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Econ. Environ. Geol. 2024; 57(3): 343-352
Published online June 30, 2024
https://doi.org/10.9719/EEG.2024.57.3.343
© THE KOREAN SOCIETY OF ECONOMIC AND ENVIRONMENTAL GEOLOGY
Study on the Chemical Composition and Lead Isotope Ratios of Lead Glaze Used on Blue Tiles from Gyeoungbokgung Palace
Correspondence to : *ydkim1@hanyang.ac.kr
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided original work is properly cited.
Abstract
Composition analysis and lead isotope ratio analysis were conducted to determine the coloring machanism on lead glaze used in Gyeongbokgung Palace and the provenance of the lead used as a flux. 31 blue tiles were classified into green, blue, and yellow. The chemical analysis of lead glazes on the blue tiles revealed that Pb, Si, and Cu were the main components, and trace amounts of Fe, Ca, Mg, and Al were detected. The Cu content was high in blue lead glaze, while Cu was not detected in yellow or brown lead glaze which instead had high Fe content. Therefore, it was found that lead was used as a flux and copper oxide as a coloring agent in the production of lead glaze. In addition, the lead isotope ratios of the lead glaze used in the blue tiles of Gyeongbokgung palace were plotted in zone 3 on the distribution map of lead isotope ratios on the Korean Peninsula, which includes Chungcheong-do and Jeolla-do. It is presumed that the flux for the lead glaze was sourced from galena found in these regions.
The lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period were mostly located outside the Korean Peninsula, showing that the provenance of lead had changed. In particular, the lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period suggest exchange with neighboring countries. Also the lead isotope ratios of the green glazes from the same temple are different, so it is believed that they were made at different times or in different workshops.
Keywords Gyeongbokgung Palace, Blue Tile, lead glaze, chemical composition, lead isotopes ratios
경복궁 청기와에 사용된 납유의 화학조성과 납동위원소 특성연구
김소진1,2 · 김영도2,*
1국립문화유산연구원 보존과학연구실
2한양대학교 신소재공학과
요 약
경복궁 전각 청기와에 사용된 납유의 발색 원리와 용융제로 사용된 납의 산지를 확인하기 위해 성분 분석과 납동위원소비 분석을 실시했다. 청기와 31점을 녹색, 청색, 황색으로 구분하여 표면에 시유된 납유의 성분을 분석한 결과 Pb, Si, Cu가 주성분으로, Fe, Ca, Mg, Al 등이 미량으로 검출되었다. 청색 납유에서는 Cu의 함량이 높았으며 황색 또는 갈색의 납유에서는 Cu는 검출되지 않았고 Fe의 함량이 높게 나타났다. 따라서 납유의 제작에 용융제로 납을, 발색제로 산화동을 사용했음을 알 수 있었다. 또한 경복궁 청기와에 사용된 납유의 납동위원소비는 한반도 납동위원소비 분포도에서 충청도와 전라도를 포함하는 zone 3 영역에 도시되었으며, 납유의 용융제는 이들 지역에서 산출되는 방연석 등을 사용했을 것으로 추정된다. 삼국과 통일신라시대 녹유의 납동위원소비는 대부분 한반도를 벗어나 위치하여 납의 산지가 변화되었음을 알 수 있었다. 특히 녹유 전돌의 납동위원소비를 통해 주변국과의 교류를 추정할 수 있었으며 동일 사찰에서 출토된 녹유 전돌의 납동위원소비가 서로 달라 다른 시기 또는 다른 공방에서 제작된 것으로 판단할 수 있었다.
주요어 경복궁, 청기와, 납유, 화학성분, 납동위원소비
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Research Paper
Econ. Environ. Geol. 2024; 57(3): 343-352
Published online June 30, 2024 https://doi.org/10.9719/EEG.2024.57.3.343
Copyright © THE KOREAN SOCIETY OF ECONOMIC AND ENVIRONMENTAL GEOLOGY.
Study on the Chemical Composition and Lead Isotope Ratios of Lead Glaze Used on Blue Tiles from Gyeoungbokgung Palace
So Jin Kim1,2, Young Do Kim2,*
1Conservation Science Division, National Research Institute of Cultural Heritage, Daejeon, 34122, Korea
2Department of Materials Science and Engineering, Hanyang University, Seoul, 04763, Korea
Correspondence to:*ydkim1@hanyang.ac.kr
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided original work is properly cited.
Abstract
Composition analysis and lead isotope ratio analysis were conducted to determine the coloring machanism on lead glaze used in Gyeongbokgung Palace and the provenance of the lead used as a flux. 31 blue tiles were classified into green, blue, and yellow. The chemical analysis of lead glazes on the blue tiles revealed that Pb, Si, and Cu were the main components, and trace amounts of Fe, Ca, Mg, and Al were detected. The Cu content was high in blue lead glaze, while Cu was not detected in yellow or brown lead glaze which instead had high Fe content. Therefore, it was found that lead was used as a flux and copper oxide as a coloring agent in the production of lead glaze. In addition, the lead isotope ratios of the lead glaze used in the blue tiles of Gyeongbokgung palace were plotted in zone 3 on the distribution map of lead isotope ratios on the Korean Peninsula, which includes Chungcheong-do and Jeolla-do. It is presumed that the flux for the lead glaze was sourced from galena found in these regions.
The lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period were mostly located outside the Korean Peninsula, showing that the provenance of lead had changed. In particular, the lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period suggest exchange with neighboring countries. Also the lead isotope ratios of the green glazes from the same temple are different, so it is believed that they were made at different times or in different workshops.
Keywords Gyeongbokgung Palace, Blue Tile, lead glaze, chemical composition, lead isotopes ratios
경복궁 청기와에 사용된 납유의 화학조성과 납동위원소 특성연구
김소진1,2 · 김영도2,*
1국립문화유산연구원 보존과학연구실
2한양대학교 신소재공학과
요 약
경복궁 전각 청기와에 사용된 납유의 발색 원리와 용융제로 사용된 납의 산지를 확인하기 위해 성분 분석과 납동위원소비 분석을 실시했다. 청기와 31점을 녹색, 청색, 황색으로 구분하여 표면에 시유된 납유의 성분을 분석한 결과 Pb, Si, Cu가 주성분으로, Fe, Ca, Mg, Al 등이 미량으로 검출되었다. 청색 납유에서는 Cu의 함량이 높았으며 황색 또는 갈색의 납유에서는 Cu는 검출되지 않았고 Fe의 함량이 높게 나타났다. 따라서 납유의 제작에 용융제로 납을, 발색제로 산화동을 사용했음을 알 수 있었다. 또한 경복궁 청기와에 사용된 납유의 납동위원소비는 한반도 납동위원소비 분포도에서 충청도와 전라도를 포함하는 zone 3 영역에 도시되었으며, 납유의 용융제는 이들 지역에서 산출되는 방연석 등을 사용했을 것으로 추정된다. 삼국과 통일신라시대 녹유의 납동위원소비는 대부분 한반도를 벗어나 위치하여 납의 산지가 변화되었음을 알 수 있었다. 특히 녹유 전돌의 납동위원소비를 통해 주변국과의 교류를 추정할 수 있었으며 동일 사찰에서 출토된 녹유 전돌의 납동위원소비가 서로 달라 다른 시기 또는 다른 공방에서 제작된 것으로 판단할 수 있었다.
주요어 경복궁, 청기와, 납유, 화학성분, 납동위원소비
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Table 1 . List of the analysed blue tile samples from Gyeongbokgung Palace.
No. Sample Site Color No. Sample Site Color 1 GB1 Jamidang Blue 17 S1 Sojubangji Green 2 GB2 Jamidang Blue 18 S9 Sojubangji Green 3 GB3 Jamidang Blue 19 S10 Sojubangji Blue 4 GB4 Jamidang Blue 20 S13 Sojubangji Blue 5 GB5 Jamidang Blue 21 S16 Sojubangji Green 6 GB6 Jamidang Blue 22 S17 Sojubangji Green 7 GG1 Jamidang Green 23 S21 Sojubangji Green 8 GG2 Jamidang Green 24 H3 Heungbokjeonji Yellow 9 GG3 Jamidang Green 25 H6 Heungbokjeonji Blue 10 GG4 Jamidang Green 26 H8 Heungbokjeonji Blue 11 GG5 Jamidang Green 27 H9 Heungbokjeonji Green 12 GG6 Jamidang Green 28 H10 Heungbokjeonji Green 13 GY1 Jamidang Yellow 29 H12 Heungbokjeonji Yellow 14 GY2 Jamidang Yellow 30 J2 Jipgueongdangi Green 15 GY3 Jamidang Yellow 31 J3 Jipgueongdangi Green 16 GY4 Jamidang Yellow
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Table 2 . Handheld XRF analysis of Standard Reference Materials of glass.
Sample SiO2 Na2O CaO MgO Al2O3 K2O SO3 As2O3 Fe2O3 TiO2 NIST 620 72.08 14.39 7.11 3.69 1.80 0.41 0.28 0.056 0.043 0.018 Mean 73.15 - 6.30 3.40 0.76 0.29 0.15 0.054 0.040 LOD LOD : Limit of Detection, unit: wt.%.
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Table 3 . Relation of colors and elements of Blue tiles from Gyeonbokgung Palace.
No. Sample Color Pb Cu Fe Ca Mg Si Al K 1 GB1 Blue 34.56 8.42 0.24 1.68 0.30 35.91 2.27 3.10 2 GB2 Blue 29.81 8.65 0.24 2.19 0.85 36.32 0.92 3.14 3 GB3 Blue 35.30 8.12 0.11 1.17 1.00 31.84 1.50 1.55 4 GB4 Blue 16.48 7.40 0.40 1.68 0.92 53.15 2.10 6.73 5 GB5 Blue 32.48 7.40 0.22 1.43 0.79 37.71 2.08 2.35 6 GB6 Blue 34.47 9.08 0.19 1.11 0.64 35.14 0.20 3.31 7 S10 Blue 36.66 7.27 0.20 0.83 0.55 32.84 0.50 1.71 8 S13 Blue 28.74 5.82 0.14 0.95 0.30 29.95 0.94 1.51 9 H6 Blue 33.70 8.26 0.21 0.74 0.58 39.11 0.83 1.64 10 H8 Blue 32.22 8.19 0.18 0.52 0.30 40.79 0.10 2.27 11 GG1 Green 33.81 2.43 0.13 0.76 ND 22.19 1.25 0.06 12 GG2 Green 31.57 2.79 0.07 0.82 ND 20.57 0.97 0.01 13 GG3 Green 28.85 3.38 0.09 1.40 ND 27.55 2.58 0.03 14 GG4 Green 26.13 2.23 0.10 0.50 ND 20.78 0.77 0.05 15 GG5 Green 31.11 3.60 0.08 0.68 0.26 24.66 1.73 0.06 16 GG6 Green 29.87 3.60 0.06 0.27 ND 19.46 0.78 0.04 17 S1 Green 27.59 2.53 0.05 0.43 ND 19.35 1.28 0.06 18 S9 Green 32.49 9.20 0.24 0.84 0.73 36.03 0.31 3.44 19 S16 Green 33.30 2.20 0.08 0.64 ND 19.06 1.61 0.07 20 S17 Green 30.56 2.62 0.14 0.94 ND 20.44 0.72 0.12 21 S21 Green 19.67 1.25 0.21 0.31 0.40 29.79 3.56 0.13 22 H9 Green 34.92 2.52 0.25 0.60 0.27 39.18 2.37 0.45 23 H10 Green 23.62 2.28 1.85 0.56 1.74 44.97 9.08 2.95 24 J2 Green 34.22 4.32 0.09 0.12 0.28 19.89 0.55 0.07 25 J3 Green 38.76 5.35 0.10 0.37 0.30 30.02 1.26 1.28 26 GY1 Yellow 45.09 ND 1.32 3.52 0.76 18.23 0.77 0.04 27 GY2 Yellow 43.54 ND 1.26 0.25 0.34 23.41 0.34 0.10 28 GY3 Yellow 44.93 ND 1.24 5.40 ND 18.74 0.22 0.05 29 GY4 Yellow 45.62 ND 1.24 5.44 0.75 12.72 0.42 0.05 30 H3 Yellow 43.22 ND 2.86 0.52 0.61 28.19 0.36 1.65 31 H12 Yellow 43.40 ND 1.39 0.25 ND 22.62 0.32 0.10 ND : Not Detected, unit: wt.%.
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Table 4 . Lead isotopes of glazes from Gyeonbokgung Palace in Joseon Dynasty.
No. Sample Color 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 207Pb/206Pb 208Pb/206Pb 1 GB1 Blue 18.439 15.719 38.865 0.8525 2.1078 2 GB2 Blue 18.385 15.727 38.824 0.8554 2.1118 3 GB3 Blue 18.167 15.668 38.451 0.8625 2.1165 4 GB4 Blue 18.514 15.775 39.077 0.8520 2.1106 5 GB5 Blue 18.224 15.712 38.629 0.8622 2.1195 6 GB6 Blue 18.458 15.766 39.038 0.8541 2.1148 7 GG1 Green 18.259 15.668 38.552 0.8581 2.1114 8 GG2 Green 18.518 15.760 39.047 0.8510 2.1085 9 GG3 Green 18.524 15.763 39.069 0.8510 2.1091 10 GG4 Green 18.251 15.715 38.665 0.8610 2.1184 11 GG5 Green 18.590 15.856 39.354 0.8529 2.1174 12 GG6 Green 18.504 15.750 39.010 0.8512 2.1082 13 GY1 Yellow 18.525 15.860 39.300 0.8561 2.1213 14 GY2 Yellow 18.390 15.711 38.817 0.8543 2.1107 15 GY3 Yellow 18.429 15.767 39.005 0.8555 2.1163 16 GY4 Yellow 18.414 15.729 38.865 0.8542 2.1106 17 S1 Green 18.566 15.826 39.261 0.8524 2.1146 18 S9 Green 18.545 15.919 39.425 0.8584 2.1258 19 S10 Blue 18.289 15.680 38.611 0.8573 2.1111 20 S13 Blue 18.479 15.848 39.216 0.8575 2.1224 21 S16 Green 18.526 15.773 39.086 0.8514 2.1097 22 S17 Green 18.289 15.741 38.760 0.8607 2.1194 23 S21 Green 18.533 15.783 39.112 0.8516 2.1105 24 H3 Yellow 17.829 15.643 37.913 0.8775 2.1261 25 H6 Blue 18.126 15.683 38.442 0.8652 2.1207 26 H8 Blue 18.372 15.721 38.796 0.8557 2.1116 27 H9 Green 18.230 15.706 38.623 0.8616 2.1187 28 H10 Green 18.071 15.704 38.263 0.8691 2.1173 29 H12 Yellow 18.427 15.742 38.903 0.8543 2.1111 30 J2 Green 18.551 15.813 39.241 0.8524 2.1152 31 J3 Green 17.940 15.659 38.047 0.8729 2.1204
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Table 5 . Lead isotopes of lead glazes in the three kingdoms and unified silla period.
No. Site 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb Ref. 1 Wanggung-ri, Iksan 17.890 15.651 38.954 BNRICH, 2007 2 Wanggung-ri, Iksan 17.234 15.513 37.935 BNRICH, 2007 3 Wanggung-ri, Iksan 17.251 15.538 38.014 BNRICH, 2007 4 Mireuksa Temple Site, Iksan 17.415 15.622 37.889 BNRICH, 2007 5 Mireuksa Temple Site, Iksan 17.522 15.622 34.681 BNRICH, 2007 6 Mireuksa Temple Site, Iksan 17.532 15.629 34.698 BNRICH, 2007 7 Mireuksa Temple Site, Iksan 17.371 15.612 34.933 BNRICH, 2007 8 Mireuksa Temple Site, Iksan 17.365 15.604 34.901 BNRICH, 2007 9 Mireuksa Temple Site, Iksan 17.409 15.620 34.893 BNRICH, 2007 10 Mireuksa Temple Site, Iksan 17.377 15.605 34.879 BNRICH, 2007 11 Mireuksa Temple Site, Iksan 17.400 15.621 34.921 BNRICH, 2007 12 Mireuksa Temple Site, Iksan 17.408 15.614 34.867 BNRICH, 2007 13 Mireuksa Temple Site, Iksan 14.335 12.816 31.797 INM, 2020 14 Mireuksa Temple Site, Iksan 16.494 14.712 36.482 INM, 2020 15 Mireuksa Temple Site, Iksan 16.725 15.131 37.293 INM, 2020 16 Mireuksa Temple Site, Iksan 16.98/0 15.189 37.482 INM, 2020 17 Mireuksa Temple Site, Iksan 14.583 13.365 32.877 INM, 2020 18 Mireuksa Temple Site, Iksan 14.044 12.626 31.563 INM, 2020 19 Mireuksa Temple Site, Iksan 15.117 13.561 33.726 INM, 2020 20 Mireuksa Temple Site, Iksan 17.030 15.061 37.559 INM, 2020 21 Buseoksa Temple, Yeongju 19.738 16.157 40.258 Kang et al., 2005 22 Buseoksa Temple, Yeongju 19.667 16.102 40.082 Kang et al., 2005 23 Buseoksa Temple, Yeongju 26.625 16.900 41.601 Kang et al., 2005 24 Cheonryongsa temple site, Gyeongju 26.021 16.760 41.318 Kang et al., 2005 25 Beopqwangsa temple site, Pohang 26.548 16.811 41.311 Kang et al., 2005 26 Beopqwangsa temple site, Pohang 25.980 16.722 41.199 Kang et al., 2005 27 Yeongmyosa temple site, Gyeongju 25.985 16.738 41.251 Jo et al., 2007 28 Yeongmyosa temple site, Gyeongju 26.677 16.847 41.519 Jo et al., 2007 29 Sacheonwangsa temple site, Gyeongju 20.146 15.976 39.156 GNRICH, 2018 30 Sacheonwangsa temple site, Gyeongju 18.225 15.749 39.290 GNRICH, 2018
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