# Continuity of lead-silver production in the area of Cartagena-La Unión (Spain) after the Phoenician trade crisis of the 6th century BC

Céline Tomczyk, Christophe Petit, María Berná, Laurent Costa, Jessica

Legendre, Jesús Moratalla, Sidonie Révillon, Pierre Rouillard

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Céline Tomczyk, Christophe Petit, María Berná, Laurent Costa, Jessica Legendre, et al.. Continuity of lead-silver production in the area of Cartagena-La Unión (Spain) after the Phoenician trade crisis of the 6th century BC. Journal of Archaeological Science: Reports, 2024, 59, pp.104742. 10.1016/j.jasrep.2024.104742. halshs-04718691

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# Continuity of lead-silver production in the area of Cartagena-La Unión (Spain) after the Phoenician trade crisis of the 6th century BC

Céline Tomczyk<sup>a, *</sup>, Christophe Petit<sup>a</sup>, María Berná<sup>b</sup>, Laurent Costa<sup>c</sup>, Jessica Legendre<sup>d</sup>, Jesús Moratalla<sup>e</sup>, Sidonie Révillon<sup>f</sup>, Pierre Rouillard<sup>c</sup>

## ARTICLE INFO

### Keywords:

- Litharge

- Metallurgy

- Lead isotopes

- Commercial crisis

- Phoenician

## ABSTRACT

The 6th century BCE is marked by major changes in the Mediterranean trade routes. These changes had a significant impact on the production of silver-lead in the Iberian Peninsula, which was previously thought to have come to an abrupt end.

However, the study of litharge from the early 5th century BCE to the first half of the 3rd century BCE, from three sites in the Alicante region, demonstrates that the types, textures and compositions of litharge remain unchanged after the crisis in Phoenician trade. Thus, although no production workshops have been found in the Cartegena mining district, it is possible to affirm that the cupellation processes used at the beginning of the first millennium BCE continued until the 3rd century BCE.

Lead isotopic analysis of the litharge and two lead artefacts indicate that they come from ores from the very rich mines of Cartagena-La Unión, which were extensively exploited between the 8th and 6th centuries BCE.

Despite a major decline in mining and metallurgical production and considerable changes in the networks of exchange in the Mediterranean, the same production chain persisted from lead extraction to the type of metallurgy practised. The economic crisis does not therefore lead to a cessation of production, but the quantity of lead (and silver) produced would probably be significantly lower.

## 1. Introduction

Throughout the first millennium BCE, the Iberian Peninsula was the site of rich and complex interactions between indigenous, Phoenician, Greek, Carthaginian and later Roman populations (see in particular Abad Casal, 1992; Momrak, 2005; Díaz, 2015; Albelda, 2018; Rouillard, 2023).

The coastal regions of the eastern Iberian Peninsula witnessed extensive agricultural production, as evidenced by significant deforestation as early as the 9th century BCE (Pappa, 2015). Pollen records indicate a specialisation in large-scale cereal, oil, wine (Buxó, 2008) and fruit production (Pérez-Jordà et al., 2017). These agricultural activities were sometimes associated with other activities, particularly mining (Pérez-Jordà et al., 2023), especially of lead-silver. The importance of

metallurgical activity was so important in the early first millennium BC that lead contamination of Phoenician-Iberian origin (~1100–800 BCE) and later of Roman origin has been detected in Greenland ice cores (McConnell et al., 2018).

However, the flourishing maritime trade from the Iberian Peninsula to the eastern Mediterranean declined in the second half of the 6th century BCE during a Phoenician trade crisis, leading to the abandonment of numerous sites in the Iberian Peninsula (Aubet, 1995; Ruiz, 2007; Puckett, 2012; Díaz, 2015; Murillo-Barroso et al, 2016). The real impact of this economic crisis remains uncertain. It could manifest itself in a severe recession (Shefton, 1995; Dietler and López-Ruiz, 2009 p.4–49) or even lead to political collapse and the overthrow of the current elites (Rothenberg and Blanco-Freijeiro, 1981; Díaz, 2015).

It was not until the arrival of the Romans, at the beginning of the 2nd

<footnote><sup>a</sup> Université Paris 1 Panthéon-Sorbonne, UMR 7041 ArScAn, équipe archéologies environnementales, France</footnote>

<footnote><sup>b</sup> Museo Histórico de Aspe, Spain</footnote>

<footnote><sup>c</sup> CNRS, UMR 7041 ArScAn, équipe mondes grecs archaïques et classiques, France</footnote>

<footnote><sup>d</sup> Ministère de la Communication et de la Culture, Centre de recherche et de restauration des musées de France (C2RMF), France</footnote>

<footnote><sup>e</sup> Universidad de Alicante, Spain</footnote>

<footnote><sup>f</sup> Laboratoire SEDISOR, UMR 6538 Géosciences Océan, France</footnote>

<footnote>* Corresponding author.</footnote>

<footnote>E-mail address: celine.tomczyk@cnrs.fr (C. Tomczyk).</footnote>
century BCE, that lead-silver production resumed on a massive scale in Iberia. At that time, the entire southwestern territory of the peninsula was exported to Rome and underwent a political, socio-economic and cultural reorganisation (Keay, 2003; Myers, 2016).

## 2. Successive phases of intensive exploitation and mining decline in the Alicante region

The Cartagena-La Unión mining area, which is 23 km long and 6.5 km wide, is located in the extreme west of the Murcia region (Spain), amidst gently rolling terrain bordering the Mediterranean coast. Several phases of mineralisation have been identified within these mines, but the dominant facies corresponds to a stratiform deposit within Triassic limestones. Silver-bearing galena (±sphalerite) is intercalated within thin bands of calcite and dolomite (Andreazini et al., 2015). The most significant mineralised veins can reach thicknesses of up to 10 m and have the highest lead concentrations in the Iberian Peninsula (Oen et al., 1975). The richness of these deposits, together with their geographical location, which facilitated the export of products via coastal sea routes, contributed to the establishment of the mines of Cartagena-La Unión as a leading mining district from the prehistoric period until their mass exploitation in the 20th century (Vilar, 1986; Rico et al., 2009).

### 2.1. Periods of intensive exploitation between the 8th and 6th centuries BCE and during the Roman period

These mines are mainly known for their intensive exploitation between the 2nd century BCE and the 1st century CE, during the Roman period (Domergue, 1990; Caparros and del Carmen, 1999; Marín et al., 2010; Fabre et al., 2014; Rico et al., 2018). Lead ingots from Cartagena were exported throughout the Mediterranean during this period (Trincherini et al., 2009; Clemenza et al., 2017; Domergue and Rico, 2024).

However, while the importance of this ancient exploitation is

undeniable, recent discoveries also reveal an earlier phase of intense lead exploitation between the 8th and the second half of the 6th century BCE. The ore from the Cartagena mines was then processed in workshops located close to the coast, less than 100 km from the mines (Fig. 1). Three Phoenician smelting workshops have been discovered:

- at La Fonteta (with smelting activity probably between 800 and 550 BCE (Renzi et al., 2009) but with occupation until the end of the 6th century (Rouillard et al., 2007))

- at Cabezo Pequeño del Estaño (750–650 BCE, Prados Martínez et al., 2018)

- at Punta de los Gavilanes (700–600 BCE, Polzer, 2014).

The presence of a fourth workshop is suspected, as paleopollution identified at the Laguna de Río Seco site suggests extractive lead metallurgy between 1550 and 550 BCE (García-Alix et al., 2013).

While Roman production was usually exported in the form of ingots, Phoenician lead was not typically exchanged in this way, but more often directly as galena or litharge. Litharges are an intermediate stage in lead-silver metallurgy. The reductive smelting of silver-bearing lead ores generates slag and bullion lead. A litharge is formed when this bullion lead is cupelled to separate the silver which is released in liquid metallic form, from the lead (which is then retained in the litharge). The reducing fusion of this litharge produced lead in metallic form.

Ships passed through along the Alicante region loaded with several tonnes of lead, as evidenced by two 7th century BCE shipwrecks discovered off the coast of the lead reduction workshop at Punta de los Gavilanes (Negueruela et al., 2004; Polzer, 2014). The first shipwreck, discovered at Bajo de la Campana, was loaded with over a ton of non-argentiferous galena from Almería (Polzer, 2014) in the form of 10,000 fragments (Polzer, 2012), accompanied by goods of exotic origin (copper and tin ingots, bronze furniture, amber and ivory (Ruiz Cabrero and Mederos Martín 2004; Nantet, 2016 p. 277–279). The second shipwreck, called Mazarrón 2, carried Phoenician amphorae and almost

<figure><img src="image_3.png" /><figcaption>Fig. 1. Lead(-silver) smelting workshops during the Phoenician period and sites studied in this study.</figcaption></figure>
three tonnes of litharges made from lead mined in the Cartagena mining district (Renzi et al., 2009).

The Phoenician coastal navigation system (Renzi et al., 2009; Tejedor, 2018) allowed the spread of lead from Cartagena along the Spanish coasts (Murillo-Barroso et al, 2016). This trade was undoubtedly crucial as lead was used, among other things, to extract silver from jarosites mined in the south of the Iberian Peninsula (Craddock, 2014; Murillo-Barroso et al, 2016). Lead exports to Rio Tinto's mines to extract silver from jarosites were organised as early as the 11th-9th centuries BC (Wood and Montero-Ruiz, 2019) and intensively between the 8th and 7th centuries BC (Neville, 2007 p. 140-141; Kaufman et al., 2016).

Between the 7th and 6th centuries BCE, lead from the Cartagena mines also reached the island of Ibiza, 250 km away. Indeed, isotopic analysis of lead show that lead from Cartagena was smelted there alongside local ores (Ramon Torres et al., 2011).

Silver production from various sites in the Iberian Peninsula was traded throughout the Mediterranean until the 7th century BCE, as demonstrated by isotopic analysis of silver artefacts from the easternmost Mediterranean (Eshel et al., 2019; Wood et al., 2019).

## 2.2. Few discoveries in the 5th-3rd centuries BC

While it is undisputed that production and export were highly significant before the 7th century BCE, to date, there is little evidence of Iberian mining activity after this period.

In the 6th century BCE, mines in Ibiza ceased activity (Ramon Torres et al., 2011), as did those in Catalonia (Rafel et al., 2010) and Rio Tinto (Fernández Jurado, 1993; Pérez Macías, 1999). Many smelting sites related to the extraction of silver from jarosites also ceased operations during this century (Rothenberg and Blanco-Freijeiro, 1981; Anguilano, 2012; Wood and Montero-Ruiz, 2019). The very limited quantity of silver artifacts discovered in the Iberian Peninsula for the following centuries (5th-3rd centuries BCE) seems to suggest that silver production shifted towards the eastern Mediterranean (Murillo-Barroso et al, 2016).

In the region of Alicante, discoveries of litharges after the 6th century BCE are also very rare, and no metallurgical workshops have yet been discovered. The question of mining remains open. The discovery of rare ceramics dated between 500 and 300 BCE in some mine workings (Domergue, 1987; Salvador, 2012; Bellón Aguilera, 2013) and of litharges cakes and cupels dated from 400 BCE at Punta de Gavilanes (Ros Sala, 1993; Ros Sala et al., 2003) suggest that the Cartagena-La Unión mines may have been exploited. This exploitation, if it took place, would have been of very low intensity: a recent study of palaeopollution in the Bay of Cartagena highlights that anthropogenic lead contamination is barely detectable from around the 6th century BCE until the intense resumption of mining activities in the Roman period (Ortiz et al., 2021).

## 3. Materials and methods

Our study aims to test whether some lead was indeed produced in the Cartagena mining district between the crisis in Phoenician trade and the Roman mining revival. To this end, litharges from sites dating between the 5th and 3rd centuries BCE were analysed in order to define their composition and deduce their geographical origin. Two lead artefacts from the 5th century BCE were also analysed using EDS (SEM) and lead isotopes to determine whether they were derived from the smelting of the litharges studied (Table 1).

All the material studied comes from the Alicante region, from three sites located approximately 80 km north of the Cartagena mines.

The first of these, El Oral (San Fulgencio, Alicante) is an Iberian settlement located on the north bank of the Segura, 7 km from its mouth. The litharge fragments were found in a dwelling house (first half of the 5th century BCE), in an open-air room, mixed with iron slag, next to a stone anvil. This room probably served as a small metalworking workshop (Casal and Sellés, 1993; Mira, 2001). The second site, Las Tres Hermanas (Aspe, Alicante), is an Iberian settlement dated to between

<caption>**Table 1**</caption>

List of sites from which the archaeological material analysed came. Their dating is based on chrono-typological studies of ceramics.

<table><thead><tr><td>Site</td><td>Datation</td><td>Material</td></tr></thead><tbody><tr><td>El Oral: San Fulgencio</td><td>First half of the 5th century BCE</td><td>litharge, lead ingot</td></tr><tr><td>Las Tres Hermanas</td><td>late 5th – middle of the 4th century BCE</td><td>litharges, shapeless</td></tr><tr><td>Campello: La Illeta dels Banyets</td><td>end of 4th – first half of 3rd century BCE</td><td>lead artifact</td></tr></tbody></table>

the end of the 5th century BCE and the middle of the 4th century BCE. A pile of litharge cakes was found in a sloping area, against the wall of a house, but no specific structure was identified (Moratalla Jávega et al., 2023). Finally, the site of La Illeta dels Banyets, in El Campello (Alicante), occupies a small coastal island that has seen various phases of occupation (Bronze Age, Iberian, late Roman). The litharges were recovered from an artisanal facility linked to fishing, in a space dedicated to storage, with no other metallurgical elements. The level has been dated to the late 4th-early 3rd century BCE (Olcina Doménech et al., 2009).

EDS analysis were carried with a Zeiss EVO 10 scanning electron microscope (SEM) on several distinct samples to determine their composition and identify any mineral phases present. Measurements were made on a sawn, flattened surface at an acceleration voltage of 20 kV and a working distance of approximately 8.5 mm.

Lead isotope analyses were then carried out by MC-ICP-MS at the Sedior laboratory to determine the origin of the material studied.

## 4. Results

### 4.1. Chemical composition and typology of the material examined

#### 4.1.1. Macroscopic appearance

The litharge cakes come from archaeological contexts dating from after the 6th century BCE. They have similar dimensions, with diameters ranging from 21 to 28 cm and thicknesses not exceeding 2 cm. They have a thin crust of cream-coloured surface alteration. When freshly fractured, their textures are quite similar: they show a more or less laminar structure characterised by parallel bands of whitish minerals and visible greyish spheres homogeneously dispersed in a red-orange matrix (Fig. 2). The most porous portions of the litharges are richer in lead metallic beads.

It is noteworthy that the diameter of the litharges studied corresponds to that of the litharges from the Mazarrón 2 shipwreck, dated to the 7th century BCE (Negueruela et al., 2004) and that the texture and thickness of these litharges are similar to those of the small fragments found in the La Fontena workshop, dated to the 8th to mid-6th century BCE (Renzi et al., 2009).

#### 4.1.2. Chemical composition of the litharge

The presence of silver metal beads on the surface of the litharge cakes indicates a cupellation process (in the case of the litharge from El Oral, the presence of 0.49 % silver had already been noted by Abad Casal and Sellés (1993 p. 265). Analysis not identify the presence of silver in the matrix of the litharge, indicating the efficiency of the separation of lead and silver (with silver present only on the surface).

The composition of the litharge matrices is very homogeneous (Tables 2, 3 and 4) and the litharges from the three sites studied are similar. They have high lead (Pb) contents, ranging from 55 to 68 %.

The lead oxide matrix is always accompanied by silicified calcium carbonates (CaCO3 ± Si,Al) corresponding to the whitish elements sometimes visible to the naked eye (Fig. 3). Pure lead beads (corresponding to the metallic beads also visible to the naked eye) are abundant in the porosities.

The chemical composition of litharge explains the metallurgical
<figure><img src="image_4.png" /><figcaption>**Fig. 2.** Plan view, left: macroscopic appearance of litharge cakes from Las Tres Hermanas; cross-section, right: top – sawn surface of a porous litharge (Las Tres Hermanas), middle – highly altered surface of a non-porous litharge (Las Tres Hermanas), bottom – a fragment of litharge (altered surface) from the Campello site (La Illeta dels Banyets).</figcaption></figure>

<table><caption>**Table 2**

EDS SEM analysis of Las Tres Hermanas litharges (averages over 6 analyses per sample).</caption><thead><tr><th>Element</th><th>C</th><th>O</th><th>Al</th><th>Si</th><th>Pb</th><th>Ca</th><th>Comment</th></tr></thead><tbody><tr><td rowspan="3">Weight %</td><td>6.97</td><td>20.20</td><td>2.39</td><td>4.66</td><td>55.41</td><td>10.38</td><td>Sample L1 TH, non-porous</td></tr><tr><td>4.78</td><td>19.49</td><td>0.77</td><td>3.03</td><td>59.56</td><td>11.63</td><td>Sample L2 TH, non-porous</td></tr><tr><td>5.11</td><td>20.28</td><td>1.11</td><td>1.62</td><td>63.57</td><td>8.20</td><td>Sample L3 TH, porous</td></tr><tr><td>Margin of error</td><td>9 %</td><td>10 %</td><td>9–11 %</td><td>8–6 %</td><td>2.5 %</td><td>5.5–12 %</td><td></td></tr></tbody></table>

<table><caption>**Table 3**

EDS SEM analysis of litharges found at Campello (sample L CA, average of 6 analyses).</caption><thead><tr><th>Element</th><th>C</th><th>O</th><th>Al</th><th>Si</th><th>Pb</th><th>Ca</th></tr></thead><tbody><tr><td>Weight %</td><td>4.16</td><td>15.76</td><td>1.54</td><td>2.81</td><td>67.5</td><td>8.23</td></tr><tr><td>Margin of error</td><td>9.18 %</td><td>11.63 %</td><td>13.38 %</td><td>9.26 %</td><td>3.40 %</td><td>9.24 %</td></tr></tbody></table>

<table><caption>**Table 4**

EDS SEM analysis of El Oral litharges (sample L EO, average of 6 analyses).</caption><thead><tr><th>Element</th><th>C</th><th>O</th><th>Al</th><th>Si</th><th>Pb</th><th>Ca</th></tr></thead><tbody><tr><td>Weight %</td><td>3.08</td><td>22.71</td><td>1.21</td><td>2.03</td><td>59.63</td><td>11.22</td></tr><tr><td>Margin of error</td><td>10.62 %</td><td>11.22 %</td><td>16.88 %</td><td>12.03 %</td><td>4.52 %</td><td>8.37 %</td></tr></tbody></table>

process employed. A mixture of lead and silver (bullion lead) is melted in a circular reactor about 25 cm in diameter. The lining of the reactor is porous and rich in calcium. It absorbs the lead by capillarity, while the silver (in metallic form) remains on the surface. The process used corresponds to a classical cupellation process (see, for example, *Izquierdo De Montes, 1997; Bayley and Eckstein, 2006; Martinón-Torres et al., 2008; L'Héritier et al., 2015; Moureau and Thomas, 2016*), but the

striking fact here is that the size and the composition of the litharges found at the three sites studied are almost identical.

Finally, the SEM (EDS) analysis of a small, highly altered lead ingot found at El Oral (Fig. 4) and a small drop of shapeless lead (approximately 1 cm wide by 3 cm high) found among the litharge fragments at Las Tres Hermanas indicate that they are composed of pure lead. This again emphasises the effective separation of lead and silver during the cupellation process.

The litharges from the three sites investigated are similar in type, texture and composition. They originate from the same type of cupellation process, probably using ceramic vessels of similar shape.

## 4.2. Identification of the origin of the lead

Although the lead-silver ore deposits of Cartagena are the closest to the sites, and the litharges have textures similar to those produced from lead from Cartagena one to two centuries earlier (Renzi et al., 2009), it cannot be ruled out that the lead contained in these litharges has other, much more distant, sources. These analyses show a very strong similarity of signatures, confirming the hypothesis of a common origin for these artefacts (Table 5).

Several hypotheses of provenance must be considered:

- The first is a local, i.e. Iberian, origin;
<figure><img src="image_5.png" /><figcaption>Fig. 3. On the left, texture and structure of a litharge: the bands of whitish minerals visible with the naked eye correspond to calcium carbonates (slightly silicified) organised in large bands, but also to small crystals (dark in EDS) interspersed in the PbO matrix; on the right, presence of pure lead beads (corresponding to the beads visible with the naked eye) in the porosity of the litharge (EDS).</figcaption></figure>

<figure><img src="image_6.png" /><figcaption>Fig. 4. Lead ingot analysed (weight 8.5 g).</figcaption></figure>

**Table 5**

Lead isotope analyses carried out as part of this study, results NIST 981 standardised.

<table><thead><tr><th>Site</th><th>ID</th><th>Description</th><th><sup>206</sup>Pb/<sup>204</sup>Pb</th><th>2σ</th><th><sup>207</sup>Pb/<sup>204</sup>Pb</th><th>2σ</th><th><sup>208</sup>Pb/<sup>204</sup>Pb</th><th>2σ</th></tr></thead><tbody><tr><td>Las Tres Hermanas</td><td>L1 TH</td><td>Litharge</td><td>18,7175</td><td>0,0004</td><td>15,6805</td><td>0,0005</td><td>39,0188</td><td>0,0016</td></tr><tr><td>Las Tres Hermanas</td><td>L2 TH</td><td>Litharge</td><td>18,7067</td><td>0,0012</td><td>15,6851</td><td>0,0009</td><td>39,0320</td><td>0,0124</td></tr><tr><td>Las Tres Hermanas</td><td>L3 TH</td><td>Litharge</td><td>18,7045</td><td>0,0012</td><td>15,6845</td><td>0,0008</td><td>39,0283</td><td>0,0114</td></tr><tr><td>Las Tres Hermanas</td><td>18 TH</td><td>Pb artefact</td><td>18,7069</td><td>0,0008</td><td>15,6824</td><td>0,0007</td><td>39,0229</td><td>0,0112</td></tr><tr><td>El Oral</td><td>L EO</td><td>Litharge</td><td>18,7071</td><td>0,0014</td><td>15,6850</td><td>0,0011</td><td>39,0325</td><td>0,0132</td></tr><tr><td>El Oral</td><td>P EO</td><td>Pb ingot</td><td>18,7080</td><td>0,0008</td><td>15,6792</td><td>0,0007</td><td>39,0156</td><td>0,0134</td></tr><tr><td>Campello</td><td>L CA</td><td>Litharge</td><td>18,6943</td><td>0,0015</td><td>15,6792</td><td>0,0011</td><td>39,0026</td><td>0,0141</td></tr></tbody></table>

- The second is from the Aegean region, where numerous lead-silver mines were in operation in the Cyclades, on the island of Thasos or in the Laurion area (Pernicka et al., 1981; Jones, 1982; Weisgerber and Pernicka, 1995; Mussche, 2006; Papadopoulou, 2011);

- The third hypothesis is Sardinian; indeed, lead-silver metallurgy workshops have been discovered in the Montevecchio mining basin in the south of the island (Caro et al., 2013);

- The last is Anatolian (Taurus Mountains), although the lead-silver exploitations are poorly dated (Pitarakis, 1998).

Bivariate plots normalised to the stable isotope ($^{204}$Pb) clearly show that a Sardinian origin can be rejected (the $^{206}$Pb/$^{204}$Pb ratios from these deposits are too low); the hypothesis of an Aegean origin must also be rejected because the $^{206}$Pb/$^{204}$Pb ratios are slightly too high. Only some
signatures from the Taurus Mountains could be close to the signatures of the artefacts in the diagram $^{208}\text{Pb}/^{204}\text{Pb}$ vs $^{206}\text{Pb}/^{204}\text{Pb}$, but they differ in the ratios $^{207}\text{Pb}/^{204}\text{Pb}$ vs $^{206}\text{Pb}/^{204}\text{Pb}$; the Anatolian origin can be rejected. The mined ores would therefore be of Iberian origin (Fig. 5).

In order to define their origin more precisely, the lead isotopic sig-
natures of the artefacts can also be compared with different mining areas
in the Iberian Peninsula. Six potential mining areas located relatively
close (within 150 km) can be considered.

Among the available signatures are those from the mines of Carta-
gena (Graeser and Friedrich, 1970; Baron et al., 2017; Milot et al., 2021;
Domergue and Rico, 2024 p. 25), which were extensively exploited in
previous centuries (10th-8th centuries BC to mid-6th century BCE) to
produce litharges similar to those studied. In addition, the signatures of
neighbouring ore deposits include:

- The closest mining district to Cartagena: Mazarón (data from the Oxalid database; Graeser and Friedrich, 1970; Milot et al., 2021)

- Sierra Almagrera (data from the Oxalid database; Arribas and Tosdal, 1994; Hunt Ortiz, 2003; Montero Ruiz and Murillo-Barroso, 2010; Murillo-Barroso et al., 2019);

- Sierra de Bedar (data from the Oxalid database; Montero Ruiz and Murillo-Barroso, 2010; Murillo-Barroso et al., 2019);

- Cabo de Gata (data from the Oxalid database; Hunt Ortiz, 2003);

- Sierra de Gador (Arribas and Tosdal, 1994; Montero Ruiz and Murillo-Barroso, 2010)

Furthermore, although located respectively 250 km and over 500 km
from the site, the mining areas of Ibiza (data from Hermanns, 2014), Rio

Tinto (Oxalid database; Marcoux, 1998; Pomiès et al., 1998; Hunt Ortiz, 2003), and Catalonia (Rafel et al., 2019; Montero Ruiz, 2017; Canals and Cardellach, 1997) were also considered. This choice is based on the fact that lead mining activity has been previously confirmed in these areas during earlier periods.

This second projection shows that the most probable origin of all the
artefacts is the Cartagena- Mazarón mining area (Fig. 6). This result is
interesting for a number of reasons. Firstly, it emphasises that lead ob-
jects were produced from the litharges in circulation. In addition, the
litharges analysed have signatures comparable to those produced at La
Fonteta one to two centuries earlier. These results support those of Renzi
et al., (2009), who also attribute a Cartagena-Mazarón origin to the
litharges from the La Fonteta workshop and the Mazarón 2 shipwreck.
Those mines probably provided the lead that led to the production of
litharges of comparable typology between the 8th and 3rd centuries BC.

Therefore, although no workshop has yet been discovered, it appears
that the production of litharge between the 5th and 3rd centuries BC
followed a similar production model that of the period before the
commercial crisis: its ore source is similar, as is its texture and chemical
composition.

**5. Discussion: Low but continuous production**

If it is confirmed that the mines of Cartagena were indeed exploited
between the 5th and 3rd centuries BCE, it is very likely that the pro-
duction processes of the litharges remained identical throughout the
period from the 8th to the 3rd century BCE, despite the commercial crisis
of the 6th century BCE. It was only during Roman exploitation that

<figure><img src="image_7.png" /></figure>

**Fig. 5.** Bivariate projections of the isotopic signatures of the artefacts analysed in this study and the signatures of lead deposits from the Iberian, Aegean, Sardinian and Taurus Mountains. Data from the Oxalid database (Stos-Gale and Gale, 2009); Graeser and Friedrich, 1970; Boni and Koeppel, 1985; Seeliger et al., 1985; Arribas and Tosdal, 1994; Marcoux, 1998; Hirato et al., 1995; Begemann et al., 2001; Sayre et al., 2001; Ceyhan, 2003; Hunt Ortiz, 2003; Santos Zalduegui et al., 2004; Tornos and Chiaradia, 2004; Valera and Valera, 2005; Koptagel et al., 2007; Montero Ruiz and Murillo-Barroso, 2010; Hanilçi and Öztürk, 2011; Hermanns, 2014; Baron et al., 2017; Murillo-Barroso et al., 2019; Milot et al., 2021 and Domergue and Rico, 2024 p. 25, keeping only the lead deposits (see Tomczyk, 2022).
<figure><img src="image_8.png" /><figcaption>**Fig. 6.** On the left, bivariate projections of lead isotopic ratios; on the right, localisation of lead-bearing deposits (orange zones) and isotopic analyses of lead from the considered deposits (the colour of the figures corresponds to that of the points representing the deposits in the left diagram, the size of the figures is proportional to the number of analyses available for each mining area). The Sierra de Gador ores are not plotted because they have low $^{206}$Pb/$^{204}$Pb ratios (average 18.3), as are the Rio Tinto ores ($^{206}$Pb/$^{204}$Pb < 18.32) and Catalonia ores ($^{206}$Pb/$^{204}$Pb < 18.55).</figcaption></figure>

practices changed: the litharges then took the form of small conical rolls, one to two centimetres in diameter (Baron et al., 2017).

The litharges would have circulated on a regional scale, where they would have been used to extract metallic lead, which could have been used to shape lead artefacts or incorporated into ternary bronze alloy compositions. Some of this lead may also have been exported along new trade routes. An argument in favour of the emergence of new exchange networks is based on the analysis of silver objects found at Mas Castellar de Pontos (Catalonia, 500–200 BCE): some of these objects are thought to have the isotopic signature of lead from the mines of Cartagena (Montero Ruiz et al., 2008). Thus, Catalonia, which had previously been a producer of lead, could have imported it at the beginning of the 5th century BCE.

The sudden end of silver production in the Iberian coastal regions (from the Rio Tinto mines to the island of Ibiza) certainly caused a drastic fall in lead production from the Cartagena mines, to the point where it would have been barely perceptible in the pollution of the bay. However, this study shows that production in Cartagena would have continued on a smaller scale. Some silver and lead would have been extracted from the mines and smelted using the same processes as before the crisis, probably by the same population group.

## 6. Conclusion

The litharges from three sites in the province of Alicante, dated to a period after the Phoenician trade crisis, show strong geochemical similarities with those produced in the same region before this crisis. The diameter, thickness, and texture of the litharges indicate a common manufacturing process involving the absorption of lead through capillarity by a porous and calcium-rich furnace lining. The presence of metallic silver on their surface indicates that they are linked to the same cupellation process.

Lead isotope analysis shows that it came from the Cartagena mines, as did the earlier litharges. This technological continuity, from the deposits mined to the metallurgical processes used to produce standardised litharges, shows that a same *chaîne opératoire* persisted throughout the 8th to 3rd century BCE in the region.

Estimating the production tonnages from the mines is complex, as the mining areas have been extensively reworked from Roman times to the modern period. However, sedimentary archives indicate a sharp

decline in production during the 6th century BCE. Production from the Cartagena mines probably declined after this crisis, but did not cease altogether.

## CRediT authorship contribution statement

**Céline Tomczyk:** Writing – original draft, Methodology, Investigation, Funding acquisition, Formal analysis, Data curation, Conceptualization. **Christophe Petit:** Writing – review & editing, Funding acquisition. **María Berná:** Resources. **Laurent Costa:** Project administration, Funding acquisition. **Jessica Legendre:** Methodology, Investigation. **Jesús Moratalla:** Validation, Supervision. **Sidonie Révillon:** Methodology, Investigation, Formal analysis. **Pierre Rouillard:** Writing – review & editing, Validation, Supervision, Project administration.

## Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

## Data availability

all data are included in the manuscript

## Acknowledgements

The SEM equipment used in this study belongs to the MAPS platform - Imagerie des patrimoines et spatialisation et microscopie pour les matériaux anciens de la MSH Mondes (UAR 3225). It was funded by the Île-de-France region as part of the major interest Matériaux anciens et patrimoniaux (DIM - MAP), the CNRS, and the LabEx "Les passés dans le présent".

The lead isotope analyses were funded by the LabEx DynamiTe and the ArScAn laboratory. We would like to thank Zoï Tshirtoni and Nicole Lozouet for their support in obtaining this funding.

The authors also wish to thank Romualdo Seva Román, María Dolores Landete Ruiz, and Cristina Biete Bañón for the preliminary analyses conducted on the material from Las Tres Hermanas.
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