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The production technology of mineral soda alumina glass: A perspective from microstructural analysis of glass beads in Iron Age Taiwan

Wang, Kuan-Wen, Iizuka, Yoshiyuki, Jackson, Caroline·2022·PLOS ONE
DOI 10.1371/journal.pone.0263986PMC PMC8846499
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Abstract

Mineral soda alumina (m-Na-Al) glass is a common glass production group found around the Indo-Pacific region. In Iron Age Taiwan, its presence dates back to the early 1 st millennium AD. This research discusses m-Na-Al glass beads excavated from Iron Age sites in Taiwan. No production sites for m-Na-Al have been found, but microstructural analysis suggests m-Na-Al glass appears to originate around South Asia and is exchanged widely. SEM-EDS and EPMA were used to analyse red, orange, yellow, green and blue m-Na-Al glass. The microstructure of the glass shows the presence of plagioclase and alkali feldspar relics in the glass, suggesting a low manufacturing temperature. Copper-based colourants are identified in red, orange, blue and green glass, while lead tin oxide is used in yellow and green glass. It appears that various types of copper-containing raw materials were procured by craftspeople, and a self-reduction process for producing red and orange glass is tentatively proposed. Additionally, the microstructure of yellow glass reveals different colouring paths were used. These results increase our understanding of the selection of raw materials, and provide an impetus for further research on the cross craft interaction between glass and copper production.

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Fig 1 Map showing the location of study sites (above), and bead samples from each site (below). (Map made with Natural Earth. Free vector and raster map data @ naturalearthdata.com.).
Fig 1 Map showing the location of study sites (above), and bead samples from each site (below). (Map made with Natural Earth. Free vector and raster map data @ naturalearthdata.com.).CC BY · PubMed Central
Fig 2 BSE image showing the heterogeneous microstructure of the glass matrix.
Fig 2 BSE image showing the heterogeneous microstructure of the glass matrix.CC BY · PubMed Central
Fig 3 A plot of m-Na-Al glasses in the Na2O-Al2O3-SiO2 phase diagram. The oxides from the base composition are further reduced into three components (SiO2, Al2O3* and Na2O*)–the FeO, MgO and CaO are transmuted to Al2O3 (labelled Al2O3*), using a transmuting factor of 0.71, 1.26 and 0.91, respectively (Rehren 2016, pers. comm.). The K2O is incorporated into Na2O (labelled Na2O*) transmuted by the factor of 0.66. The base phase diagram is from Levin and McMurdie [23].
Fig 3 A plot of m-Na-Al glasses in the Na2O-Al2O3-SiO2 phase diagram. The oxides from the base composition are further reduced into three components (SiO2, Al2O3* and Na2O*)–the FeO, MgO and CaO are transmuted to Al2O3 (labelled Al2O3*), using a transmuting factor of 0.71, 1.26 and 0.91, respectively (Rehren 2016, pers. comm.). The K2O is incorporated into Na2O (labelled Na2O*) transmuted by the factor of 0.66. The base phase diagram is from Levin and McMurdie [23].CC BY · PubMed Central
Fig 4 BSE image showing the relics in red glass, in which (a) silver particles are observed in copper sulphide inclusion (JXL02), (b) a copper oxide inclusion showing partial reduction process (JXL10), (c) a metallic copper inclusion showing partial oxidation (GS004), and (d) a cluster of needle-like tin oxide remain the crude cassiterite shape (JXL22).
Fig 4 BSE image showing the relics in red glass, in which (a) silver particles are observed in copper sulphide inclusion (JXL02), (b) a copper oxide inclusion showing partial reduction process (JXL10), (c) a metallic copper inclusion showing partial oxidation (GS004), and (d) a cluster of needle-like tin oxide remain the crude cassiterite shape (JXL22).CC BY · PubMed Central
Fig 5 BSE image showing the microstructure of orange glass, in which (a) copper-bearing crystals of micro size distribute linearly over the glass matrix or fill within round voids (JXL27), (b) large copper oxide crystals are found in the red striae, while the particles of sub-micron size spread over the orange matrix (JXL24), (c)-(e) oxidised bronze prill was observed (JXL25, wt%), (f) a cluster of copper oxide and tin oxide suggesting decomposition from bronze (KWL005), and (g) large metallic copper crystals are confirmed by EDS (KWL003).
Fig 5 BSE image showing the microstructure of orange glass, in which (a) copper-bearing crystals of micro size distribute linearly over the glass matrix or fill within round voids (JXL27), (b) large copper oxide crystals are found in the red striae, while the particles of sub-micron size spread over the orange matrix (JXL24), (c)-(e) oxidised bronze prill was observed (JXL25, wt%), (f) a cluster of copper oxide and tin oxide suggesting decomposition from bronze (KWL005), and (g) large metallic copper crystals are confirmed by EDS (KWL003).CC BY · PubMed Central
Fig 6 BSE image the microstructure of blue glass, in which (a) clusters of copper oxide (grey) and tin oxide (bright) (JXL28) and (b) the prismatic barite inclusions (JXL17) are observed.
Fig 6 BSE image the microstructure of blue glass, in which (a) clusters of copper oxide (grey) and tin oxide (bright) (JXL28) and (b) the prismatic barite inclusions (JXL17) are observed.CC BY · PubMed Central
Fig 7 BSE image showing microstructure of yellow glass, in which (a) clusters of tiny lead tin oxide crystals are frequently found with large and newly formed nephelines in Case 1 (JXL15), (b) the cores of Pb(Sn,Si)O3 exhibits possible Pb2SnO4 remnants (JXL05), (c) lead tin oxide clusters solely, without any nepheline, in Case 2 (DY14), (d) porous bone ash is observed (GS028), and (e)-(f) Ba-bearing K-feldspar and lead tin oxide is found in the bone ash-containing samples, and the bone ash is particularly high in PbO (>60wt%) (JXL48).
Fig 7 BSE image showing microstructure of yellow glass, in which (a) clusters of tiny lead tin oxide crystals are frequently found with large and newly formed nephelines in Case 1 (JXL15), (b) the cores of Pb(Sn,Si)O3 exhibits possible Pb2SnO4 remnants (JXL05), (c) lead tin oxide clusters solely, without any nepheline, in Case 2 (DY14), (d) porous bone ash is observed (GS028), and (e)-(f) Ba-bearing K-feldspar and lead tin oxide is found in the bone ash-containing samples, and the bone ash is particularly high in PbO (>60wt%) (JXL48).CC BY · PubMed Central
Fig 8 BSE image showing microstructure of green glass, in which (a) a tin oxide rich in Fe, Zn and Ni is found (DY42-1), (b) a tin-rich inclusion containing Ca, Al and Si is observed (GS103), and (c) a visible red inclusion showing inhomogeneous distribution of CuO, TiO2, FeO and SO3, as well as prismatic barite crystals and partially melted sodium aluminosilicate (JXL09).
Fig 8 BSE image showing microstructure of green glass, in which (a) a tin oxide rich in Fe, Zn and Ni is found (DY42-1), (b) a tin-rich inclusion containing Ca, Al and Si is observed (GS103), and (c) a visible red inclusion showing inhomogeneous distribution of CuO, TiO2, FeO and SO3, as well as prismatic barite crystals and partially melted sodium aluminosilicate (JXL09).CC BY · PubMed Central

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Metadata

Authors
Wang, K.-W., Iizuka, Y., & Jackson, C.
ORCID
Wang, Kuan-Wen
Venue
PLOS ONE
Publisher
Public Library of Science (PLoS)
Published
2022-02-15
Volume
17
Issue
2
Pages
e0263986
ISSN
1932-6203
DOI
10.1371/journal.pone.0263986
PMC
PMC8846499
Cited by
6
References
0
Language
en
Licence
creativecommons.org/licenses/by/4.0/ (vor)

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