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Insight Into the Crystallinity of Chinese Ancient Silk by Synchrotron Radiation-Based and Conventional X-ray Diffraction Methods

  • Gong, Decai (Basic Research Center of Conservation Science, Department of the History of Science and Scientific Archaeology, University of Science and Technology of China) ;
  • Zhang, Xiaoning (Basic Research Center of Conservation Science, Department of the History of Science and Scientific Archaeology, University of Science and Technology of China) ;
  • Gong, Yuxuan (Basic Research Center of Conservation Science, Department of the History of Science and Scientific Archaeology, University of Science and Technology of China)
  • Received : 2019.09.25
  • Accepted : 2019.11.24
  • Published : 2020.02.20

Abstract

This study investigates the crystallinity distribution of ancient silk. Owing to the inherent multi-hierarchical structure of silk protein and the complicated structural changes that occur due to various burial environments, it is challenging but worthwhile to study ancient silk ageing behavior, which is based on the fact that ageing begins with a single fiber and then spreads to a whole fabric. Crystallinity was one of the most effective indicators found to reveal the ageing status of silk. Therefore, a synchrotron radiation-based X-ray diffraction(SR-XRD) method was employed to study the crystallinity distribution of single fibers of ancient silk unearthed from seven archaeological sites in China from historical periods including the warring states, Han dynasty, Song dynasty, and Ming dynasty. In comparison, the conventional X-ray diffraction method, which uses large amounts of samples, was also performed to determine the integral crystallinity of ancient silk. Thermal stability experiments by thermogravimetry(TG) as well as morphology observations by scanning electron microscopy(SEM) and optical microscopy(OM) all confirmed the deterioration of ancient silk. Moreover, the ageing mechanism of ancient silk was proposed with the assistance of an artificial ageing study. The results confirmed the effectiveness of SR-XRD as an ageing indicator, revealing the crystallinity distribution. This research could provide motivation to determine the deterioration status of ancient silk, and would also aid in explaining the fragility of ancient silk due to ageing.

Keywords

References

  1. Badillo-Sanchez, D., Chelazzi, D., Giorgi, R., Cincinelli, A. and Baglioni, P., 2018, Characterization of the secondary structure of degummed Bombyx mori silk in modern and historical samples. Polymer Degradation and Stability, 157, 53-62. https://doi.org/10.1016/j.polymdegradstab.2018.09.022
  2. Baek, Y.M., Goto-Doshida, S. and Saito, M., 2012, Effects of the wet cleaning to the color change of the dyed fabrics with natural dyes. Journal of Conservation Science, 28(1), 21-27. (in Korean with English abstract) https://doi.org/10.12654/JCS.2012.28.1.021
  3. Bertrand, L., Cotte, M., Stampanoni, M., Thoury, M., Marone, F. and Schoder, S., 2012a, Development and trends in synchrotron studies of ancient and historical materials. Physics Reports, 519(2), 51-96. https://doi.org/10.1016/j.physrep.2012.03.003
  4. Bertrand, L., Robinet, L., Thoury, M., Janssens, K., Cohen, S.X. and Schöder, S., 2012b, Cultural heritage and archaeology materials studied by synchrotron spectroscopy and imaging. Applied Physics A, 106(2), 377-396. https://doi.org/10.1007/s00339-011-6686-4
  5. Drummy, L.F., Farmer, B.L. and Naik, R.R., 2007, Correlation of the $\beta$-sheet crystal size in silk fibers with the protein amino acid sequence. Soft Matter, 3(7), 877-882. https://doi.org/10.1039/B701220A
  6. Fang, G.Q., Huang, Y.F., Tang, Y.Z., Qi, Z.M., Yao, J.R., Shao, Z.Z., and Chen, X., 2016, Insights into silk formation process: Correlation of mechanical properties and structural evolution during artificial spinning of silk fibers. Acs Biomaterials Science & Engineering, 2(11), 1992-2000. https://doi.org/10.1021/acsbiomaterials.6b00392
  7. Greiff, S., Kutzke, H., Riekel, C. and Wyeth, P., 2005, Surveying silk fibre degradation by crystallinity determination: A study on the Tang-Dynasty silk treasure from Famen Temple, China. Scientific Analysis of Ancient and Historic Textiles: Informing Preservation, Display and Interpretation. AHRB Research Centre for Textile Conservation and Textile Studies, First Annual Conference 2004.
  8. Guo, C.C., Zhang, J., Jordan, J.S., Wang, X.G., Henning, R.W. and Yarger, J.L., 2018, Structural comparison of various silkworm silks: An insight into the structure-property relationship. Biomacromolecules, 19(3), 906-917. https://doi.org/10.1021/acs.biomac.7b01687
  9. Ha S.W., Gracz, H.S., Tonelli, A.E. and Hudson, S.M., 2005, Structural study of irregular amino acid sequences in the heavy chain of bombyx mori silk fibroin. Biomacromolecules, 6(5), 2563-2569. https://doi.org/10.1021/bm050294m
  10. Hao, X.Y., Wang, X., Yang, W.M., Ran, J.B., Ni, F.F., Tong, T., Dai, W., Zheng, L.Y., Shen, X.Y., and Tong, H., 2019, Comparisons of the restoring and reinforcement effects of carboxymethyl chitosan-silk fibroin (Bombyx Mori/Antheraea Yamamai/Tussah) on aged historic silk. International Journal of Biological Macromolecules, 124, 71-79. https://doi.org/10.1016/j.ijbiomac.2018.11.203
  11. Hermes, A.C., Davies, R. J., Greiff, S., Kutzke, H., Lahlil, S., Wyeth, P. and Riekel, C., 2006, Characterizing the decay of ancient Chinese silk fabrics by microbeam synchrotron radiation diffraction. Biomacromolecules, 7(3), 777-783. https://doi.org/10.1021/bm0508313
  12. Janssens, K., Alfeld, M., Van, d. S.G., De, N.W., Vanmeert, F., Radepont, M., Monico, L., Dik, J., Cotte, M. and Falkenberg, G., 2013, The use of synchrotron radiation for the characterization of artists' pigments and paintings. Annual Review of Analytical Chemistry, 6(1), 399-425. https://doi.org/10.1146/annurev-anchem-062012-092702
  13. Kang, D.I., 2009, The stability appraisement on cultural property material with the replacing fumigation gas of methyl bromide. Journal of Conservation Science, 25(3), 283-291. (in Korean with English abstract)
  14. Kim, M.N., Lim, B.A. and Lee, S.M., 2014, Damage characteristics of korean traditional textiles by formaldehyde. Journal of Conservation Science, 30(4), 353-364. (in Korean with English abstract) https://doi.org/10.12654/JCS.2014.30.4.04
  15. Kim, M.N., Lim, B.A. and Lee, S.M., 2016, Damage characteristics of korean traditional textiles by acetaldehyde. Journal of Conservation Science, 32(3), 321-331. (in Korean with English abstract) https://doi.org/10.12654/JCS.2016.32.3.03
  16. Kim, M.N., Lim, B.A., Kim, S. and Lee, S.M., 2013, Damage characteristics of Korean traditional textiles by nitrogen dioxide (NO2) concentrations. Journal of Conservation Science, 29(3), 197-207. (in Korean with English abstract) https://doi.org/10.12654/JCS.2013.29.3.01
  17. Kim, M.N., Lim, B.A., Shin, E.J. and Lee, S.M., 2012, Damage characteristics of korean traditional textiles by sulfur dioxide. Journal of Conservation Science, 28(4), 321-328. (in Korean with English abstract) https://doi.org/10.12654/JCS.2012.28.4.321
  18. Koperska, M.A., Lojewski, T. and Lojewska, J., 2015, Evaluating degradation of silk's fibroin by attenuated total reflectance infrared spectroscopy: Case study of ancient banners from Polish collections. Spectrochimica Acta Part A Molecular & Biomolecular Spectroscopy, 135, 576-582. https://doi.org/10.1016/j.saa.2014.05.030
  19. Koperska, M.A., Pawcenis, D, Bagniuk, J., Zaitz, M.M., Missori, M., Lojewski, T. and Lojewska, J., 2014, Degradation markers of fibroin in silk through infrared spectroscopy. Polymer Degradation and Stability, 105, 185-196. https://doi.org/10.1016/j.polymdegradstab.2014.04.008
  20. Li, M.Y., Zhao, Y., Tong, T., Hou, X.H., Fang, B.S., Wu, S.Q., Shen, X.Y. and Tong, H., 2013, Study of the degradation mechanism of Chinese historic silk (Bombyx mori) for the purpose of conservation. Polymer Degradation & Stability, 98(3), 727-735. https://doi.org/10.1016/j.polymdegradstab.2012.12.021
  21. Liu, H.L., Zhao, S.H., Zhang, Q., Yeerken, T. and Yu, W.D., 2019, Secondary structure transformation and mechanical properties of silk fibers by ultraviolet irradiation and water. Textile Research Journal, 89(14), 2802-2812. https://doi.org/10.1177/0040517518803788
  22. Lu, Y.H., Lin, H., Chen, Y.Y., Wang, C. and Hua, Y.R., 2007, Structure and performance of Bombyx mori silk modified with nano-TiO2 and chitosan. Fibers and Polymers, 8(1), 1-6. https://doi.org/10.1007/BF02908152
  23. Luo, X.Y., Wu, J.Q., Intisar, A., Geng, J.P., Wu, L.M., Zheng, K.Y. and Du, Y.P., 2012, Study on light aging of silk fabric by Fourier transform infrared spectroscopy and principal component analysis. Analytical Letters, 45(10), 1286-1296. https://doi.org/10.1080/00032719.2012.673098
  24. Martel, A., Burghammer, M., J Davies, R. and Riekel, C., 2007, Thermal behavior of Bombyx mori silk: Evolution of crystalline parameters, molecular structure, and mechanical properties. Biomacromolecules, 8(11), 3548-3556. https://doi.org/10.1021/bm700935w
  25. Martin, M.C., Schade, U., Lerch, P. and Dumas, P., 2010, Recent applications and current trends in analytical chemistry using synchrotron-based Fourier-transform infrared microspectroscopy. TrAC Trends in Analytical Chemistry, 29(6), 453-463. https://doi.org/10.1016/j.trac.2010.03.002
  26. Oh, J.S., Choi, J.E., Noh, S.J. and Eum, S.W., 2014, The effects of anoxic treatments on color and mechanical property in fabrics, natural dyed fabrics, papers, natural dyed papers and paints. Journal of Conservation Science, 30(2), 219-234. (in Korean with English abstract) https://doi.org/10.12654/JCS.2014.30.2.10
  27. Park, H.J., Hwang, M. and Chung, Y.J., 2018, An assessment of the deterioration of fabricated metal thread with light, and temperature and humidity factors: A focused study of Asian textile collections at the Metropolitan Museum of Art, New York. Journal of Conservation Science, 34(4), 245-257. https://doi.org/10.12654/JCS.2018.34.4.01
  28. Park, H.J., Hwang, M. and Chung, Y.J., 2019, Cleaning fabricated metal thread: A post‐treatment stability assessment after artificial deterioration and the application of synthetic soil. Journal of Conservation Science, 35(1), 19-31. https://doi.org/10.12654/jcs.2019.35.1.03
  29. Riekel, C. and Vollrath, F., 2001, Spider silk fibre extrusion: Combined wide- and small-angle X-ray microdiffraction experiments. International Journal of Biological Macromolecules, 29(3), 203-210. https://doi.org/10.1016/S0141-8130(01)00166-0
  30. Salvado, N., Butí, S., Cotte, M., Cinque, G. and Pradell, T., 2013, Shades of green in 15th century paintings: Combined microanalysis of the materials using synchrotron radiation XRD, FTIR and XRF. Applied Physics A: Materials Science and Processing, 111(1), 47-57. https://doi.org/10.1007/s00339-012-7483-4
  31. Sampath, S., Isdebski, T., Jenkins, J.E., Ayon, J.V., Henning, R.W., Orgel, J.P., Antipoa, O. and Yarger, J.L., 2012, X-ray diffraction study of nanocrystalline and amorphous structure within major and minor ampullate dragline spider silks. Soft Matter, 8(25), 6713-6722. https://doi.org/10.1039/c2sm25373a
  32. Tsuboi, Y., Ikejiri, T., Shiga, S., Yamada, K., and Itaya, A., 2001, Light can transform the secondary structure of silk protein. Applied Physics A, 73(5), 637-640. https://doi.org/10.1007/s003390100984
  33. Xu, D., Shi, X.Y., Thompson, F., Weber, W.S., Mou, Q.S., Yarger, J.L., 2015, Protein secondary structure of Green Lynx spider dragline silk investigated by solid-state NMR and X-ray diffraction. International Journal of Biological Macromolecules, 81, 171-179. https://doi.org/10.1016/j.ijbiomac.2015.07.048
  34. Xu, J.J., Wei, Y.F., Jia, H.Q., Xiao, L. and Gong, D.C., 2017, A new perspective on studying burial environment before archaeological excavation: Analyzing bacterial community distribution by high-throughput sequencing. Scientific Reports, 7, 41691. https://doi.org/10.1038/srep41691
  35. Zhang, X.N., Gong, D.C., and Gong, Y.X., 2019, Insight into the orientation behavior of thermal-aged and historic silk fabrics by polarized FTIR microspectroscopy. Journal of Cultural Heritage, 38, 53-63. https://doi.org/10.1016/j.culher.2019.02.007
  36. Zhou, C.Z., Confalonieri, F., Jacquet, M., Perasso, R., Li, Z.G., and Janin, J., 2001, Silk fibroin: Structural implications of a remarkable amino acid sequence. Proteins-Structure Function and Genetics, 44(2), 119-122. https://doi.org/10.1002/prot.1078