Journal of Archaeological Science 43 (2014) 239e255

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Journal of Archaeological Science

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Smelting of magnetite and magnetiteeilmenite iron ores in the

northern Lowveld, South Africa, ca. 1000 CE to ca. 1880 CE
David Killick a, *, Duncan Miller b
a
Department of Anthropology, University of Arizona, Tucson, AZ 85721-0030, USA
b
Department of Geology, University of the Free State, Nelson Mandela Drive, Bloemfontein, Brandhof 9324, South Africa

a r t i c l e i n f o a b s t r a c t

Article history: The Lowveld of north-eastern South Africa is poorly suited to agriculture or pastoralism but is rich in
Received 10 November 2012 mineral resources. There is much evidence of exploitation of the copper, iron and salt resources of this
Received in revised form region during the second millennium CE. The bloomery iron smelting technologies of this region show
15 December 2013
several unusual features: (1) all known smelting sites used almost pure oxide ores, requiring the addition
Accepted 25 December 2013
of silicate flux to produce slag; (2) some used magnetiteeilmenite ores that produced slags containing up
to 25 mass % TiO2; and (3) iron ore was carried substantial distances to smelting sites. Modern blast
Keywords:
furnaces cannot use iron ores containing more than 2% TiO2, but in the bloomery process TiO2 combines
Archaeometallurgy
Technology
with iron oxides and silica to produce highly fluid slags that separate cleanly from iron metal. This
Smelting allowed ancient ironworkers to process a much wider range of iron ores than modern industry can use.
Iron The archaeological significance of this study is that we show that the geological source of ore used at any
Slag smelting site in the Lowveld can be determined by chemical analysis or thin-section microscopy of the
South Africa slag. This will allow archaeologists to include iron production in future network analyses of past regional
economic interaction in this region.
Ó 2013 Elsevier Ltd. All rights reserved.

1. Introduction Much of this archaeological evidence relates to exploitation of

The northern Lowveld (Fig. 1) forms the extreme northeast
corner of South Africa. It is a low plain bounded to the west by the
north-south escarpment, above which lies the Highveld, and to the
east by the low Lebombo Hills in modern Mozambique. It is covered
by hot infertile savanna woodland, prone to drought and host to
many endemic human and animal diseases, including malaria, tick
fever, sleeping sickness and bilharzia. These made the Lowveld
unattractive for agriculture or pastoralism, and even today it is
relatively sparsely populated.
There is little archaeological evidence for permanent human
settlement in the Lowveld before 1000 CE, although its western
boundary
the escarpment around Tzaneen (Fig. 1)
has been
settled by iron-working agriculturalists since at least 350e450 cal.
CE (Klapwijk and Huffman, 1996). Nevertheless, the northern
Lowveld does have a rich archaeological record during the Late Iron
Age, which is defined here as the interval from about 1000 cal. CE to
1880 CE, when European miners and missionaries first settled in
the region.
* Corresponding author. Tel.: þ1 520 621 8685; fax: þ1 520 621 2088.
E-mail address: killick@email.arizona.edu (D. Killick).
the rich mineral resources of the northern Lowveld. Late Iron Age
populations produced salt at six saline springs in the region, mined
copper ores in at least six locations, and smelted copper and iron at
many sites, some of which are up to 50 km from any potential
source of ore (Fig. 1). A previous synthesis (Miller et al., 2001)
provided an introduction to the archaeology of metal production in
the region. This study focuses upon the technology and spatial
distribution of iron working. Copper working will be discussed in a
future paper.
2. Prior studies of iron production in the Lowveld
The greatest concentration of Iron Age mining and smelting
activity in the Lowveld is around the modern mining town of
Phalaborwa (Fig. 1). Until open-pit mining began in 1965, the
summit of Lolwe hill, just south of the town, was riddled with old
shafts, trenches and adits for mining oxidised copper ores. The
lower slopes were covered with a blanket of magnetite scree, used
as ore for smelting iron. Karl Mauch, a European explorer, observed
the mining and smelting of copper here in 1868 (Bernhard, 1971;
pp. 41, 54), but all indigenous metallurgical activity seems to have
ceased by 1880. The abandoned mines and smelting furnaces were
described by a succession of visiting geologists (Mellor, 1906; Hall,

0305-4403/$ e see front matter Ó 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jas.2013.12.016
240 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255

Fig. 1. Map of the northern Lowveld, showing principal locations mentioned in this paper.

1912; Trevor, 1912; Schwellnus, 1937; Verwoerd, 1956; Hanekom
et al., 1965). The first scientific analyses of metallurgical residues
from archaeological sites around Phalaborwa were those of
Schwellnus (1937) and Verwoerd (1956).
The earliest written account of an archaeological excavation at
Phalaborwa appears to be an unpublished report by D. S. van der
Merwe, who excavated five smelting furnaces (van der Merwe,
1936), but no trained archaeologist excavated there until shortly
before open-pit mining began at Lolwe in 1965. R. Mason conducted
several test excavations in 1962 on terraced settlements on the
volcanic hills around Phalaborwa (Mason, 1968), and in 1965 N. J.
van der Merwe carried out further excavations on both habitation
and smelting sites and produced the first radiocarbon dates for the
region (Stuiver and van der Merwe, 1968). Between 1970 and 1973
van der Merwe led an American team, which conducted an exten-
sive field survey of the wider region, including much of the
Murchison Range and northern portions of the Kruger National Park
(Thorne, 1974). In 1977 Killick and van der Merwe revisited most of
the smelting sites located by this survey to collect ore and slag
samples for chemical analysis, and in 1978 and 1979 Killick carried
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
out further survey in the Murchison and Sutherland Ranges (Fig. 1;
van der Merwe and Killick, 1979). These surveys introduced the
regional approach to past mining and metallurgy to South Africa.
Excavations of smelting sites at Eiland (Fig. 1; Evers, 1975, 1982)
and around Tzaneen (Fig. 1; Klapwijk, 1986) revealed the distinctive
triangular furnaces previously noted at Phalaborwa. Comparison of
the spatial distributions of iron ore resources (see below) and
smelting sites showed that ores were transported over substantial
distances (van der Merwe and Killick, 1979; Miller et al., 2002). In
the Soutpansberg mountains, which define the northern boundary
of the Lowveld (Fig. 1), a remarkable historical account (Giesekke,
1930; translated and annotated by Miller et al., 2002) notes the
regular transport of iron ore by human porters from the carbonatite
complex at Schiel (Fig. 1) to the northern mountains. Indigenous
iron smelting appears to have continued in the Soutpansberg to the
end of the nineteenth century (Wessmann, 1908; Junod, 1927;
Stayt, 1931; de Waal, 1942). An anthropological study of the
Lobedu people also notes that iron ore was formerly transported
from this source to Modjadji (Fig. 1), which is about 55 km south of
Schiel (Krige, 1941). Mining trenches and smelting sites have been
recorded around Schiel (Miller et al., 2002; Mathoho, 2012) but no
systematic survey for smelting sites north of the Murchison Range
has yet been undertaken.
Subsequent studies of metal production in the Phalaborwa re-
gion by the University of Pretoria include the work of Meyer (1986)
in the Kruger National Park, and the intensive archaeological and
oral historical study by Pistorius (1989) of metal working sites
around Phalaborwa. This identified three different groups of metal
workers in the Phalaborwa region, and confirmed that there were
two discrete periods of occupation at Phalaborwa itself (Pistorius,
1989; Plug and Pistorius, 1999).
3. Distribution and geology of iron ores in the northern
Lowveld
All iron ores in the northern Lowveld are of Precambrian age
because younger strata have been stripped away by westward-
moving erosion, exposing the Precambrian basement as far as the
escarpment (which runs along the left edge of Fig. 1). Most of the
bedrock exposed across the Lowveld is Archaean granite gneiss,
which hosts no iron ores. Within the granite there are meta-
morphosed remnants of older rocks. There are several greenstone
belts (sedimentary and igneous rocks subsequently meta-
morphosed to the greenschist facies) and two intrusive carbonatite
complexes. Two of the greenstone belts and both carbonatites are
potential sources of iron ore for past bloomery iron smelting.
3.1. The Sutherland Range
The Sutherland Range (Fig. 1), forming part of the Giyani
Greenstone Belt (Brandl et al., 2006), is roughly 70  20 km in
extent, composed of metavolcanic schists of ultramafic and mafic
composition (McCourt and van Reenen, 1992). These include minor
Banded Iron Formations (BIF), which have white layers of chert
alternating with red layers of haematite and/or siderite. BIF ores
have not yet been noted on iron smelting sites in the Lowveld. It is
likely that their silica contents are too high for bloomery smelting,
though systematic investigation of them has not yet been under-
taken. Attempts by Killick to split the silica-rich from the iron-rich-
layers with hammer and chisel were unsuccessful.
3.2. The Murchison Range and Rooiwater Complex
The Murchison Range (Fig. 1) is a 140  20 km greenstone belt
that trends WSW to ENE, and is mostly composed of tightly folded
241
metasedimentary and metavolcanic rocks that originally formed
around 3.0 billion years ago (Brandl et al., 2006; Jaguin et al., 2012).
These include minor BIF and host epigenetic antimony, mercury,
zinc and copper deposits (van Eeden et al., 1939). The sediments
were intruded on their northern side by the Rooiwater Complex, an
ancient layered suite of igneous rocks. This contains two thin sheets
of magnetite (Fe3O4) e ilmenite (FeTiO3) ore that were formed by
oxidation and gravitational separation in a magma chamber. These
now dip nearly vertically because of tight folding of the Rooiwater
Complex. These parallel bands are only 4
6 m wide and are about
700 m apart. Both are exposed intermittently in schists for 14 km
along strike in flat terrain to the north of the Murchison range,
directly south of Eiland in Fig. 1 (van Eeden et al., 1939). To the west
of this double band there are two reported outcrops of a single
magnetite band in the Rooiwater Complex. A “magnetite lens” was
mapped by van Eeden et al. (1939) 8 km due west of the west-
ernmost exposure of the double band, while Schwellnus et al.
(1962, p. 16) report a magnetite band “2 feet thick” in basic
schists in the valley of the Thabina River about 25 km SSE of Tza-
neen. Millions of tons of magnetite rubble are exposed at surface, so
there would have been no need for iron smelters ever to mine the
ore.
Reynolds (1986) published chemical analyses of fourteen sam-
ples of ore from the bands in the central Murchison Range, five of
which are reproduced here in Table 1. In his analyses TiO2 contents
range from 14 to 25 mass % TiO2, V2O5 contents from 0.75 to 1.40
mass %, and samples from the lower band also contain up to 1.5
mass % Cr2O3. The high levels of these elements mean that Rooi-
water magnetites cannot be used in modern blast furnaces (for
which the cut-off is 2 mass % TiO2) but we show below that they
posed no problem for ironworkers using the bloomery process. In
polished section the microstructure of these ores is quite variable
(Reynolds, 1986), as some are more affected than others by meta-
morphism, but all have at least two phases
magnetite and
ilmenite (Fig. 2)
and many also have exsolved lamellae of ulvö-
spinel (Fe2TiO4) or ilmenite within the magnetite. Crystals of
pleonaste
solid solutions of magnesian spinel (MgAl2O4) in her-
cynite (FeAl2O4)
may also occur as a minor component. Many
samples are heavily altered, with much of the magnetite converted
to haematite, and the ilmenite to leucoxene.
3.3. The Phalaborwa Complex
The other two ore sources in the Lowveld are both carbonatite
complexes. The Phalaborwa Complex is the eroded throat of a
volcano that intruded through the Archaean granite 2.0 billion
years ago (Hanekom et al., 1965; Palabora Mining Company
Geological Staff, 1976; Verwoerd, 1986; Verwoerd and du Toit,
2006). The cross-section shown in Fig. 3 represents the situation
as open-pit mining began in 1965. Almost all of the section shown
here was mined away by 2002, when the pit reached a depth of
800 m below the former summit of Lolwe Hill. The mine was then
converted from an open-pit to a shaft mine, and is now more than
1300 m deep.
The inner portion of the complex, centred on Lolwe Hill, was a
vertical pipe of roughly concentric bands of pyroxenite, phoscorite,
and carbonatite, cross-cut by younger dolerite dykes (Fig. 3).
Phoscorite is a rock composed principally of magnetite (Fe3O4),
apatite (Ca5(PO4)3(OH,F,Cl)) and olivine ((Mg,Fe)2SiO4). Two gen-
erations of carbonatite volcanism (the banded and transgressive
carbonatites) are recognised but have similar mineral assemblages,
the major minerals being calcite (CaCO3, with 2e5% Mg substitut-
ing for Ca) and magnetite. Phalaborwa is unique among the world’s
carbonatite complexes in possessing exploitable copper minerali-
sation (Verwoerd, 1986). The copper sulphide minerals are found in
242 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255

Table 1
Analyses of magnetites from the Phalaborwa Complex (PC) and the Rooiwater Complex (RC). SARM1 is from Stoch (1978); PMC5, PMC9 and PMC12 are unpublished analyses
from drill cores in the Transgressive Carbonatite member of the PC, reproduced by permission of the Palabora Mining Company; RW18 and RW19 are from the upper
magnetiteeilmenite band of the RC, while RW27 and RW32 are from the lower band. RW2 is from the “magnetite lens” (all from Reynolds, 1986, Table 1). TB1 is an analysis by
Killick of an archaeological sample of magnetite ore from the farm Broederstoomdrift 534LT, Tzaneen.

SAMPLE SiO2 TiO2 Al2O3 Cr2O3 Fe2O3 FeO MnO MgO CaO V2O5 H2Oþ H2O
TOTAL

Rooiwater magnetiteeilmenite ores

RW18 1.78 14.62 2.68 0.80 66.05 11.09 0.21 1.75 nd 1.41 nd nd 99.24
RW19 2.92 14.93 2.34 1.19 61.82 14.00 0.18 0.86 nd 1.32 nd nd 99.61
RW27 2.66 20.83 3.83 <0.05 48.37 22.5 0.32 1.68 nd 0.80 nd nd 100.94
RW32 2.21 21.52 4.08 <0.05 52.00 17.06 0.27 2.34 nd 0.84 nd nd 100.27
RW2 2.09 12.23 6.12 <0.05 55.11 22.97 0.19 1,78 nd 0.86 nd nd 99.52
TB1 2.23 23.22 2.26 nd 40.08 26.71 0.33 2.37 0.01 0.99 0.96 0.08 99.24
Phalaborwa magnetite ores
SARM12 0.34 0.72 0.77 <0.01 95.28 nd 0.22 2.80 1.09 0.05 nd nd 101.26
PMC5 0.34 0.76 0.75 <0.01 94.95 nd nd 1.60 0.98 0.09 nd nd 99.47
PMC9 0.31 1.43 0.41 <0.01 95.81 nd nd 0.70 0.73 0.15 nd nd 99.55
PMC12 0.49 2.66 0.47 <0.01 93.95 nd nd 1.96 0.98 0.11 nd nd 100.62

shear zones in the phoscorite and carbonatite zones, but have enclose crystals of apatite, as in Fig. 4. The low-Ti magnetite from
highest values in the transgressive carbonatite, which formed the carbonatite often contains arrays of tiny cubic crystals of
Lolwe Hill, in which prehistoric copper mines were located. magnesian spinel and may show fractures filled with calcite and
The phoscorite and carbonatite members contain vast quanti- copper sulphides (Hanekom et al., 1965; Palabora Mining
ties of magnetite iron ore, but it appears that this was not mined in
precolonial times, except when removed incidentally during
copper mining. Millions of tons of magnetite, the residual product
of erosion, formed thick scree over the lower slopes of Lolwe Hill
and the surrounding pyroxenite. This was an inexhaustible ore
source for bloomery ironworkers. The major impurity in the
magnetite is a variable amount of titanium. The lowest values of
TiO2 (0
2%) are in magnetite from the transgressive carbonatite
(e.g. analyses in Table 1). In the phoscorite the magnetite contains
up to 4% TiO2, and in the surrounding pyroxenite the TiO2 content
rises to as much as 8% (Hanekom et al., 1965; pp.63
65). As TiO2 is
not reduced in bloomery iron smelting, all of it should end up in
the slag. The TiO2 contents of slags smelted from Phalaborwa
magnetite thus allow us to infer from which of these rocks the ore
originally derived. In polished section Phalaborwa magnetite is
easily distinguished from Rooiwater Complex magnetite because
Phalaborwa magnetite lacks euhedral crystals of ilmenite and may

Fig. 2. Polished section of sample KSME from the lower magnetiteeilmenite band of
the Rooiwater Complex e reflected cross-polarized light (XPL) in air. Subhedral
ilmenite crystals showing strong bireflectance from medium to very dark grey are
surrounded by heavily weathered magnetite (light grey) containing lamellae and
irregular patches of ulvöspinel (medium grey, isotropic). The small black areas within
the magnetite are pitting from sample preparation.
Fig. 3. Vertical geological section through the central lobe of the Phalaborwa Complex
before the onset of open-pit mining in 1965, as defined by drill cores. Depth levels are
from the summit of the former Lolwe Hill. (Redrawn after Palabora Mining Company
Geological Staff, 1976, Fig. 5.)
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Company Geological Staff, 1976). The high-Ti magnetite from the
outer phoscorite and pyroxenite is a solid solution of ulvöspinel in
magnetite, and in consequence has a strong pinkish brown colour
in reflected plane polarised light (PPL) (Fig 4). Parallel arrays of
thin to coarse plates of ilmenite or ulvöspinel can sometimes be
seen in some high-Ti magnetite crystals; these have formed by
solid-state oxidation exsolution after crystallisation of the host
magnetite crystal. These microstructural signatures allow Phala-
borwa magnetite to be identified on smelting sites distant from
the ore body, and to be readily distinguished from the magnetitee
ilmenite ores of the Rooiwater Complex.
3.4. The Schiel Complex
The Schiel Complex (Fig. 1) is also a carbonatite complex. It has
not been mined within the last 150 years, but oral histories state
that this was a major source of iron ore for the Venda of the
Soutpansberg, as is reflected in its Venda name Tshimbupfe, which
means “iron mountains” (Wessmann, 1908; Junod, 1927;
Schwellnus, 1937; Stayt, 1931; de Waal, 1942; Miller et al., 2002;
Mathoho, 2012). It is thought to be of roughly the same age as
the Phalaborwa Complex but has a less well-defined annular
structure and has minimal copper mineralisation (Verwoerd,
1986; Stettler et al., 1993; Verwoerd and du Toit, 2006). The car-
bonatite, phoscorite and pyroxenite members form irregular
subparallel lines and arcs in syenite. They have eroded faster than
the syenite, and are thus obscured by soil, their presence being
indicated at surface largely by lines of magnetite rubble
(Verwoerd, 1986). Shallow trenches up to a hundred metres in
length from pre-European mining were still visible in the 1990s,
and there is a smelting furnace on the farm Schuynshoogte (VS2 in
Table 2) that was preserved to its full height of 1.2 m until the
1990s, but has since been vandalized. (Compare photographs in
Stayt (1931) and Miller et al. (2002) with that in Mathoho (2012)).
Much of the iron ore accessible to past miners derived from the
phoscorite, which drill cores have shown to contain about 15%
magnetite along with phlogopite mica, calcite, apatite and
accessory biotite. Magnetite samples from drill cores contained
1
5% TiO2, averaging 3%, and contain only trace amounts of va-
nadium (Verwoerd, 1986; Mathoho, 2012). An unpublished report
by the mining company FOSKOR states that in the two polished
Fig. 4. Polished section of magnetite (sample PMC) from the Phalaborwa Complex
(reflected plane-polarized light (PPL), air). The medium grey crystals (brown in online
version) are titaniferous magnetite, oxidized to haematite along grain boundaries and
cracks. The two dark grey subhedral crystals are heavily altered apatite.
243
sections examined the TiO2 was in solid solution (“in vaste
oplossing”) in the magnetite.
3.5. Summary of the iron ore resources
In summary, at three locations in the northern Lowveld huge
amounts of iron ore could be obtained from surface scree or from
shallow trenches. The magnetiteeilmenite ores of the Murchison
Range are located between the two carbonatite complexes, and can
be clearly distinguished from magnetite in the carbonatites by ore
microscopy and by higher contents of TiO2 and V2O5. Neither of
these oxides can be reduced in bloomery furnaces, and thus they
should transfer quantitatively to the slag. It should therefore be
easy to determine the geological source of ore used on any smelting
site in the region from chemical analysis of the slags. (We assume
that ore from the Phalaborwa Complex was not transported north
across the Murchison Range, and conversely that ore from the
Schiel Complex was not transported south across the Murchison
Range.) It has also been shown that forged iron artefacts produced
in the Lowveld can be traced to either the Rooiwater bands or to the
carbonatites by electron microprobe analysis of the slag stringers
that they contain (Gordon and van der Merwe, 1984).
4. Smelting sites and samples
Table 2 lists 43 smelting sites recorded by van der Merwe and
his teams between 1965 and 1973, and by Killick between 1977 and
1979. Slag samples were collected for analysis from many of these
sites in 1977 and 1978. This is far from a complete listing of known
smelting sites in the northern Lowveld; for additional sites see
Evers (1981), Klapwijk (1986), Meyer (1986), Pistorius (1989) and
Mathoho (2012).
4.1. Sites around the Phalaborwa Complex
The outermost ring of the Phalaborwa Complex consists of a
circle of syenite pipes emplaced vertically through the Archaean
granite. These are more resistant to erosion than the granite and
now form steep-sided hills. These hills were terraced in antiquity,
and several investigators have excavated houses, smelting furnaces
and forges on these terraces and at the base of the hills (Mason,
1968; van der Merwe and Scully, 1971; Meyer, 1986; Evers and
van der Merwe, 1987; Pistorius, 1989; Plug and Pistorius, 1999)
The earlier sites (10th
13th centuries cal. CE) were open villages on
flat land at the bases of syenite hills. The later sites (17th
19th
centuries cal. CE) are located on terraces built on the lower slopes of
these hills (Evers and van der Merwe, 1987).
The smelting sites of SPK4, SPK5 and SPK6 are located around
the base of Kgopolwe hill. Each had one or more iron smelting
furnaces. All excavated examples had a triangular plan with a
tuyère port at each apex (Evers and van der Merwe, 1987; Miller
et al., 2001). The distance from each apex to the opposite wall
was 1.2 m in the best-preserved furnace at SPK5 (Evers and van der
Merwe, 1987, Fig. 15), and the shaft height in intact examples is
about 1.0 m. Radiocarbon dates are 280  60 BP (Y-1658) for the
SPK4 furnace, 80  45 BP (Pta-339) for the SPK5A furnace and
520  60 BP (Y-1657) for a slag heap at SPK4 (Evers and van der
Merwe, 1987). A stratigraphic sequence of three house floors was
excavated by N. J. van der Merwe at SPK3 and yielded radiocarbon
dates ranging from 960  80 BP (Y-1638) to 820  80 BP (Y-1662).
These yielded a few iron artefacts, some of which are examined
below.
At the base of Matsepe Hill there are several clusters of undated
smelting furnaces and slag heaps. Sites SPM2, SPM3 and SPM4 are
unexcavated iron smelting sites. SPM2 had an intact triangular
244 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255

Table 2
Smelting sites recorded by the 1970e1973 surveys (Thorne, 1974; Evers and van der Merwe, 1987) the 1978e1979 surveys (Killick, unpublished) and some other published
sources.

Site label Coordinates 1:50,000 map sheet Farm name Source Comments

Phalaborwa
SPK4 310746E 235600S 2331CC Phalaborwa Laaste 24LU Evers and van der Merwe (1987) Iron furnace
SPK5 310746E 235600S 2331CC Phalaborwa Laaste 24LU Evers and van der Merwe (1987) Iron furnace
SPK6 310746E 235600S 2331CC Phalaborwa Laaste 24LU Evers and van der Merwe (1987) Iron furnace
SPM1 310513E 235957S 2331CC Phalaborwa Wegsteek 30LU van der Merwe survey 1972/73 Copper furnace
SPM2 310513E 235955S 2331CC Phalaborwa Wegsteek 30LU van der Merwe survey 1972/73 Iron furnace
SPM3 310513E 235952S 2331CC Phalaborwa Wegsteek 30LU van der Merwe survey 1972/73 3 iron furnaces
SPM4 310513E 235952S 2331CC Phalaborwa Wegsteek 30LU van der Merwe survey 1972/73 Slag heap
Mashishimali hills and Murchison range
PQ1M 305623E 240313S 2430BB Mica Square 150 KT van der Merwe and Killick (1979) 7 iron furnaces
IH1M 305409E 240244S 2430BB Mica Hope 149 KT van der Merwe survey 1972/73 Iron furnace
IH2M 305445E 240233S 2430BB Mica Hope 149 KT van der Merwe survey 1972/73 Slag heap
IH4M 305358E 240313S 2430BB Mica Hope 149 KT van der Merwe survey 1972/73 Iron (?) furnace
IL2M 305343E 240424S 2430BB Mica Lillie 148 KT van der Merwe survey 1972/73 Iron furnace
IL4M 305358E 240422S 2430BB Mica Lillie 148 KT van der Merwe survey 1972/73 Slag heap
IL6M 305309E 240410S 2430BB Mica Lillie 148 KT van der Merwe survey 1972/73 Slag heap
IL8M 305115E 240428S 2430BB Mica Lillie 148 KT Killick survey 1978 Village/slag
IL12M 305017E 240411S 2430BB Mica Lillie 148 KT van der Merwe survey 1972/73 Iron furnace
IL17M 305134E 240423S 2430BB Mica Lillie 148 KT Killick survey 1978 Iron furnace
IL18M 305108E 240433S 2430BB Mica Lillie 148 KT Killick survey 1978 Slag heap
GG1M 305328E 235125S 2330DD Mulati Granville 767 LT van der Merwe survey 1972/73 Slag heap
GG2M 305205E 235118S 2330DD Mulati Granville 767 LT van der Merwe survey 1972/73 Slag heap
GQ1M 303445E 235149S 2330DC Gravelotte Quagga 759 LT Killick survey 1978 Iron furnace
GM3M 303036E 235848S 2330DC Gravellotte Maranda 675 LT van der Merwe survey 1972/73 Slag heap
GM5M 303017E 235738S 2330DC Gravelotte Maranda 675 LT Killick survey 1977 Slag heap
GM7M 302901E 235729S 2330CD Letsitele Maranda 675 LT van der Merwe survey 1972/73 Slag heap
GM9M 302904E 235724S 2330CD Letsitele Maranda 675 LT van der Merwe survey 1972/73 Slag heap
GM10M 303040E 235808S 2330DC Gravelotte Maranda 675 LT Killick survey 1977 Slag heap
GM11M 302926E 235809S 2330CD Letsitele Maranda 675 LT Killick survey 1977 Slag heap
GR3M 302816E 235639S 2330CD Letsitele Rooiwater 673 LT van der Merwe survey 1972/73 Slag heap
GR4M 302735E 235648S 2330CD Letsitele Rooiwater 673 LT van der Merwe survey 1972/73 Slag heap
GR6M 302804E 235431S 2330CD Letsitele Rooiwater 673 LT van der Merwe survey 1972/73 Slag heap
GN1M 302758E 235229S 2330CD Letsitele The Neck 565 LT Evers and van der Merwe (1987) Iron furnace
GN2M 302832E 235322S 2330CD Letsitele The Neck 565 LT van der Merwe survey 1972/73 Iron furnace
North of Murchison
EIL1 303933E 234254S 2330DA La Cotte Mabete 726 LT Evers (1982) Iron furnace
EIL2 303936E 234253S 2330DA La Cotte Mabete 726 LT Killick survey 1978 Slag
EIL3 304126E 234202S 2330DA La Cotte Mabete 726 LT Killick survey 1978 Ore and slag
EIL4 304219E 234036S 2330DA La Cotte Eiland 725 LT Killick survey 1978 Ore and slag
EIL5 304144E 234135S 2330DA La Cotte Eiland 725 LT Killick survey 1978 Slag
EIL6 304134E 234054S 2330DA La Cotte Eiland 725 LT Killick survey 1978 Iron furnace
GAZ1M 302705E 231935S 2330AD Hildreth Ridge State Land Killick survey 1979 Slag
GAZ2M 302652E 232058S 2330AD Hildreth Ridge State Land Killick survey 1979 Slag
Schiel complex
VS1M 302241E 230751S 2330AB Levubu Schuynshoogte 29LT van der Merwe survey 1972/73 Iron furnace
VS2M 302520E 230908S 2330AB Levubu Schuynshoogte 29LT Miller et al. (2002) Iron furnace
VD1M 302613E 231052S 2330AB Levubu Tabaan 55LT van der Merwe survey 1972/73 Slag

three-port furnace about 1.5 m high. SPM3 had three similar
smelting furnaces in fair condition encircled by a large ring of slag.
SPM4 was a slag heap without any visible furnaces. We selected
these sites as a reference group that can safely be assumed to have
smelted magnetite ore from the Phalaborwa Complex.
4.2. Sites on the Mashishimali Hills, south of the Murchison Range,
and near Tzaneen
The Mashishimali Hills (Fig. 1) are 20e30 km WSW of the
modern town of Phalaborwa. They are of particular interest because
they host the largest known ancient iron smelting site in South
Africa (PQ1M, on the farm Square). This is at least 20 km from any
potential source of iron ore (van der Merwe and Killick, 1979). The
site has seven furnaces surrounded by an estimated 180,000 kg of
slag (Fig. 5), which is an order of magnitude larger than on any
other smelting site in the northern Lowveld. There is a single
radiocarbon date on charcoal from the slag heap of 220  35 BP
(Pta-2402). The furnaces have the same three vertical slits for tu-
yères, but a more rounded plan than the triangular furnaces plan
excavated around the Phalaborwa Complex. A very similar well-
preserved iron smelting furnace (IL-17M; Fig. 6) was excavated by
Killick in 1978 on the adjacent farm Lillie, and yielded a radiocarbon
date of 250  45 BP (Pta-2408).
Each of the sites listed so far had visible furnace remains above
ground level, which explains the relatively recent radiocarbon
dates obtained from them. The surveys of van der Merwe’s group
from 1970 to 1973 and of Killick in 1978 and 1979 found many other
sites that consist only of slag heaps. None of these are dated, but
slags from several of them are included in this study because they
offer opportunities to test our prediction that chemical analysis of
slags can establish which source of ore was used. Coordinates for
these sites are provided in Table 2. They include multiple sites from
the farms Lillie and Hope in the Mashishimali Hills, and from the
farms Rooiwater, Maranda and The Neck, all three of which are in
the Murchison Range just west of the town of Gravelotte (Fig. 1).
Two smelting sites on the farms Granville are in the eastern
Murchison Range, north of the road linking Gravelotte to Phala-
borwa. Further west, Killick was shown several smelting sites
around Tzaneen by J. Witt and M. Klapwijk and provided with
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 5. Plan of the iron smelting site PQ1M on the farm Square in the Mashishimali Hills (after van der Merwe and Killick, 1979, Fig. 3).
samples of slag and ore (see below). The locations of these are
shown on Fig. 1. There are many other iron smelting sites around
Tzaneen; see Klapwijk (1986, Fig. 1) for the locations of an addi-
tional 36 sites in this area.
4.3. Sites north of the Murchison Range and at the Schiel Complex
On the north side of the Murchison Range there are six smelting
sites (EIL1 through EIL6) on the farms Eiland and Mabete, near an
important ancient saltworks (Evers, 1975, 1981, 1982). EIL1 is a
furnace excavated by Evers (his 2330 DA:2), which produced a
radiocarbon date of 270  40 BP (Pta-2505; Evers, 1982). EIL6M is
also a well-preserved furnace; the other four are just slag heaps or
surface scatters. GAZ1M and GAZ2M are far to the north of Eiland,
near the Anderson Mission, and on the eastern side of the Middle
Letaba River (Fig. 1). No systematic survey has been done around
the Schiel Complex (Fig. 1), but three smelting sites (VS1M, VS2M
and VD1M) were recorded by van der Merwe, and more recently
Mothoto (2012) has recorded additional smelting sites in the vi-
cinity. VS2M is the standing furnace that is depicted in Junod
(1927), Miller et al. (2002) and Mathoho (2012).
5. Analytical methods
Major- and trace-element compositions of selected slag, ore and
sand samples were obtained by wavelength-dispersive X-ray
fluorescence (WD-XRF) in the Department of Geochemistry, Uni-
versity of Cape Town. Killick conducted the analyses, under the
supervision of A. Duncan and J. Willis, between 1977 and 1979.
About 500 g of washed sample was powdered in a rotary agate mill
to pass a 400 mesh screen. To avoid cross-contamination, a load of
pure quartz was milled between each sample. Where more than
one slag sample was analysed from a site, the samples are distin-
guished by suffixes (a through d). Major elements were measured
on lithium metaborate glass fusion discs by the method of Norrish
and Hutton (1969). Because of their high iron content, samples of
ore and slag powder were diluted 1:1 with pure powdered SiO2
245
before being made into glass discs. The chemical analyses were
recalculated to remove the effect of this dilution. This worked well
for slag analyses but did not produce acceptable analyses for many
of the ore specimens. Most analyses with totals outside the range
99.0e101.0% were discarded. Duplicate discs were prepared for all
samples and if both totals were acceptable the results were aver-
aged. Adsorbed water (H2O
) was estimated by weighing before
and after heating overnight to 100  C. Samples were then heated in
a muffle furnace at 850  C to convert all ferrous iron to ferric iron,
and stored in a desiccator until preparation of the discs. Bound
water (H2Oþ) and carbon dioxide were measured by a CO2/H2O
analyser on a separate portion, and ferric iron by titration using
another weighed portion dissolved in HF and HNO3 in platinum
dishes.
X-ray diffraction (XRD) analysis was conducted on selected
powdered samples at the University of Arizona in 1997, but the
results proved difficult to interpret. This is because of extensive
solid solution series in most of the minerals present in these slags,
so that their diffraction lines rarely matched those of the end
members of the series in XRD reference materials. Forty specimens
of ores and slags were prepared as polished epoxy mounts for study
in reflected light, and a further twenty specimens of slag as
24  48 mm polished thin sections. Initial petrographic and
reflected-light examinations were mostly conducted by Killick and
Miller at the University of Arizona in 1997. The metallographic
analyses of iron objects were done by Miller. In 2012 Killick made
more detailed studies of some of the slag and ore sections by optical
microscopy, and measured the composition of silicate and oxide
phases in selected thin sections, using a Cameca SX-100 electron
microprobe and natural mineral standards.
6. Results
6.1. Slags from sites around the Phalaborwa Complex
Samples SPM 2a, 2b, 2c, 3a, 3b, 4a, and 4b in Table 3 were all
from the iron smelting sites around Matsepe hill. Comparison of
246 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 6. Smelting furnace IL17M on the farm Lillie in the Mashishimali Hills. (Photo: D.
Killick).
these results with those for Phalaborwa magnetites in Table 1
showed that the slags had higher contents of TiO2. This indicates
that the magnetite selected for smelting must have derived from
the outer edges of the phoscorite or from the pyroxenite of the
Phalaborwa Complex (Hanekom et al., 1965). (The low-TiO2 mag-
netites in Table 1 were all from the transgressive carbonatite.) The
CaO contents of five of the seven samples were in the range 10e12
mass %, which is quite high for slags from bloomery iron smelting.
Four polished blocks and a polished thin section from SPM3 and
SPM4 were examined. All were dominated by small dendrites of
wüstite (Fe1-xO) in a matrix of tiny parallel-sided laths of silicates
and a dark glass crowded with crystallites. Almost all of the wüstite
crystals were densely speckled with tiny cubes of a darker phase.
Examination of these by electron microprobe showed that they had
higher titanium contents than their wüstite hosts, so they were
tentatively identified as ulvöspinel, but they were too small for
quantitative analysis by microprobe. Polygonal crystals of titanif-
erous magnetite were the second phase to crystallise, and formed
overgrowths on some wüstite dendrites (Fig. 7). The silicate phase
identified by microprobe in a thin section from SPM3 (see Table 4)
was kirschsteinite (CaFeSiO4) with some monticellite (CaMgSiO4) in
solid solution. The microstructures were very fine, which suggests
Fig. 7. Microstructure of a slag from SPM4 (reflected PPL, air). White grains (A) are
metallic iron, the rounded grains (B) are wüstite, the angular grains (C) are titaniferous
magnetite, and the dark laths (D) are fayalite or kirschsteinite.
Fig. 8. Partial phase equilibrium diagram and liquidus surfaces for iron oxide, silica
and titania under reducing conditions (redrawn after Fig. 3.292 in Verein Deutscher
Eisenhüttenleute, 1995).
rapid cooling, and a couple of slag sections had very thin skins of
magnetite. Since these slags were definitely not tapped, we think it
likely that the temporary seals on the vertical slits above the tu-
yères were broken open while some of the slag was still liquid.
Fig. 8 shows the experimentally determined equilibrium dia-
gram (mass percent) for iron oxides, titania and silica under
reducing atmospheric conditions. The phase diagram correctly
predicts the sequence of crystallisation seen in these slags, though
kirschsteinite crystallises rather than the predicted fayalite
(Fe2SiO4) because of the higher calcium contents in the slag. Note
also that both of the ternary eutectics in the iron-rich corner of the
phase diagram are below 1200  C, very close to the temperatures of
the two eutectics in the binary FeOeSiO2 phase diagram. Because of
their high levels of CaO (5e12%) and Al2O3 (4e12%) we did not try
to reduce the compositions of the slags in Table 3 to the three
components of the FeOeTiO2eSiO2 phase diagram. As these oxides
Fig. 9. Typical slag microstructure from PQ1M (reflected PPL, air). Primary rounded
dendrites of wüstite (white) have overgrowths of darker subcubic titaniferous
magnetite, which also forms dark spots within some wüstite dendrites (through solid-
state exsolution). The matrix between the oxide phases is composed of subhedral grey
laths of fayalite and/or kirschsteinite in glass.
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 10. A partially-reduced piece of Phalaborwa ore within a slag from site IL8M
(reflected PPL, air). The matrix of low-Ti magnetite (light grey) in the lower half of the
frame has exsolved small laths of ulvöspinel (medium grey) on (111) crystallographic
planes. The magnetite has been reduced to metallic iron (white) around its exterior,
but the ulvöspinel laths were not reduced, and two can be seen within the iron rim at
upper left. Reduction of the magnetite by CO has formed large bubbles of CO2 (the
black cavities) that were trapped in the slag e at the top of the frame e when it
solidified.
have opposite effects e CaO would lower the melting temperature,
while Al2O3 would increase it e we expect liquidus temperatures in
these slags to be little different from those indicated in Fig. 8.
6.2. Slags from sites of the Mashishimali Hills
Four samples from the estimated 180,000 kg of slag at PQ1M in
the Mashishimali Hills (Fig. 1) produced acceptable bulk chemical
analyses (Table 3). These were taken from different slag piles on the
site (Fig. 5). All had very similar chemical compositions. TiO2 varied
from 4.13 to 4.73 mass %, and CaO from 9.7 to 13.7%. We examined
eight polished blocks and five thin sections of slag from PQ1M, each
taken from a different portion of the slag pile. All were very similar
samples that had abundant dendrites of wüstite and titaniferous
magnetite, with the latter often seen as darker overgrowths on the
former. These occurred with small grains of iron metal and minute
laths of a silicate in a glass (Fig. 9). Microprobe analysis of the sil-
icates in one thin section (PQ1Mb in Table 4) showed that they were
kirschsteinite. The microstructures were very fine and some pol-
ished sections showed thin skins of magnetite, suggesting that the
vertical slits in the furnace wall above each tuyère were opened
while some of the slag was still molten.
The chemistry and microstructures of all of these samples were
essentially identical to most of the slags derived from magnetite
from the phoskorite or pyroxenite zones of the Phalaborwa Com-
plex, which is 20 km east of the site.
IL6M is a slag scatter (no furnace) on the farm Lillie in the
Mashishimale Hills. As the slag contains only a half percent of
titania (Table 3) the ore from which it derived must have come from
the central carbonatite at Phalaborwa.
IL8M is on the southern flank of Ga-Mashishimale hill, 9 km to
the west. In 1978 it was a rapidly eroding scatter about 50 m across
of diverse materials, including burned house daub, slag and a spill
of bronze. It is the only site in our sample to have provided evidence
for use of ores from both the Phalaborwa Complex (29 km ENE) and
the magnetiteeilmenite band of the Rooiwater Complex (minimum
distance 31 km NW). The bulk slag sample analysed from this site
had 15.01 mass % TiO2 and 1.47% V2O5 (Table 3). This must have
247
derived from ore from the lower magnetiteeilmenite band of the
Rooiwater Complex (compare with samples RW-18 and RW-19 in
Table 1 and with Reynolds, 1986). One of the three polished blocks
prepared from slags from IL8M had large subhedral and skeletal
ulvöspinels and late-forming silicates, which corresponded well to
the bulk chemical analysis, but the other two did not. Both of these
had microstructures very much like those described above for
PQ1M, which suggested that both derived from smelting Phala-
borwa ores. Each also contained a large (ca. 10 mm) grain of partly
dissolved magnetite. One of these had the regular array of tiny
spinel crystals, characteristic of magnetites from the central car-
bonatite member of the Phalaborwa Complex. The other (Fig. 10)
had exsolved fine laths of ulvöspinel along the octahedral (111)
planes of the host magnetite, which is characteristic of the higher-
TiO2 magnetite from the phoscorite and pyroxenite members of the
Phalaborwa Complex (Hanekom et al., 1965).
6.3. Slags from sites of the Murchison Range and near Tzaneen
Samples GR3Ma, GR4Mb, GR6Ma, GM5M, GM7M and GM11M in
Table 3 all had TiO2 contents above 20 mass %. The silica contents
were unusually low for bloomery slags, ranging from a low of 7.44
to a high of 19.29%. The range of V2O5 measured in these slags was
0.79e1.28%
significantly higher than in the slags from around the
Phalaborwa Complex (0.07e0.24%
see Table 3). The elevated
levels of TiO2 and V2O5 showed that these slags were produced by
smelting ores from the magnetiteeilmenite bands of the Rooiwater
Complex. The nearest outcrops of these bands are only 5
10 km
due north from each of these sites (Fig. 1).
Six polished blocks and two thin sections of these slags were
examined. All but one of these were cut from dense black blocks
that evidently had solidified at the base of the furnace. The
exception, from GR3M, was from a rounded nodule that evidently
had solidified in charcoal above the base. All appear to have been
very fluid when molten, as the microstructures of all but the nodule
were homogenous, with no flow boundaries noted. Two types of
microstructure were recorded.
In the first type 75
90% of the area of the slide was taken up by
pale to dark pink subhedral cubic crystals of a spinel (Fig. 11). These
were unzoned and were isotropic in reflected XPL. The small
amount of interstitial space was occupied by quenched feathery
dendrites of a silicate (visible only at high magnification) in glass. In
transmitted light these dendrites had a strong reddish brown
colour, which made it impossible to estimate birefringence. In only
two of these sections (one each from GR3M and GM1M) were
crystals of this phase large enough for analysis by electron micro-
probe. When analyses of this phase (Table 4) were recalculated by
standard mineralogical techniques, the best match was achieved
for 6 oxygens, when the number of cations closely approached 4.0.
This suggests that this mineral is a calcium-iron pyroxene, possibly
related to the augite/ferroaugite/titanaugite complex, though the
TiO2 contents are much higher than in naturally-occurring augites.
There was very little glass.
The compositions of spinels were determined by electron
microprobe in three thin sections, from GR3M, GR4M and GM1M
(Table 5). They showed no evidence of zoning under backscattered
SEM, and the TiO2 contents varied from 28 to 33 mass %. These
spinels are therefore solid solutions in which the dominant mole-
cule is ulvöspinel (64.27% FeO, 35.73% TiO2). In terrestrial rocks
solid-state oxidation exsolution is inevitably seen in iron-titanium
spinels (Haggerty, 1991), but rapid quenching to ambient temper-
ature has preserved a metastable single phase in these slags.
The second type of microstructure had elongated skeletal laths
of ilmenite (FeTiO3) with skeletal cubes of pink ulvöspinel, in a
matrix of the same feathery silicate dendrites (Fig. 12). Ulvöspinel
248 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 11. Microstructure of slag from the Murchison Range (site GR4M, reflected PPL,
air). The subhedral cubic and octahedral crystals are ulvöspinel; the interstitial ma-
terial consists of very fine feathery silicate dendrites in glass (not resolved at this
magnification).
was the first phase to crystallise, followed by ilmenite. Electron
microprobe analyses of ilmenites in a thin section from GM1M
(Table 5) gave an average composition very close to the composi-
tion of pure ilmenite (52.65 mass % TiO2, 47.35% FeO), with the high
totals suggesting the presence of a small proportion of ferric iron.
Note that the initial crystallisation in these slags is in agreement
with the FeOeTiO2eSiO2 phase diagram (Fig. 8), in that ulvöspinel
is the first phase to crystallise. But continuing precipitation of
ulvöspinel should drive the composition of the remaining melt
towards the fayalite field, not towards the ilmenite field. The
presence of ilmenite in some of these slags probably means that the
assumption on which Fig. 8 is based e that the atmosphere is
strongly reducing e was violated in the late stages of solidification
of these slags. If the furnaces were opened while the slags were
partially molten, the furnace atmospheres would become more
oxidising, which would favour the simultaneous crystallisation of
ilmenite and titaniferous magnetite, as in many igneous rocks (e.g.
Fig. 12. Microstructure of slag from the Murchison Range (site GR3M, reflected PPL,
air). The bright skeletal laths showing bireflectance are ilmenite; the darker subhedral
cubes and octohedra are ulvöspinel; the grey matrix consists of feathery dendrites of
silicates in glass (not resolved at this magnification); and the black areas are voids from
gas bubbles entrapped as the matrix solidified.
Carmichael, 1967). Some of the late-forming spinel was probably
titaniferous magnetite rather than ulvöspinel, but it is difficult to
distinguish these in reflected light. This would also explain the
relatively high levels of ferric iron in some of these slags (Table 3).
The thin section from GR3M was composed of several small
flows fused to each other. One of these contained a mineral that
formed thin jagged laths like ilmenite, but which had much lower
reflectance and was not bireflectant. Electron microprobe analysis
of this phase (Table 5) showed a consistent composition with about
70% mass TiO2. We have been unable to identify this mineral.
We did not obtain acceptable chemical analyses for slag samples
from sites GG1M and GG2M in the eastern Murchison Range
(Table 2 and Fig. 1), but the four polished sections and one thin
section prepared from these slags were all dominated by crystals of
ulvöspinel solid solution, as large subhedral cubes and octohedra,
or as skeletal dendrites with octahedral facets. The space between
these was occupied by a silicate phase and glass. The microstruc-
tures were very similar to the first type described above from the
western Murchison range, so we deduced that the ores from which
these slags derived came from one of the two bands in the Rooi-
water Complex, the nearest outcrop of which is about 15 km NW of
these sites.
In 1978 Killick was shown some smelting sites on the farms
Hasivona 561LT and Sivurahli 560LT, both of which are south east of
Tzaneen (Fig. 1), by local residents J. Witt and M. Klapwijk, who also
provided some slags for analysis. We do not have bulk chemical
analyses for these slags, but we examined a polished thin section
and two polished blocks from each site. All had very similar mi-
crostructures, dominated by large subhedral cubes and dendrites of
a spinel, with a small amount of late-forming ilmenite in jagged
laths and small amounts of interstitial dark brown glass containing
faint feathery dendrites of a silicate. Microprobe analysis of a thin
section from Sivurahli (Table 5) showed that the spinel was close to
the composition of ulvöspinel and that the ilmenite was also near
its ideal formula (FeTiO3). This thin section was very similar to that
previously described for site GM1M in the central Murchison
Range.
Killick also collected a block of magnetite from a smelting site on
the farm Broederstroomdrift 534LT, just northeast of Tzaneen
(Fig. 1). Chemical analysis of this block (Table 1, analysis TB1)
Fig. 13. Microstructure of ore from site TB1 near Tzaneen (reflected PPL, air). The large
featureless crystals are ilmenite. The speckled areas around them were originally
titaniferous magnetite, but have been largely oxidised to hematite (white). The black
areas between former magnetite grains are a microcrystalline mixture of haematite
and iron hydroxides, resulting from weathering of the magnetite.
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 14. Microstructure of slag from VS2M (reflected PPL, air). Dendrites of wüstite
(white) are surrounded by minute grey laths of fayalite or kirschsteinite in a darker
grey glass. The darker speckles within the dendrites and the overgrowths on them are
titaniferous magnetite.
showed 23.22% TiO2 and 0.99% V2O5. The microstructure (Fig. 13)
consisted of coarse crystals of unaltered ilmenite surrounded by
crystals of titaniferous magnetite that had been largely oxidised to
haematite. This ore sample clearly derived from the magnetitee
ilmenite bands of the Rooiwater Complex. The nearest outcrop is
that reported by Schwellnus et al. (1962, p. 16) in the Thabina River
about 25 km south of Tzaneen, but we have not sampled this and
there are no published analyses or micrographs of it. The ore
sample and slags could derive equally well from the upper
magnetite band of the Murchison Range north of Gravellotte, the
nearest outcrop of which is about 40 km east of Tzaneen (Fig. 1).
6.4. Slags from sites between the Murchison Range and the Schiel
Complex
Two slags from sites at Eiland (Fig. 1) were analysed (Table 3).
Slag sample EIL2M had 12.66 mass % TiO2 and 0.55% V2O5, which
suggested that the ore came from the isolated magnetite lens 33 km
SW of EIL2M at the contact between the Rooiwater Complex and
the Archaean granite (van Eeden et al., 1939; Reynolds, 1986). The
one analysis available from this lens (Table 1, analysis RW2) has the
lowest TiO2 content of any magnetiteeilmenite sample yet pub-
lished from the Rooiwater complex. (Samples from the lower band
have 14
16% TiO2 but their V2O5 content is much higher at 1.08e
1.37% - see Reynolds, 1986, Table 1). Sample EIL6M has 19.71 mass %
TiO2 and 0.95% V2O5, and thus used ore from the lower magnetitee
ilmenite band of the Rooiwater Complex, which is 25 km south of
the site.
A slag sample published by Evers (1982) from an intact furnace
(his 2330DA:2; our EIL1M) only 200 m distant from EIL2M has 14%
TiO2. Thus all three furnaces at Eiland from which we have analyses
used ores from the Rooiwater Complex magnetite-ilmentite bands,
but from three different locations within them.
We examined a thin section and three polished sections from
these sites. In polished section the dominant phase is a spinel in
subhedral cubes and octahedra, with variable but always subordi-
nate wüstite, metallic iron and short laths of a silicate as a late-
forming phase in the interstices between the oxide minerals.
Microprobe analyses of the late-forming silicates in one of these
samples (EIL2M) showed that at least two different minerals are
present. One is an olivine near to the end-member fayalite (analysis
249
EIL2Mb in Table 4). The other (EIL2Ma in Table 4) is the same un-
identified pyroxene previous noted in slags GR3M and GM1M from
the Murchison Range. The spinel (Table 5) is an ulvöspinel with
minor hercynite (FeAl2O4) in solid solution, and is very close in
composition to those already noted in slags GM1M, GR3M and
GR4M from the Murchison Range.
The thin silicate laths, though small, were better crystallised
than in other high-TiO2 slag samples. In thin section two different
silicates were noted. One was strong red-brown in PPL and had
inclined extinction in XPL; the other was colourless in PPL and had
third-order birefringence and straight extinction in XPL. These are
consistent with a clinopyroxene and an olivine respectively.
In 1978 two samples of slag from smelting sites to the east of the
Middle Letaba River e roughly on a line between Schiel and
Modjadji (Fig. 1) e were given to Killick by J. Witt of Tzaneen with
the co-ordinates of the sites from which they were collected. These
were analysed by WD-XRF (Table 3). The slag from site GAZ1M has
only 2.5 mass % TiO2, so we infer that this was produced with ore
from Schiel, which is about 23 km distant in a straight line. The
sample from the other site (GAZ2M) had 23.7% TiO2, and must
therefore have used ore from the upper band of the Rooiwater
Complex, the nearest outcrop of which is a straight-line distance of
73 km south of this site. This is the greatest distance between ore
source and smelting site yet documented in the Lowveld.
6.5. Slag from a site on the Schiel Complex
Slag sample VS2M in Table 3 was from the well-preserved
furnace depicted in Miller et al. (2002) on the farm Schuyn-
shoogte. This site is within 1 km of the ancient magnetite mines of
the Schiel Complex. As expected from the known composition of
the Schiel magnetite, the TiO2 content of this slag was very low. This
particular sample was more diluted by undissolved silica than were
most other slags, so the original TiO2 content of the ore would have
been about 1.0 mass %. One thin section and one polished block
were examined. The thin section was dominated by fine dendrites
of wüstite in a matrix of tiny skeletal laths of a silicate and glass
(Fig. 14). It was therefore richer in iron than the bulk chemical
analysis. Almost all of the wüstite dendrites had exsolved tiny cubes
of a darker phase, and a few had overgrowths of pink titaniferous
magnetite. Electron microprobe analysis of the very small laths
(Table 4) showed that they were complex silicates rich in titania
and alumina. The polished block had much less wüstite and more
titaniferous magnetite and silicate laths. It also had many eutectic
intergrowths (Fig. 15) of iron oxide in kalsilite (KAlSiO4). We as-
sume that abundance of the latter mineral in this section reflected
the presence in the sand used as flux of a substantial amount of
potassium feldspar from the syenite hills around the Schiel
Complex.
7. Metallographic analyses
There was very little iron preserved on any of the excavated
sites. The soils of the region are extremely acid, and preservation
depends strongly on a favourable microenvironment, like burial in
an alkaline ash deposit. This is illustrated by the fact that the iron
artefacts from Nagome, a 19th century site, were completely oxi-
dised, while the iron bead and iron strip from SPK3 (11th
12th
centuries cal CE) still contained metal. We examined an iron bead
and an iron strip from SPK 3. Both were made from bloomery iron.
They showed elongated stringers of slag, composed of wüstite in a
dark glass, transversely fractured by working below the glass
transition temperature, which is generally between 500 and 700  C
(Babcock, 1977, p.26). Etched in nital, the bead (SPK3.1) consisted of
annealed equiaxed ferrite with a grain size of ASTM 6
7 (ASTM,
250 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Fig. 15. Slag from VS2M with inferred higher potassium and titanium content than
that in Fig. 14 (reflected PPL, air). Initial crystallisation of rounded dendrites of wüstite
(white) was followed by subhedral cubes of titaniferous magnetite light (grey), and
then by and eutectic intergrowths of wüstite (white) and kalsilite (black). The last
phase to crystallize was fayalite, which is the large parallel-sided light grey lath in the
upper half of the picture.
1981), with intergranular pearlite islands. The overall carbon con-
tent was about 0.1e0.2%. Elongated grains on the outer perimeter
and near the cut ends were evidence of cold work subsequent to the
final anneal. The bead had been cut out of strip and bent or
hammered to shape cold. The average Vickers microhardness was
HV 137 (200 g for 10 s, n ¼ 9, range 112e156), the relatively high
hardness reflecting extensive internal strain from cold work. A
raster EDAX analysis detected only iron.
The iron strip (SPK3.2) consisted of very fine grained ferrite
(about ASTM 10), due to annealing after heavy cold work. There was
prominent banding with variation in grain size and carbon content,
probably due to variations in phosphorus content. The overall
carbon content was low, around 0.1%, but was difficult to assess
because of the inhomogeneity. The Vickers microhardness was
relatively high for a ferritic microstructure, probably due to phos-
phorus in the segregation banding, with an average of HV 142
(n ¼ 5, range 134e154). A raster EDAX analysis in the SEM detected
only iron as a major element. A spot analysis of a glassy inclusion
indicated an iron silicate glass composition with about 4% phos-
phorus, 3% calcium and 2% potassium.
The microstructures and fabrication technology of these iron
artefacts were typical of indigenous bloomery in southern Africa
(Miller, 2002). No larger items of iron were recovered in excava-
tions. Six iron tools recovered during surface survey have been
studied by Gordon and van der Merwe (1984). These had inho-
mogeneous air-cooled microstructures of ferrite or air-cooled steel,
with carbon contents up to 1 mass % C and numerous slag in-
clusions. Two of the six objects had slag inclusions with high levels
of TiO2, indicating that they were smelted from the magnetitee
ilmenite ores of the Murchison Range. The lack of evidence for heat-
treatment of steel in these hoes conformed to the usual practice in
the southern African Iron Age (Miller, 2002).
8. Discussion
8.1. The use of magnetite and magnetiteeilmenite ores
The Late Iron Age iron smelting technology of the northern
Lowveld has several unusual aspects, both within the context of
African iron smelting and also within the totality of bloomery
smelting technologies in the Old World. Most African bloomery
smelters used laterite ores, which are products of intensive
weathering on old stable land surfaces. The dominant iron minerals
in laterites are iron hydroxides, which lose water in the early stages
of smelting, creating open porosity that allows carbon monoxide
access to the interior. This promotes rapid reduction to iron
throughout lumps of ore (Killick, 1990; Killick and Gordon, 1988).
But laterite ores cannot form on eroding landscapes like those of
the Lowveld, so ironworkers there had to learn how to smelt the
available magnetite and magnetiteeilmenite ores. It is not yet clear
when they first did this. The oldest date for iron slag in a securely
dated context in this region is at Silverleaves (Klapwijk and
Huffman, 1996), which is on the escarpment near Tzaneen (Fig. 1)
and is associated with a radiocarbon date of 1680  55 BP (Pta-901),
but it is not known what ore was used to produce it.
In global context, magnetites were rarely used in bloomery
furnaces because of their lack of porosity. Reducing magnetite is
like peeling an onion; reduction proceeds from the exterior of the
grain to the interior, with shells of reduced iron spalling off to allow
carbon monoxide to react with the next layer of oxide (Killick and
Gordon, 1988). This is well illustrated in Fig. 10, which shows an
incompletely reduced piece of magnetite in a slag sample from
IL8M.
The reduction of lumps of magnetite to iron metal is therefore
much slower than reduction of similarly-sized lumps of hydroxide
ores like laterites or bog iron. To ensure complete reduction as the
ore descends through the furnace stack (which in the case of
bloomery furnaces is often less than one metre tall), magnetite
must be charged to the furnace as very small grains. Thus almost all
published instances of the use of magnetite ores in hand-blown
bloomery furnaces have noted the use of “black sands”, recovered
from streams or beaches, with an average grain size of 1e2 mm. The
magnetites in these sands originated as accessory minerals in
igneous rocks. These were freed by erosion and concentrated by
streams or wave action because of their relatively high specific
gravity.
Most of these records are from Africa (Cline, 1937; Brown, 1995;
David et al., 1989; Ige and Rehren, 2002; Iles and Martínon-Torres,
2009). Other recorded instances are from Macedonia (Photos et al.,
1984), Japan (Rostoker et al., 1989), Taiwan (Chen, 2000) and Korea
(Park and Rehren, 2011). The sands were typically beneficiated by
washing or winnowing to raise their iron content, but still con-
tained enough aluminosilicate minerals to form a slag. Slag is
required in most bloomery furnace designs for two reasons: (1) it
transports the small grains of iron to the base of the furnace, and
then drains away, pulling the iron grains together to form the
bloom; and (2) it protects the small grains of iron from reoxidation
as they pass through the oxidising zone at the mouths of the
tuyères.
The use of magnetite ores with up to 20% TiO2 was noted in an
exploratory study of iron production at the 19th century site of
Marothodi near Rustenburg on the margins of the Bushveld Com-
plex, although the source of these ores is unknown (Hall et al.,
2006). The only other cases, to our knowledge, where massive
magnetite ores were used in bloomery furnaces were in Korea in
the early first millennium CE (Park and Rehren, 2011) and in the
19th century iron industry of upper New York State, USA (Gordon
and Killick, 1992, 1993). The technology of the Korean bloomeries
has not yet been published in detail. The New York furnaces
employed water-powered bellows and preheated blast, and hence
are not directly comparable to the technology discussed here.
In the Lowveld bloomery furnaces, massive magnetite or
magnetiteeilmenite ores containing less than 3 mass % silica were
used. These had to be crushed to sand size, and silica or
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255 251

Table 3
Chemical analyses of iron-smelting slags from the Lowveld, made by wavelength-dispersive X-ray fluorescence (WD-XRF) analysis of glass fusion discs (method of Norrish and
Hutton (1969). The samples are labelled by site; suffixes (a, b, c, d) indicate analysis of two or more samples per site.

Sample SiO2 TiO2 Al2O3 Fe2O3 FeO MnO MgO CaO Na2O K2O P2O5 V2O5 NiO CO2 H2Oþ H2O- TOTAL

Phalaborwa
SPM2a 30.79 4.42 6.58 7.42 33.34 0.19 2.65 10.09 0.94 2.20 0.42 0.18 0.07 0.58 0.30 0.13 100.3
SPM2b 23.60 7.62 4.63 2.12 42.39 0.28 3.48 12.05 0.30 1.87 0.66 0.12 n.d. 0.30 0.06 0.06 99.54
SPM2c 53.52 2.31 11.28 4.57 14.47 0.12 2.02 5.73 1.81 3.02 0.26 0.07 0.24 0.26 0.10 0.10 99.88
SPM3a 36.66 4.70 7.74 8.33 27.86 0.22 2.71 6.72 1.14 2.22 0.35 0.16 0.30 0.30 0.10 99.51
SPM3b 22.73 6.45 4.55 6.13 40.56 0.28 3.60 11.34 0.51 1.84 0.58 0.22 0.06 0.48 0.24 0.10 99.67
SPM4a 21.34 6.99 4.86 5.64 40.58 0.25 3.44 12.31 0.58 1.46 0.61 0.24 0.05 0.36 0.26 0.09 99.06
SPM4b 19.19 4.25 4.79 7.25 45.51 0.23 3.60 11.80 0.62 1.71 0.55 0.16 0.06 0.40 0.18 0.20 100.5
Mashishimali hills
PQ1Ma 20.10 4.39 4.76 9.50 43.34 0.28 3.77 9.71 0.47 1.37 0.60 n.d. n.d. 0.56 0.40 0.42 99.67
PQ1Mb 20.25 4.68 4.28 6.83 43.40 0.24 3.60 12.33 0.44 1.45 0.58 n.d. n.d. 0.72 0.22 0.25 99.27
PQ1Mc 21.89 4.73 4.48 6.14 40.62 0.26 3.67 13.68 0.44 1.53 0.69 n.d. n.d. 0.66 0.20 0.36 99.35
PQ1Md 17.85 4.13 4.12 9.79 45.52 0.24 3.50 10.59 0.41 1.27 0.50 n.d. n.d. 0.36 0.16 0.29 98.73
IL6M 32.45 0.55 7.00 15.79 36.86 0.08 0.76 3.08 1.03 2.13 0.25 0.03 0.17 0.32 0.36 0.36 101.22
IL8M 10.21 15.01 4.86 10.01 50.04 0.31 1.70 4.32 0.24 0.69 0.13 1.47 0.13 0.40 0.40 0.27 100.19
Murchison range
GR3Ma 17.16 20.90 5.37 2.62 40.59 0.30 1.20 7.54 0.12 0.83 0.42 0.91 0.06 0.48 0.26 0.17 98.93
GR4Mb 11.83 23.87 3.97 8.89 41.83 0.37 1.56 4.47 0.05 0.63 0.28 0.79 0.11 0.18 0.06 0.08 98.97
GR6Ma 12.94 21.13 5.20 8.53 42.23 0.30 0.99 6.10 0.13 0.53 0.23 0.79 0.01 0.46 0.40 0.09 100.06
GM5M 7.44 25.18 3.97 5.53 48.99 0.36 1.42 3.36 0.06 0.60 0.13 1.28 0.08 0.22 0.08 0.07 98.77
GM7M 19.29 21.31 5.15 2.42 37.4 0.75 1.14 9.13 0.19 0.95 0.30 0.81 0.08 0.40 0.28 0.22 99.82
GM11M 17.55 21.86 5.24 2.70 38.55 0.41 0.93 9.58 0.21 1.04 0.32 0.96 0.09 0.38 0.2 0.06 100.08
North of Murchison
EIL2M 19.36 12.66 4.86 9.14 41.56 0.40 1.92 6.40 0.22 0.52 1.10 0.55 0.03 0.36 0.52 0.25 99.85
EIL 6M 10.43 19.71 3.86 13.76 45.31 0.25 0.72 2.88 0.17 0.47 0.08 0.95 0.02 0.24 0.18 0.33 99.34
GAZ1M 27.51 2.50 6.22 6.97 40.68 0.51 2.43 7.39 0.10 3.02 1.46 0.15 0.00 0.18 0.16 0.06 99.34
GAZ2M 12.37 23.67 4.58 5.40 42.49 0.39 1.02 6.45 0.13 0.74 0.36 0.70 0.01 0.22 0.24 0.09 98.86
Schiel complex
VS2M 41.37 0.49 10.37 1.66 36.68 2.01 0.82 0.65 0.23 0.96 1.75 0.02 0.38 0.68 0.64 0.48 99.19

aluminosilicate flux then had to be added to form slag. At all Pha-
laborwa sites and at PQ1M ‘Square’ (van der Merwe and Killick,
1979) pieces of crushed magnetite 5
10 mm were recovered with
a magnet from around the furnaces, and the large syenite boulders
and bedrock around Kgopolwe hill (the locus for sites and samples
with a prefix of SPK) are pockmarked by grinding hollows, from
which magnetite grains can still be extracted with a magnet. The
final size for ore presented to the furnace is not known, but we
assume that it was probably less than 2 mm, as we have rarely seen
pieces of incompletely reacted ore in the slags that we have studied
in polished section (although one of these is shown in Fig. 10).
8.2. The smelting furnaces
Archaeological evidence shows that two types of smelting
furnace were employed in the Lowveld in the second millennium
CE. A forced-draft shaft furnace with three tuyères was used to
smelt iron, while a much smaller domed furnace, blown through a
single tuyère, served for smelting copper (Evers and van der
Merwe, 1987; Miller et al., 2001). All intact iron smelting furnaces
recorded to date, whether triangular or circular in plan, had shaft
heights of about one metre and had three vertical slits 120 apart,
sometimes extending the full height of the shaft, separated by a
distance of 1.0e1.2 m from the opposite wall. These slits were
clearly for insertion of tuyères, and there is good evidence on some
furnaces that the slits above the tuyères were plastered shut when
the furnace was in use. Since used tuyères on these sites are typi-
cally slag-wetted for 15
20 cm from the nose, we assume that a
single iron bloom accumulated in the centre of the furnace, and that
the purpose of the slits was to allow the solid bloom to be levered
out, using three poles, without damaging the furnace walls. It is
clear from the map of PQ1M (Fig. 5) that these furnaces could be
used for many smelts. Bag bellows made of leather were used in the
Soutpansberg in the late 19th century (Junod, 1927; Miller et al.,
2002) and we assume that they were also used in earlier times,
as there is no historical record of the use of carved wooden or fired
ceramic pot bellows in South Africa. Slag was not tapped from these
furnaces.
In the hills around the Phalaborwa Complex (Pistorius, 1989,
Evers and van der Merwe, 1987), at Eiland (Evers, 1975, 1981,1982)
and in the foothills around Tzaneen (Klapwijk, 1986) all iron
smelting furnaces recorded to date have a triangular plan, with a
vertical slit at each apex. In the Mashishimali Hills (van der Merwe
and Killick, 1979) and in the Soutpansberg (Miller et al., 2002) they
have a circular plan. Another variable aspect of furnace design is the
presence or absence of a small cylindrical pit, sometimes found
covered by a flat slab of stone, in the centre of the floor of the
furnace. Where present, most of these are empty, but finds of hu-
man finger bones in several such pits around Phalaborwa (Plug and
Pistorius, 1999) suggest that their function was to provide protec-
tion against magical spells cast by others.
8.3. The use of sand flux and the effect of wood ashes
As all the potential ores in this region are essentially pure iron
and titanium oxides, it was obvious from the beginning of this
study that a silicate flux must have been added to the furnace
charge to produce slag. The FeOeSiO2 phase diagram (Levin et al.,
1964, Figs 80 and 81) shows that pure FeO melts at 1377  C un-
der atmospheric conditions. In practice a temperature at least
100  C above this would be required to provide a free-flowing slag,
and it would be very difficult to maintain a temperature around
1500  C in a hand-powered bloomer furnace. But if the FeO is fluxed
with between 20 and 40 mass % SiO2, liquidus temperatures are
lowered into the range 1178e1205  C (Levin et al., 1964, Figs 80 and
81). With 100  C superheat to ensure free flow this translates to
1200
1300  C, a range of temperature easily attained under
reducing conditions in a bloomery furnace.
252 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255

Table 4
Electron microprobe analyses (in mass %) of silicates in thin sections of slags from selected sites.

Sample SiO2 Al2O3 TiO2 FeO MnO MgO CaO Na2O K2O P2O5 Total Comment

Phalaborwa
SPM3 32.11 0.22 0.38 33.06 0.27 5.61 26.65 0.23 0.12 0.90 99.55 Kirschsteinite
Mashishimali hills
PQ1Mb 32.44 0.24 0.38 33.12 0.33 6.76 24.92 0.15 0.21 0.66 99.21 Kirschsteinite
Murchison range
GR3M 39.53 8.48 7.22 18.62 0.21 2.85 22.55 0.17 0.01 0.45 100.09 Pyroxene
GM1M 41.48 7.05 4.53 22.53 0.21 1.73 22.25 0.11 0.01 nd 99.90 Pyroxene
North of Murchison
EIL2Ma 39.53 9.76 5.67 19.69 0.21 2.34 21.61 0.21 0.16 nd 99.18 Pyroxene
EIL2Mb 31.13 0.20 0.57 58.05 0.74 6.68 2.34 0.02 0.04 nd 99.77 Olivine
Schiel complex
VS2M 26.31 13.41 8.58 33.32 0.26 4.73 12.67 0.11 0.06 0.18 99.63 Unidentified

The composition of the slags (Table 3) differs from that of the
magnetite ores (Table 1) mainly in the much higher SiO2, Al2O3 and
CaO contents of the slags. Silica and alumina could potentially have
entered the slag from chemical attack of the tuyères and furnace
walls by liquid iron oxides, but inspection of the analyses in Table 3
will show that the silica to alumina ratios are in most cases
significantly higher than the 3:1 ratio in illite, the dominant clay
mineral in Lowveld soils. Crushed quartz could have been added,
and some was noted around the furnaces at PQ1M (van der Merwe
and Killick, 1979), but another possible flux is the granitic sand that
is ubiquitous in Lowveld stream beds. In 1978 Killick collected
samples of sand for chemical analysis from the bed of the Selati
River. These sands derive from the Archaean granite gneiss that
forms the bedrock over most of the northern Lowveld.
In Table 6 we compare the compositions of a Rooiwater ore
(from Table 1), two analyses of sands from the Selati River, and a
slag from the Mashishimali Hills (from Table 3). This suggests that
addition of these sands can explain the elevation of SiO2, Al2O3, K2O
and Na2O concentrations in the slag, and the corresponding dilu-
tion of TiO2 and iron oxides. However, it cannot explain the high
levels of CaO in the slags (Table 3). The sands contain more K2O
than CaO, but all the slags contain much more CaO than K2O. The
most likely explanation for this inversion is that most of the CaO
derives from the ash content of the charcoal fuel. The preferred tree
for making charcoal in the Lowveld today is leadwood, Combretum
imberbe. When burned this produces copious quantities of white
ash. We analysed one sample of ash from this species and found
that it was about 90 mass % CaO when H2O and CO2 were removed
from the analysis and the total normalised to 100%. Slags from the
vicinity of the Phalaborwa Complex tend to have higher CaO con-
tents than those derived from the magnetiteeilmenite ores of the
Rooiwater Complex (Table 3). This is a real difference, as the totals
of (SiO2 þ TiO2 þ Al2O3) vary within the same range e 35e45 mass
% e in both groups. We cannot explain why this should be the case.
Magnetite is associated with calcite in the carbonatite and phos-
corite members of the Phalaborwa Complex, but the relatively high
TiO2 levels in the slags from adjacent sites (those with SPM prefixes
in Table 3) show unequivocally that the magnetite ore use to pro-
duce them came from the pyroxenite member of the Phalaborwa
Complex, in which calcite is not abundant (Hanekom et al., 1965). It
is possible that the differences in the CaO contents reflect the use of
different species of charcoal to smelt ore from the Phalaborwa and
Rooiwater Complexes, but we have not identified the tree species
used to produce the charcoal at each site.
8.4. The high titanium slag system
Many of the slags reported here have from 12 to 25 mass % TiO2.
We can find no published record of such high levels of TiO2 in
bloomery iron smelting slags. These slags also have very unusual
microstructures, with up to 90% by area in polished section con-
sisting of crystals of ulvöspinel, a mineral that is seen in geological
contexts only as exsolved oxidation lamellae within crystals of
magnetite (Haggerty, 1991). One of our more interesting findings is
that slags with 20e25 mass % TiO2 do not seem to have been any
less fluid than those with less than 10% TiO2. Slags that solidified
among charcoal pieces have smooth glossy well-rounded surfaces,
while those from the pool of slag at the furnace base form dense
blocks without visible boundaries between flows. The high-TiO2
slags produced from the Rooiwater ores are black in freshly broken
section, while those with lower TiO2, deriving from Phalaborwa and
Schiel ores, are usually medium grey. No evidence for the tapping of
liquid slag from the furnaces was noted.
It appears that in bloomery furnaces TiO2 is essentially equiva-
lent to SiO2
neither is reduced, and both form highly fluid slags by
reaction with FeO. The minimum liquidus temperature in the

Table 5
Electron microprobe analyses (in mass %) of oxide phases in thin sections of slags from selected sites.

Sample MgO Al2O3 TiO2 Cr2O3 FeO MnO SiO2 CaO V2O3 NiO Total Comment

Mashishimali hills
PQ1Mb 1.45 4.63 24.83 0.07 66.60 0.22 0.87 0.57 0.24 0.01 99.52 Spinel
Murchison range
GR3M 0.82 2.55 32.77 0.16 63.00 0.46 0.08 0.20 0.44 0.02 100.51 Spinel
GR4M 1.10 2.95 27.67 0.18 67.26 0.32 0.08 0.03 0.68 0.01 100.26 Spinel
GM1M 0.86 2.50 32.96 0.21 63.23 0.36 0.08 0.04 0.83 0.02 101.09 Spinel
GM1M 0.86 0.29 52.63 0.08 46.62 0.41 0.04 0.11 0.38 0.01 101.43 Ilmenite
GR3M 5.37 1.54 71.37 0.41 17.31 0.28 0.28 0.87 3.99 0.02 101.44 Unidentified
Near Tzaneen
Sivurahli 1.39 3.86 33.98 0.21 60.11 0.50 0.05 0.06 0.87 0.01 101.03 Spinel
Sivurahli 1.35 0.19 52.00 0.10 45.14 0.63 0.39 0.46 0.14 0.01 100.32 Ilmenite
North of Murchison
EIL2M 1.25 3.48 30.50 0.32 62.75 0.41 0.15 0.19 0.64 0.02 99.70 Spinel
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255 253

Table 6
Chemical analyses of a magnetiteeilmenite ore (from Reynolds (1986) and Table 1), two sands from the bed of the Selati River (Killick, unpublished) and slag from site IL8
(Table 3). This comparison is for illustration only; it is not suggested that this ore produced this slag.

Sample SiO2 TiO2 Al2O3 Fe2O3 FeO MnO MgO CaO Na2O K2O P2O5 V2O5 CO2 H2Oþ H2O- Total

Ore RW27 2.66 20.83 3.83 48.37 22.50 0.32 1.68 n.d. n.d. n.d. n.d. 0.80 n.d. n.d. n.d. 100.99
Sand A 84.69 0.14 7.57 0.22 1.09 0.01 0.29 0.92 2.41 2.16 0.02 0.00 0.20 0.16 0.03 99.91
Sand B 76.91 0.11 11.88 0.24 1.18 0.02 0.30 1.34 2.99 4.12 0.04 0.00 0.20 0.21 0.03 99.56
Slag IL8M 10.21 15.01 4.86 10.01 50.04 0.31 1.70 4.32 0.24 0.69 0.13 1.47 0.40 0.40 0.27 100.06

binary system TiO2eFeO is 1300  C, near the limit for average
temperature across the entire profile of a bloomery furnace, so
some SiO2 must be added to FeOeTiO2 to obtain slags that melt in
the optimal range for the bloomery furnace (1100
1200  C). Liq-
uidus temperature as low as 1145  C occur in the system TiO2e
FeO(n)eSiO2 under reducing conditions (Fig. 8). Comparison of the
chemical compositions of ore (Table 1) and slag (Table 3) compo-
sitions shows the ironworkers of the Lowveld invariably added
siliceous flux. The actual melting temperatures of these slags are
affected by oxides not accounted for in the phase diagram, espe-
cially CaO and Al2O3, but it seems safe to say that they would be
under 1250  C.
8.5. The presence of ferric iron
8.6. The mass balance and yield
Unfortunately it is not possible (contra van der Merwe and
Killick, 1979) to calculate the mass of magnetite required to pro-
duce a given mass of slag, nor to infer the yield of iron from our
chemical analyses of ores and slags. This is because we cannot know
how much slag was produced in each smelt. Since the magnetites
from the carbonatite complexes are not self-fluxing, the amount of
slag formed was determined by the quantity of aluminosilicate flux
that the smelters chose to mix with the crushed ore. Too little flux
would adversely affect the fluidity of the slag, and thus the
consolidation of the bloom; too much would lower the yield of iron
metal. The ratio of magnetite to flux in the furnace charge cannot be
inferred from the composition of the slag.

In all of these slags metallic iron coexists with ferric iron (Fe3þ),
which is not possible under equilibrium conditions. Table 3 shows
that ferric iron (determined by titration) accounts for between 2
and 16 mass % of these slags. Some of this may be due to subsequent
corrosion, but few specimens showed any signs of it, either in hand
specimen or when examined in thin section or polished blocks. We
have noted mineralogical and chemical evidence in some slags for a
change of atmosphere from reducing to oxidising while the slags
were partially molten, almost certainly because the slits above the
tuyères were in some cases opened to extract the bloom while hot.
We suggest that most of the ferric iron is therefore in the last
minerals to crystallise and in the glass.
The electron microprobe cannot distinguish between the
different valence states of elements, and thus valence must be
assumed when calculating microprobe data as oxides. By conven-
tion, iron in electron microprobe analyses is calculated as FeO, but
various post-hoc schemes for deriving the proportion of ferric iron
in particular minerals from microprobe analyses have been pro-
posed. Since ulvöspinel solid solutions are by far the most abundant
minerals in our titanium-rich slags, we also checked whether there
could be ferric iron in some of the spinels. We calculated the pro-
portion of ferric iron from the microprobe analyses of spinels in
Table 5 according to the widely-used recalculation scheme of
Carmichael (1967) and obtained the following results:
GR4M 55.84% FeO 12.70% Fe2O3
GR3M 60.35% FeO 2.95% Fe2O3
GM1M 60.96% FeO 2.62% Fe2O3
Sivurahli 60.99% FeO
0.98% Fe2O3
These results suggest that in at least one specimen (GR4M) the
spinel is a solid solution of titaniferous magnetite in ulvöspinel. In
the other three cases the calculation shows that the iron is almost
all ferrous, and thus that most of the ferric iron in the bulk analyses
must be in another phase (magnetite?) or in the glass. Neither of
the silicate phases in these slags can contain much ferric iron
because their totals in microprobe analysis are close to 100%
(Table 5).
8.7. Provenance of iron ores
We have shown that chemical analysis of slags from archaeo-
logical sites in the Lowveld provides unequivocal evidence of the
sources of the iron ores used to produce the slags. The Phalaborwa
and Schiel Complexes are essentially point sources at the scale of
the region shown in Fig. 1, while the main exposure of the
magnetite-ilmentite bands in the Rooiwater Complex is only about
14 km long, with two smaller outcrops between this and the
western escarpment. The ore, being very dense, was not moved any
significant distance from outcrop by alluvial processes, so it is easy
to establish the minimum distance over which ore must have been
carried.
Ore was in several instances carried more than 20 km to
smelting sites, and in one case (GAZ2M) more than 70 km. Oral
histories also mention ore being carried as far as 55 km from the
Schiel Complex (Giesekke, 1930; Krige, 1941). In the tradition
recorded by Giesekke (1930) the use of human porters is specif-
ically mentioned. PQ1M, the largest smelting site in the region, has
an estimated 180,000 kg of slag (van der Merwe and Killick, 1979).
From the site plan (Fig. 5) it appears that this was produced in a
relatively short span of time. We cannot accurately estimate the
quantity of ore brought from the Phalaborwa Complex, 20 km away,
but it clearly must have exceeded 200,000 kg. With no historical
evidence for the use of pack animals to transport ore in the Low-
veld, this represents several thousand man-journeys. We do not
know why the scale of iron production is so much larger at PQ1M
than at any other site in the region. There is no obvious explanation
to be found in distribution of resources
both fuel wood and clay
would have been available much closer to the ore source. There is
unfortunately too little supporting archaeological and historical
data for us to decide whether: (a) the Phalaborwa ore deposit was
an open resource, owned by no-one, or (b) access to the ore deposit
reflected alliance with, or a negotiated agreement between, a group
asserting ownership of this ore source and a group resident in the
Mashishimali Hills.
We have demonstrated that the source(s) of ore for iron
smelting sites in the northern Lowveld can be established by
chemical analysis of the slag. This provides archaeologists in this
region with the means to study the regional organisation of iron
254 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
production. Slag inclusions trapped in iron artefacts produced in
this region can also be related to the source of ore used to produce
them (Gordon and van der Merwe, 1984). The main barrier to
reconstructing the regional organisation of iron production is that
of dating the sites. Many of the radiocarbon dates cited in this
article are less than 300 BP, and thus fall into a well-known “black
hole” in the radiocarbon calibration curve. (After calibration at two
sigma, all dates in the range 300
50 BP fall in the unhelpful cal-
endar age range of ca. 1640
1900 CE). The fact that most of the
radiocarbon dates for iron production in the northern Lowveld are
300 BP or less reflects the preferences of archaeologists for exca-
vating well-preserved furnaces. Iron production in the Lowveld
goes back at least to the 11th
12th centuries cal. CE (as shown by
the iron samples from SPK 3, described above) and to at least 350e
450 cal. CE on the western escarpment (Klapwijk and Huffman,
1996). Radiocarbon dating has useful precision for investigating
the prehistory of iron production in the Lowveld before ca. 1640 cal.
CE (see Fig. 2 in Miller et al., 2001), but all more recent sites will
need to be redated by archaeomagnetic dating, thermolumines-
cence or optically-stimulated luminescence dating of furnace
ceramics.
9. Conclusions
This study reports the direct smelting of bulk magnetitee
ilmenite ores, with slags containing up to 25% TiO2 as the principal
waste product. Although these ores are of potential interest today
as sources of titanium and vanadium, they cannot be used to pro-
duce iron in modern blast furnaces. In the highly reducing atmo-
sphere of the blast furnace, titanium 4þ oxides are reduced to
mixtures of titanium nitride (TiN), titanium carbide (TiC) and Ti2þ
and Ti3þ oxides, which in combination make blast furnace slags
unacceptably viscous (McGannon, 1971). Even the magnetites of
the Phalaborwa Complex, which have much lower titanium con-
tents than those of the Rooiwater Complex, are mostly unusable
today. A few million tons with TiO2 content below 2 mass % have
been sold, but hundreds of millions of tons of powdered magnetite
with higher TiO2 concentrations reside in waste dumps around the
modern copper mine. Yet the Late Iron Age metalworkers of the
Lowveld had no difficulty in producing pure iron and highly fluid
slags from titaniferous magnetite ores by employing the bloomery
process.
Although there is evidence of the bloomery smelting of
magnetite sands elsewhere in sub-Saharan Africa, and occasional
reports from elsewhere (Japan, Korea, Taiwan, Macedonia and the
eastern United States), this is the first published study to report the
smelting of high-titanium iron ores. This finding serves to
emphasize the point that though the bloomery smelting process
was less productive than the blast furnace process, it was far more
versatile. Bloomeries can smelt iron ores with high levels of
phosphorus, arsenic, antimony, aluminium and nickel (Rostoker
and Bronson, 1990), none of which are suitable for modern blast
furnaces. To this list we can now add iron ores high in titanium and
vanadium.
There is little evidence of any human occupation of the northern
Lowveld in the first millennium CE, but in the second millennium
(the Later Iron Age) settlers appear to have been attracted to this
region by its wealth of inorganic resources, mostly metal ores and
saline springs from which salt could be obtained (Evers, 1981). We
do not believe that settlers were specifically attracted to the Low-
veld by the vast quantities of magnetite and magnetiteeilmenite
ores in the region. As we shall show in a separate study (in prep-
aration), the saline springs and copper ores of the Lowveld were the
main attraction. But the settlers would have needed iron, and
through experiment they successfully adapted bloomery smelting
techniques to unfamiliar ores. Whether iron was ever exported
from the Lowveld west to the Highveld, or east to Mozambique, is a
question for future researchers to investigate. But within the
Lowveld future archaeological studies can use the composition of
ore or slag fragments on smelting sites as evidence for the distances
travelled to procure ores.
Acknowledgements
Most of the sites reported here were discovered by teams led by
Professor Nikolaas van der Merwe between 1970 and 1973. In the
mid-1970s both of the present authors were undergraduate stu-
dents in geology and archaeology at the University of Cape Town
(UCT), and were encouraged by van der Merwe to take up the study
of archaeometallurgy by working on this material, which we have
done intermittently over the last thirty five years. We are both most
grateful to him for his mentorship, support and friendship. This
work could not have been carried out without the generous help of
Jurgen Witt and Menno Klapwijk, both of Tzaneen, and of Charles
More, Ike Lombaard and Jan Scholtemeyer, all of Phalaborwa. Each
of them shared with us their deep knowledge of indigenous mining
and metal working in the northern Lowveld. We also wish to thank
the Department of Archaeology, UCT for access to specimens in
their care, and Professor Nikolaas van der Merwe, Professor W. J.
Verwoerd, Dr Julius Pistorius, Dr Udo Küsel, Professor Thilo Rehren
and Professor Robert Heimann for valuable discussion. We are most
grateful to the Phalaborwa Mining Company and to FOSKOR for
allowing us to use data from unpublished reports. For assistance in
the analysis of samples we thank: the Director, Electron Microscope
Unit, UCT; the Department of Geochemistry, UCT (and especially Dr
Andy Duncan and Dr James Willis); and at the University of Arizona,
Gary Chandler for assistance with electron microscopy, Dr Ken
Domanick for the electron microprobe and Mr. Phil Anderson for X-
ray diffraction. Archaeological fieldwork by van der Merwe’s team
was funded by a Ford Foundation Foreign Area Fellowship and by
National Science Foundation Grants GS-281 and GS-2744. Analysis
of samples was partly funded by National Science Foundation Grant
SBR-9602033 to Killick, and partly by multiple grants to Miller from
the National Research Foundation, South Africa, Anglo American
PLC, De Beers PLC, and AngloGold PLC. We are most grateful to all
these institutions for their support and to the three referees whose
detailed criticisms and suggestions significantly improved this
paper. Opinions expressed in this report, and conclusions arrived at,
are those of the authors and are not to be attributed to any of the
supporting agencies.
References
ASTM, 1981. Standard Methods of Estimating the Average Grain Size of Metals. In:
ASTM Standards e Part II. E 112. American Society for Testing and Materials,
Philadelphia, PA, pp. 186e220.
Babcock, C.L., 1977. Silicate Glass Technology Methods. Wiley, New York, NY.
Bernhard, F.O., 1971. Karl Mauch, African Explorer. Struik, Cape Town.
Brandl, G., Cloete, M., Anhaeusser, C.R., 2006. Archaean greenstone belts. In:
Johnson, M.R., Anhaeusser, C.R., Thomas, R.J. (Eds.), The Geology of South Africa.
Council for Geoscience, Pretoria, pp. 9e56.
Brown, J., 1995. Traditional Metalworking in Kenya. In: Cambridge Monograph in
African Archaeology, vol. 38. Oxbow Books.
Carmichael, I.S.E., 1967. The iron-titanium oxides of sialic rocks and their associated
ferromagnesian silicates. Contrib. Mineral. Petrol. 14, 36e64.
Ph.D. thesis Chen, K.T., 2000. Ancient Iron Technology of Taiwan. Harvard
University.
Cline, W.W., 1937. Mining and Metallurgy in Negro Africa. George Banta Publishing
Company, Menasha, WI.
David, N., Heimann, R., Killick, D.J., Wayman, M., 1989. Between bloomery and blast
furnace: Mafa iron-smelting technology in North Cameroon. Afr. Archaeol. Rev.
7, 185e210.
de Waal, J.B., 1942. Ysterbewerking deur die Bawenda en die Balemba in Sout-
pansberg. Tydskr. vir. Wet. Kuns 3, 45e53.
 D. Killick, D. Miller / Journal of Archaeological Science 43 (2014) 239e255
Evers, T.M., 1975. Recent iron age research in the eastern Transvaal, South Africa.
South Afr. Archaeol. Bull. 30, 71e83.
Evers, T.M., 1981. The iron age in the eastern Transvaal. In: Voigt, E.A. (Ed.), Guide to
Archaeological Sites in the Northern and Eastern Transvaal. Transvaal Museum,
Pretoria, pp. 64e109.
Evers, T.M., 1982. Two later iron age sites on Mabete, Hans Merensky Nature
Reserve, Letaba District, NE Transvaal. South Afr. Archaeol. Bull. 37, 63e67.
Evers, T.M., van der Merwe, N.J., 1987. Iron age ceramics from Phalaborwa, north
eastern Transvaal Lowveld, South Africa. South Afr. Archaeol. Bull. 42, 87e106.
Giesekke, E.D., 1930. Die Eisenindustrie der Bawenda. Die Brücke, pp. 5e9.
Gordon, R.B., Killick, D.J., 1992. The metallurgy of the American bloomery process.
Archeomaterials 6, 141e167.
Gordon, R.B., Killick, D.J., 1993. Adaptation of technology to culture and environ-
ment: bloomery iron smelting in America and Africa. Technol. Cult. 34, 243e
270.
Gordon, R.B., van der Merwe, N.J., 1984. Metallographic study of iron artefacts from
the eastern Transvaal Lowveld, South Africa. Archaeometry 26, 108e127.
Haggerty, S., 1991. Oxide textures: a mini-atlas. In: Lindsley, D.H. (Ed.), Oxide
Minerals: Petrologic and Magnetic Significance, Reviews in Mineralogy, vol. 25,
pp. 129e219.
Hall, A.L., 1912. Geology of the Murchison Range and District. In: Union of South
Africa Geological Survey, Memoir, vol. 6. Pretoria.
Hall, S., Miller, D., Anderson, M., Boeyens, J., 2006. An exploratory study of copper
and iron production at Marothodi, an early 19th century Tswana town, Rus-
tenburg District, South Africa. J. Afr. Archaeol. 4, 3e35.
Hanekom, H.J., van Staden, C.M., Smit, P.J., Pike, D.R., 1965. The Geology of the
Phalaborwa Igneous Complex. In: Geological Survey of South Africa Memoir,
vol. 54. Pretoria.
Ige, A., Rehren, T., 2002. Black sand and iron stone: iron smelting in Modakeke, Ife,
south western Nigeria. IAMS 22, 19e21.
Iles, L., Martinón-Torres, M., 2009. Pastoralist iron production on the Laikipia
Plateau, Kenya: wider implications for archaeometallurgical studies. J. Archaeol.
Sci. 36, 2314e2326.
Jaguin, J., Gapais, D., Poujol, M., Boulvais, P., Moyen, J.-F., 2012. The Murchison
greenstone belt, South Africa e a general tectonic framework. South Afr. J. Geol.
115, 65e76.
Junod, H.A., 1927. The Life of a South African Tribe. MacMillan, London.
Killick, D.J., 1990. Technology in its Social Setting: Bloomery Iron Working at
Kasungu, Malawi, 1860e1940. Ph.D. thesis. Yale University.
Killick, D.J., Gordon, R.B., 1988. The mechanism of the bloomery process. In:
Farquhar, R.M., Hancock, R.G.V., Pavlish, L.A. (Eds.), Proceedings of the 26th
International Symposium on Archaeometry. University of Toronto Department
of Physics, Toronto, pp. 120e123.
Klapwijk, M., 1986. A late iron age furnace excavation on the farm Longridge, Agatha,
north-eastern Transvaal, South Africa. South Afr. Archaeol. Bull. 41, 22e26.
Klapwijk, M., Huffman, T.N., 1996. Excavations at Silver Leaves: a final report. South
Afr. Archaeol. Bull. 51, 84e93.
Krige, E.J., 1941. Economics of exchange in a primitive society. South Afr. J. Econ. 9,
1e21.
Levin, E.M., Robbins, C.R., McMurdie, H.F., 1964. Phase Diagrams for Ceramists.
American Ceramic Society, Columbus.
Mason, R.J., 1968. Transvaal and Natal Iron Age settlement revealed by aerial
photography and excavation. Afr. Stud. 27, 1e14.
Mathoho, N.E., 2012. Indigenous Iron Production South of the Luvuvhu River,
Limpopo Province, South Africa. M.A. dissertation. University of Cape Town.
McGannon, H.E., 1971. The Making, Shaping and Treatment of Steel, ninth ed. United
States Steel Corporation, Pittsburgh.
Mellor, E.T., 1906. The Geology of the District about Haenertsburg, Leydsdorp and
the Murchison Range. In: Geological Survey of the Transvaal, pp. 21e52.
Pretoria.
McCourt, S., van Reenen, D.D., 1992. Structural geology and tectonic setting of the
Sutherland greenstone Belt, Kaapvaal Craton, South Africa. Precambrian Res. 55,
93e110.
Meyer, A., 1986. ’n Kultuurhistoriese Interpretasie van die Ystertydperk in die
Nasionale Krugerwildtuin. Ph.D. thesis. University of Pretoria.
Miller, D.E., 2002. Smelter and smith: metal fabrication technology in the southern
African Early and Late Iron Age. J. Archaeol. Sci. 29, 1083e1131.
Miller, D.E., Killick, D.J., van der Merwe, N.J., 2001. Metal working in the northern
Lowveld, South Africa, AC 1000-1890. J. Field Archaeol. 28, 401e417.
255
Miller, D.E., Malaudzi, M., Killick, D.J., 2002. An historical account of bloomery iron
working in the Lowveld, South Africa. Hist. Metall. 36, 112e121.
Norrish, K., Hutton, J.T., 1969. An accurate X-ray spectrographic method for the
analysis of a wide range of geological samples. Geochim. Cosmochim. Acta 33,
431e453.
Palabora Mining Company Geological Staff, 1976. The geology and the economic
deposits of copper, iron and vermiculite in the Palabora Igneous Complex. Econ.
Geol. 71, 177e192.
Park, J.-S., Rehren, T., 2011. Large-scale 2nd to 3rd century AD bloomery iron
smelting in Korea. J. Archaeol. Sci. 38, 1180e1190.
Photos, E., Koukouli-Chrysanthaki, H., Gialoglou, G., 1984. Iron metallurgy in Eastern
Macedonia: a preliminary report. In: Scott, B.G., Cleere, H. (Eds.), The Crafts of
the Blacksmith. Ulster Museum, Belfast, pp. 113e120.
Pistorius, J., 1989. Die Metaalbewerkers Van Phalaborwa. Ph.D. thesis. University of
Pretoria.
Plug, I., Pistorius, J., 1999. Animal remains from industrial iron age communities in
Phalaborwa, South Africa. Afr. Archaeol. Rev. 16, 155e184.
Reynolds, I.M., 1986. Vanadium-bearing titaniferous iron ores of the Rooiwater
Complex, north-eastern Transvaal. In: Anhaeusser, C.R., Maske, S. (Eds.), Mineral
Deposits of South Africa. Geological Society of South Africa, Johannesburg,
pp. 451e460.
Rostoker, W., Bronson, B., 1990. Pre-industrial Iron: its Technology and Ethnology.
Archeomaterials Monograph no. 1. Archaeomaterials Publishers, Philadelphia.
Rostoker, W., Bronson, B., Dvorak, J.R., 1989. Smelting to steel by the Japanese tatara
process. Archeomaterials 3, 11e25.
Schwellnus, C.M., 1937. Short notes on the Palaboroa smelting ovens. South Afr. J.
Sci. 33, 904e912.
Schwellnus, J.S.I., Englebrecht, L.N.J., Coertze, F.J., Russell, H.D., Malherbe, S.J., van
Rooyen, D.P., Cooke, R., 1962. The Geology of the Olifants River Area, Transvaal.
Government Printer, Pretoria.
Stayt, H., 1931. The Bavenda. Oxford University Press, Oxford.
Stettler, E.H., Coetzee, H., Rogers, H.J.J., Lubala, R.T., 1993. The Schiel alkaline
complex: geological setting and geophysical investigation. South Afr. J. Geol.
96, 96e107.
Stoch, H., 1978. The Preparation and Certification of a Reference Sample of
Magnetite Ore. National Institute for Metallurgy Report, Randburg, South Africa.
Stuiver, M., van der Merwe, N.J., 1968. Radiocarbon chronology of the Iron Age in
sub-Saharan Africa. Curr. Anthropol. 3, 178e196.
Thorne, R.M., 1974. Archaeological Survey in South Africa: Conceptual, Methodo-
logical and Practical Problems: The Phalaborwa Complex, a Case Study. Ph.D.
thesis. University of Missouri, Columbia, MO.
Trevor, T.G., 1912. Some observations on ancient mine workings in the Transvaal.
Journal of the Chemical. Metallurgical Min. Soc. S. Afr. 12, 267e275.
van der Merwe, D.S., 1936. A Preliminary Survey of Places of Archaeological Interest
in the Northern Transvaal. Unpublished typescript, File 9/3. University of the
Witwatersrand Archaeological Research Unit, South Africa.
van der Merwe, N.J., Killick, D.J., 1979. Square: an iron smelting site near Phala-
borwa. South Afr. Archaeol. Soc. Goodwin Ser. 3, 86e93.
van der Merwe, N.J., Scully, R.T.K., 1971. The Phalaborwa story: archaeological and
ethnographic investigation of a South African Iron Age group. World Archaeol.
3, 78e196.
van Eeden, O.R., Kent, L.E., Brandt, J.W., 1939. The Mineral Deposits of the Murchison
Range East of Leydsdorp. In: Union of South Africa Department of Mines,
Memoir, vol. 36. Pretoria.
Verein Deutscher Eisenhüttenleute, 1995. Schlackenatlas/Slag Atlas, second ed., 2
vols. Verlag StahlEisen, Düsseldorf.
Verwoerd, W.J., 1956. Sekere produkte van primitiewe koper-, yster-, en bronss-
meltery in Oos Transvaal met besonder verwysing na Phalaborwa. Tegnikon 9,
91e104.
Verwoerd, W.J., 1986. Mineral deposits associated with carbonatites and alkaline
rocks. In: Anhaeusser, C.R., Maske, S. (Eds.), Mineral Deposits of South Africa.
Geological Soc. S. Afr., 2173e2191. Johannesburg.
Verwoerd, W.J., du Toit, M.C., 2006. The Phalaborwa and Schiel complexes. In:
Johnson, M.R., Anhaeusser, C.R., Thomas, R.J. (Eds.), The Geology of South Africa.
Council for Geoscience, Pretoria, pp. 291e299.
Wessmann, R., 1908 (1969). The Bawenda of the Spelonken (Transvaal): a Contri-
bution towards the Psychology and Folklore of African Peoples (L. Weinthal,
Trans.). Negro Universities Press, New York.