995; Sayre et al. 2001; Seeliger et al. 1985; Wagner et al. 1985, 1986, 2003; Yener et al. 1991), in particular with respect to their 207Pb/204Pb ratio. Of course, there are some LI ratio overlaps between the assemblage presented here and those ores (more specifically, for the samples with relatively higher 206Pb/204Pb ratios). However, these mainly concern the ore samples (which were mined in Sinai beyond any reasonable doubt) and four copper alloys which closely resemble those ores (two are scrap from the same workshops). Furthermore, the distribution of this Middle Kingdom assemblage cross-cuts the LI ranges defined by different Anatolian ore deposits, rather than overlapping with one particular deposit. All of these factors indicate that the (majority of) finds presented here are unlikely related to an Anatolian ore deposit. Even if an Anatolian origin cannot be formally excluded for one or two copper alloys, their consistency with the rest of the presented material argues against this.

  20. Petrie (1890, p. 38) notes the occurrence of orpiment (As2S3) at Gurob during the New Kingdom, where the presence of copper ore and slag in a crucible leads him to suggest that “smelting was done in the town”. The listing of other minerals such as hematite and green feldspar along with orpiment (it is unclear whether they belong to the same context) does not allow for a conclusion as to its possible use as a pigment or within a metallurgical context. Orpiment is indeed considered a common pigment used during the New Kingdom, but has been discovered already in Middle Kingdom contexts (e.g., Lee and Quirke 2000), and was traded as a raw material during the Late Bronze Age (e.g., Uluburun cargo: Bass 1986). Other arsenic sulphide minerals include realgar (As4S4) and arsenopyrite (FeAsS). Arsenic-rich minerals noted at Wadi Tarr include koutekite (Cu5As2) and domeykite (Cu3As) (Ilani and Rosenfeld 1994).

  21. Umm Semiuki in the Eastern Desert might have presented an alternative source. Mainly considered to be a silver source from modern geological perspective (Shalaby et al. 2004), secondary deposits in the upper oxidation zone appear to have been exploited for copper production at some point in antiquity (El Shazly and Afia 1958; Hume 1937; Lucas 1962; Pfeiffer 2013), but evidence has been destroyed by modern mining according to Klemm and Klemm (2008). Lucas (1962, p. 236— referring to Hume (1937, pp. 837–842)) describes it as an important mining site for copper, with “extensive ancient workings with several shafts. At the surface, the ore is malachite and azurite, of which there is a thickness of about seven metres and below this are copper and zinc sulphides and lead ore … There are also ore crushers, pottery (possibly broken crucibles) and slag. These are the most important deposits of copper ore yet discovered in Egypt, some of the workings being 40 to 50 feet underground”. While arsenic-bearing sulphides such as tennantite are described by Shalaby et al. (2004), it is unclear to which extent arsenic is present in the surface deposits. Silver, antimony, arsenic and particularly zinc might be present to some degree in the malachite/azurite, but no elemental or LI data are available (El Shazli and Afia mention only possible zinc enrichment—LI ratios determined for the primary Precambrian Cu/Pb/Zn ore by Stos-Fertner and Gale (1979) have expectedly low 206-207-208Pb/204Pb ratios). Whether copper-arsenic alloys could be directly smelted from this deposit or an arsenic alloying agent was extracted is unclear but appears unlikely (rather, copper with high levels of zinc is expected: Afia 1985). As for Wadi Tarr, the extent and timing of ancient exploitation of this deposit cannot be assessed confidently.

  22. Hauptmann (2007) similarly dismisses Wadi Tarr as a source for arsenical copper objects in the Southern Levant. While this may very well be true, this argument is equally based on the premise that arsenical copper was produced directly from Wadi Tarr ores, rather than by alloying with (other) copper (resulting in mixed LI ratios).

  23. Only Nabi Salah ore sample 48 has an elevated (2600 μg/g) tin level (Beit Arieh 2003), but no LI ratios are available.

  24. Tin contents in some Sinai copper finds summarised by Pfeiffer (2013) are comparable, but their dating is unclear and not all elements (e.g., arsenic) are consistently reported on, making it difficult to differentiate possible alloys.

  25. At least those characterised by Rademakers et al. (2018b)—tin contents exceeding 500 μg/g occur in a few artefacts presented by Kmošek et al. (2018), but are not further discussed there.

  26. Raw copper itself may further reflect different ores mixed in a single smelting batch.

  27. Many of the analysed artefacts from Tell el-Dab’a date to the (transition to the) Second Intermediate Period, which is characterised by a fast succession of kings, often described in ancient texts as a period of chaos. The organisation of metal production by the state may have changed significantly at that time. Furthermore, the 12th Dynasty material at Tell el-Dab’a shows strong connections with Syro-Palestine, including metalwork of Syro-Palestinian styles, and there is significant settlement by west Asian population during the 13th Dynasty (Philip 2006, p. 27), suggesting possibly different metal provisioning systems at this Delta site. Overall, Philip (2006, p. 228) notes a relative paucity of metals from the Middle Kingdom strata: possibly, “the issue and recycling of metal tools was more closely controlled during the Middle Kingdom”, although other factors probably play into the observed pattern as well. Arsenic appears in similar concentrations (0.1–3%) in artefacts dated to later strata, in some cases accompanied by tin in variable levels (trace to percentage level), in other cases as a pure arsenical copper alloy. This validates the gradual replacement of arsenic by tin in bronze, as suggested by the data presented here. Philip (2006, p. 211) views arsenic as an ore contaminant, not actively sought (or even recognised) by the Tell el-Dab’a metalworkers (except for chisel 6110). It is, however, difficult to discuss the levels of arsenic here without LI ratio data, as the arsenic concentrations of the relevant source materials should be assessed (as for the low tin concentrations). Philip (2006, p. 215) notes that “the presence of tin, at well below optimum levels, in some of the artefacts from Tell el-Dab’a certainly points towards a degree of recycling”.

  28. Exceptions exist, such as two tin bronzes from the 2nd Dynasty Tomb of Khasekhemwy (Cowell 1987—these can be considered “ternary bronzes”, with ca. 0.5–1% arsenic content) and a Predynastic to Old Kingdom tin bronze from Buto (Pernicka and Schleiter 1997). Without lead isotope analysis, it is not possible to verify if these represent imports or rather early examples of tin alloying in Egypt.

  29. Low tin concentrations are often interpreted as a sign of recycling (e.g., Maddin et al. 2003; Pernicka 2014). Gilmore (1986) equally interprets low tin contents in Middle Kingdom Kahun alloys as a possible result of mixing scrap bronze alloys.

  30. The changing stock may equally be reflected in other materials. The idea to trace copper sources in Egyptian Blue was presented by Jaksch et al. (1983) for the New Kingdom, and by Schiegl et al. (1990) for the Old Kingdom up to the Roman period. They suggest that the chronological distribution of arsenic, tin and lead in copper-based pigments may allow for a more accurate dating of changes in Egyptian bronze technology. Rademakers et al. (2017) highlight this relation between New Kingdom pigments and circulating copper alloys in terms of LI ratios.

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Acknowledgements

This research was conducted in the framework of the Egyptian and African copper metallurgy project (EACOM) funded by the Belgian Science Policy (BELSPO) BRAIN-BE programme BR/143/A3/EACOM. Additional funding was provided by the KU Leuven Centre for Archaeological Sciences (CAS). We would like to thank the entire EACOM team for their collaboration, and in particular Charlotte Doyen and Hugues Paridans. We further thank our colleagues at the RMAH, especially the late Dirk Huyge, curator for the Prehistoric and Early Dynastic Egypt collection, Isabelle Therasse and Nathalie Halgand. We wish to thank Ayn Soukhna’s excavation directors Pierre Tallet and Claire Somaglino, as well as Damien Laisney for his very precious help with the topography. We are grateful to Elvira Vassilieva and Nancy Weyns for their help in the sample preparation, ICP-OES and XRD analyses at KU Leuven. We thank Kris Latruwe for performing quantitative Pb determination using ICP-MS and Pb isotopic analysis using MC-ICP-MS at Ghent University. FR would like to thank Barry Kemp for pointing out Charles’ publication of the probable speiss find at Amarna, and Myrto Georgakopoulou for discussing the evidence from Dhaskalio. We are very grateful to the editor and two anonymous reviewers for their constructive comments which have helped to further improve this paper.

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  1. KU Leuven, Earth and Environmental Sciences, Celestijnenlaan 200e, 3001, Leuven, Belgium

    Frederik W. Rademakers & Patrick Degryse

  2. Royal Museums of Art and History, 10 Parc du Cinquantenaire, 1000, Brussels, Belgium

    Georges Verly & Luc Delvaux

  3. Department of Analytical Chemistry, Ghent University, Krijgslaan 281 - S12, 9000, Gent, Belgium

    Frank Vanhaecke

  4. Faculty of Archaeology, Leiden University, Einsteinweg 2, 2333, CC, Leiden, The Netherlands

    Patrick Degryse

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  1. Frederik W. Rademakers
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Rademakers, F.W., Verly, G., Delvaux, L. et al. From desert ores to Middle Kingdom copper: elemental and lead isotope data from the RMAH collection, Belgium. Archaeol Anthropol Sci 13, 100 (2021). https://doi.org/10.1007/s12520-021-01329-w

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