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Accelerated Degradation Test and Failure Analysis of Rapid Curing Epoxy Resin for Restoration of Cultural Heritage

문화재 복원용 속(速)경화형 Epoxy계 수지의 가속열화시험 및 고장분석 연구

  • Nam, Byeong Jik (Restoration Technology Division, National Research Institute of Cultural Heritage) ;
  • Jang, Sung Yoon (Conservation Science Division, National Research Institute of Cultural Heritage)
  • 남병직 (국립문화재연구소 복원기술연구실) ;
  • 장성윤 (국립문화재연구소 보존과학연구실)
  • Received : 2017.10.16
  • Accepted : 2017.11.27
  • Published : 2017.12.20

Abstract

In this study, the degradation properties by temperature stress of $Araldite^{(R)}$ rapid-curing epoxy resin used for inorganic cultural heritages, was identified. The tensile and tensile shear strength of durability decreased for 12,624 hours at temperatures of $40{\sim}60^{\circ}C$. In terms of stability of external stress and temperature, the slow-curing epoxy was superior to the rapid-curing epoxy, and cultural heritage conservation plans should therefore consider the strength and stress properties of restoration materials. Color differences increased for 12,624 hours at temperatures of $40{\sim}60^{\circ}C$, and glossiness decreased. Both color and gloss stability were weak, which necessitates the improvement of optical properties. Thermal properties (weight loss, decomposition temperature, and glass transition temperature) of adhesives are linked to mechanical properties. Interfacial properties of the adherend and water vapor transmission rates of adhesives are linked to performance variation. For porous media (ceramics, brick, and stone), isothermal and isohumid environments are important. For outdoor artifacts on display in museums, changes in physical properties by exposure to varying environmental conditions need to be minimized. These results can be used as baseline data in the study of the degradation velocity and lifetime prediction of rapid-curing epoxy resin for the restoration of cultural heritages.

본 연구에서는 문화재 복원용 속(速)경화형 Epoxy계 수지인 $Araldite^{(R)}$ rapid의 온도 스트레스에 의한 열화 특성을 분석하였다. 인장강도 및 접착강도는 $40{\sim}60^{\circ}C$에서 12,624시간까지 감소하여 내구성 및 접착특성의 미약한 열화가 발생하였다. 외부 응력 및 온도에 대한 안정성은 속(速)경화형에 비해 일반 경화형 Epoxy계 수지가 우수하여, 복원부의 강도 특성 및 응력 상태를 고려한 복원재료의 적절한 선택과 적용이 요구된다. $40{\sim}60^{\circ}C$에서 12,624시간까지 색차의 증가와 광택도의 감소 등 색상 및 광택 안정성은 취약하여, 향후 광학특성의 개선을 위한 안정성 향상 연구가 필요하다. 특히 접착제의 열적 특성(중량감소량, 열분해온도, 유리전이온도)은 기계적 물성 변화에 부분적으로 관여하였고, 피착재의 계면 특성 및 접착제의 기체투과특성(수분투과도)은 접착성능의 중요인자로 작용하였다. 따라서 도자기, 벽돌 및 석재와 같은 다공성 재질의 경우 항온항습에 의한 보존환경 관리가 중요하며, 옥외 전시유물의 경우 노출환경에 의한 물성 변화를 최소화할 수 있는 보존대책의 수립이 절실하다. 향후 이러한 결과는 문화재에 사용된 Epoxy계 수지의 열화속도 및 수명예측 자료로 활용될 것으로 기대된다.

Keywords

References

  1. Ahn, S.M., Lee, Y.D. and Kim, D.S., 2003, Galmeori site Jinan, Jeollabuk-do, Honam cultural properties research center excavation report ; 13, 62-63, 340-341, 344-345, Honam cultural property research center. (in Korean with English abstract).
  2. Cho, N.C., Kim, S.C., Kim, W.H. and Shin, Y.S., 2010, A study on the bonding materials used for the great jar of the proto-three kingdoms period from Daechuri site, Pyeongtaek. Journal of Conservation Science, 26(4), 371-376. (in Korean with English abstract).
  3. Choi, Y.S., Chae, I.S., Kang, Y.S., Won, J.O., Kim, J.J. and Kim, S.D., 2011, Tuning thermal expansion coefficient of composites containing epoxy resin/inorganic additives for stone conservation. Journal of Conservation Science, 27(4), 431-440. (in Korean with English abstract).
  4. Choi, Y.S., Lee, J.H., Jeong, Y.S., Kang, Y.S., Won, J.O., Kim, J.J. and Kim, S.D., 2012, Performance improvement of hydrogenated bisphenol-A epoxy resin/inorganic additives composites for stone conservation by controlling their composition. Journal of Conservation Science, 28(3), 265-276. (in Korean with English abstract). https://doi.org/10.12654/JCS.2012.28.3.265
  5. Down, J.L., 1984a, Adhesive testing at the Canadian Conservation Institute, Past and future. in Brommelle, N.S. et al.(eds.), Adhesives and consolidants. IIC Preprints of the contributions to the Paris congress, 2-8 september 1984. London, UK: IIC, 4-6.
  6. Down, J.L., 1984b, The yellowing of epoxy resin adhesives: report on natural dark aging. Studies in Conservation, 29(2), 63-76. https://doi.org/10.2307/1506076
  7. Down, J.L., 1986, The yellowing of epoxy resin adhesives: report on high-intensity light aging. Studies in Conservation, 31(4), 159-170. https://doi.org/10.2307/1506247
  8. Down, J.L., 2015, Adhesive compendium for conservation. Canadian Conservation Institute, 99-100.
  9. Frigione, M., Lettieri, M., and Mecchi, A.M., 2006, Environmental effects on epoxy adhesives employed for restoration of historical buildings. Journal of Materials in Civil Engineering, 18(5), 715-722. https://doi.org/10.1061/(ASCE)0899-1561(2006)18:5(715)
  10. Grassie, N., Guy M.I. and Tennent, N.H., 1985a, Degradation of epoxy polymers: part 1 - products of thermal degradation of bisphenol-A diglycidyl ether. Polymer Degradation and Stability, 12(1), 65-91. https://doi.org/10.1016/0141-3910(85)90057-6
  11. Grassie, N., Guy M.I. and Tennent, N.H., 1985b, Degradation of epoxy polymers: part 2 - mechanism of thermal degradation of bisphenol-A diglycidyl ether. Polymer Degradation and Stability, 13(1), 11-20. https://doi.org/10.1016/0141-3910(85)90131-4
  12. Grassie, N., Guy, M.I. and Tennent, N.H., 1985c, Degradation of epoxy polymers: part 3 - photo-degradation of bisphenol-A diglycidyl ether. Polymer Degradation and Stability, 3(3), 249-259.
  13. Grassie, N., Guy, M.I. and Tennent, N.H., 1986a, Degradation of epoxy polymers: part 4- thermal degradation of bisphenol-A diglycidyl ether cured with ethylene diamine. Polymer Degradation and Stability, 14(2), 125-137. https://doi.org/10.1016/0141-3910(86)90011-X
  14. Grassie, N., Guy, M.I. and Tennent, N.H., 1986b, Degradation of epoxy polymers: part 5- photo-degradation of bisphenol-A diglycidyl ether cured with ethylene diamine. Polymer Degradation and Stability, 14(3), 209-216. https://doi.org/10.1016/0141-3910(86)90044-3
  15. Han, W.S., Wi, K.C., Park, G.J. and Hong, T.K., 2009, The development of the unfading polyvinyl butyral gap-filling material based on reversible properties and restoration of a punchong plate from Sam-cheon temple site with this polyvinyl butyral product. Journal of Conservation Science, 25(3), 293-298. (in Korean with English abstract).
  16. Han, W.S., Park, G.J., Lim, S.J., Lee, Y.H., Hong, T.K. and Wi, K.C., 2010, The development of the unfading urethane polymer based on reversible properties for ceramics and restoration with this urethane product. Journal of Conservation Science, 26(2), 183-190. (in Korean with English abstract).
  17. Huntsman, 2011, Advance material Araldite$^{(R)}$ rapid transparent.
  18. Hwang, Y.E. and Yoon, S.H., 2011, Effect of combined environmental factors on adhesive shear strengths and chemical structures of adhesives. Composites Research, 24(1), 31-36. (in Korean with English abstract). https://doi.org/10.7234/kscm.2011.24.1.031
  19. Hwang, H.S., Lee, H.S. and Yi, Y.H., 2001, The conservation of a Spanish gourd-style jar(donated object by Sir Ganeko). Conservation Science in Museum, 3, 15-19. (in Korean with English abstract).
  20. Hwang, H.S. and Lee, H.S., 2004, Conservation of ceramicware to be exhibited at Yongsan new national museum at its opening-restoration of blue-and-white porcelain jar with phoenix design and celadon peahen- shaped water dropper-. Conservation Science in Museum, 5, 5-15. (in Korean with English abstract).
  21. Hwang, H.S., 2015, A scientific study on the conservation of pheonix head-shaped glass ewer from the Gyeongju No.98 south mound and the manufacturing technique of gold wires. DONG WON collection of academic papers, 16, 90-107. (in Korean with English abstract).
  22. Kang, H.S. and Ahn, B.C., 1999, Restoration of pottery and celadon for exhibition. Conservation Science in Museum, 1, 33-42. (in Korean with English abstract).
  23. Kim, M.D. and Choi, J.A., 2015, Conservation treatment of comb-shaped bone jewelry from Daeseong-dong tomb No.88, Gimhae. Conservation Science in Museum, 16, 114-121. (in Korean with English abstract).
  24. Kim, M.S., 2006, Failure analysis of polymer-guideline. Publication ING, 82-91.
  25. Kim, S.D., Shin, E.J., Lee, J.W., Wi, G.C. and Yang, H.J., 2002, Restoration and conservation treatment about north monk-stupa.east monk-stupa in Yeongoksa. Conservation Studies, 23, 163-177. (in Korean with English abstract).
  26. Kim, S.D. and Choi, J.H., 2013, Conservation treatment of the Bonghwa Bukjiri Maaeyeoraejwasang(rock-carved seated buddha statue), Korea. Conservation Studies, 34, 6-17. (in Korean with English abstract).
  27. Kim, W.H., Cheong, D.S., Bae, J.S., Jee, J.Y. and Wi, K.C., 2014, A study on the development and physical properties of low yellowing epoxy for ceramic preservation. Journal of Conservation Science, 30(2), 181-187. (in Korean with English abstract). https://doi.org/10.12654/JCS.2014.30.2.07
  28. Kim, J.H., Jeong, K.W., Yoo, Y.S., Yang, K.J. and Park, Y.K., 1999, Evaluation of aging properties of silicone rubber for outdoor by artificial acid rain immersion and inclined-plang method. Sungkyunkwan University International Journal of Research Institute of Science and Technology, 50(1), 53-64. (in Korean with English abstract).
  29. Kim, J.H., Choi, K.Y., Joo, H.J., Kim, B.L. and Park, S.J., 2005, A study on the water resistance and thermo-mechanical behaviors of epoxy adhesives. Elastomer, 40(3), 166-173. (in Korean with English abstract).
  30. Kim, J.H., Joo, H.J., Kim, J.H., Kim, F.L. and Park, S.J., 2006, Effect of thermal aging temperature on weight loss and glass transition temperature of epoxy adhesives. Elastomer, 41(1), 19-26. (in Korean with English abstract).
  31. Kim, J.W., Jung, T.H. and Yong, B.J., 2007, Conservation treatment of seated stone Bhaishajyaguru-vaidurya buddha statue from Yongjang-gye. Conservation Science in Museum, 8, 3-11. (in Korean with English abstract).
  32. Kim, J.W. and Lee, S.R., 2013, Conservation treatment of Janghang-ri stone standing buddha. Conservation Science in Museum, 14, 115-124. (in Korean with English abstract).
  33. Kim, T.G., Yang, J.H. and Cho, S.B., 1998, A study on the enhancement of bonding strength for dissimilar materials. Theses collection of the institute of advanced materials, 10, 25-32. (in Korean with English abstract).
  34. Kwon, H.N. and Ahn, B.C., 1999, Report on the conservation treatment for the artifacts exhibited in the newly-opened Kimhae National Museum. Conservation Science in Museum, 1, 15-26. (in Korean with English abstract).
  35. Lee, E.J. and Jang, S.Y., 2016, Evaluation of physical properties according to mixing ratio and the survey of the current situation for epoxy resin used in conservation. Journal of Conservation Science, 32(2), 223-234. (in Korean with English abstract). https://doi.org/10.12654/JCS.2016.32.2.11
  36. Lee, H.K., Choi, H.W., Lee, S.L. and Gwak, H.I., 2013, Conservation of the human shaped terra cotta mask excavated from Jungcheon-ri, Jinju. Conservation Science in Museum, 14, 23-28. (in Korean with English abstract).
  37. Lee, H.S. and Yun, E.Y., 2007, Conservation of porcelain possessed by Jeonju National Museum, -Rice-bale-shaped battle white porcelain and big jar with incised fish design buncheon ware-. Conservation Science in Museum, 8, 31-40. (in Korean with English abstract).
  38. Lee, M.S., Jung, M.H., Jung, Y.D. and Lee, C.H., 2006, Deterioration and conservation treatment of the three storied stone pagoda in Seoak-ri, Gyeongju. Journal of Conservation Science, 18, 63-74. (in Korean with English abstract).
  39. Lee, S.S., 1978, Conservation treatment of earthenware funerary objects in the shape of a warrior on horseback. MISULJARYO, 22. (in Korean).
  40. Lee, S.S., 1993, Conservation of pottery. Journal of Conservation Science, 2(2), 63-69. (in Korean).
  41. Lee, S.S. and Ahn, B.C., 2008, A pioneer in the conservation and restoration of cultural assets. Hanrimwon, Seoul, 133-144. (in Korean).
  42. Lee, S.Y., 2002, Analysis of surface ageing mechanism by UV-treatment on outdoor polymeric insulating materials. Master's thesis, Inha University, Incheon. (in Korean with English abstract).
  43. Lim, K.B., Nam, K.D., Kim, K.H., Park, S.H. and Hwang, M.H., 2008, A study on the thermal degradation properties of epoxy resin for cast resin transformer. Journal of Korean Institute of Fire Sci. & Eng., 22(2), 44-48. (in Korean with English abstract).
  44. Meyer, F., Sanz, G., Eceiza, A. and Mondragon, I., 1995, The effect of stoichiometry and thermal history during cure on structure and properties of epoxy networks. Polymer, 36(7), 1407-1414. https://doi.org/10.1016/0032-3861(95)95918-Q
  45. Michaels, A.S. and Bixler, H.J., 1961, Flow of gases through polyethylene. Journal of Polymer Science, 50(154), 413. https://doi.org/10.1002/pol.1961.1205015412
  46. Nam, B.J., 2007, Study on the weathering of adhesives and restoration materials for iron artifacts, Master's Thesis, Gyeongju University. (in Korean with English abstract).
  47. Nam, B.J., Jeong, S.R. and Jang, S.Y., 2012, Study on the demand characteristics of epoxy resins applied to the restoration of ceramics. Journal of Adhesion and Interface, 13(4), 171-181. (in Korean with English abstract). https://doi.org/10.17702/jai.2012.13.4.171
  48. Nam, B.J. and Jang, S.Y., 2015, A study on the degradation properties of DGEBA/TETA epoxy system for Restoration of ceramics by temperature. Journal of Conservation Science, 31(4), 373-386. (in Korean with English abstract). https://doi.org/10.12654/JCS.2015.31.4.05
  49. National Research Institute of Cultural Heritage, 2012, Stability estimation of adhesives for ceramic restoration : result report. 28. (in Korean with English abstract).
  50. Osawa, Z., Wu, S. and Konoma, F., 1988, Properties and chemiluminescence of polypropylene stored for a long period. Polymer Degradation and Stability, 22(2), 97-107. https://doi.org/10.1016/0141-3910(88)90034-1
  51. Park, G.J., Lee, J.H. and Kim, S.K., 2005, Conservation work on the blue & white porcelain jar with cloud & dragon design from the National Palace Museum Collection. The Journal of Conservation of Cultural Properties, 2, 58-73. (in Korean with English abstract).
  52. Park, G.J., 2007, Conservation and research on the porcelain of excavated at Samcheon temple site. The Journal of Conservation of Cultural Properties, 4, 15-30. (in Korean with English abstract).
  53. Park, G.J., 2010, Conservation treatment of ceramic wares and synthesis of non-yellowing Butvar resin. Ph. D. dissertation, Hanseo University, Seosan. (in Korean with English abstract).
  54. Park, H.S., 2012, Conservation of reliquary from the east pagoda at Gameunsa temple site. Conservation Science in Museum, 13, 59-69. (in Korean with English abstract).
  55. Park, Y.S., 2008, Yanggi-ri site Anseong, Jungwon cultural properties institute excavation report. 50, 209-210. (in Korean with English abstract).
  56. Setnescu, R., Jipa, S., Setnescu, T., Podina, C. and Osawa, Z., 1998, Chemiluminescence study on the oxidation of several polyolefins: II. Chemiluminescence from ${\gamma}$-irradiated polymers. Polymer Degradation and Stability, 61(1), 109-117. https://doi.org/10.1016/S0141-3910(97)00137-7
  57. Shaw, S.J., 1996, Adhesives in demanding applications. Polymer International, 41(2), 193-207. https://doi.org/10.1002/(SICI)1097-0126(199610)41:2<193::AID-PI623>3.0.CO;2-6
  58. Shim, S.C. and Chang, S.K., 1979, Photodegradation of polymers. Polymer(Korea), 3(6), 346-347. (in Korean).
  59. Shim, S.H., 1998, The effect of acid rain on the tracking resistance of epoxy resin for outdoor use. Samchok National University International Journal of Research Institute of Industrial Science and Technology, 3, 11-16. (in Korean with English abstract).
  60. Takahara, S., Yoshida, T., Tanabe, T., Okada, M. and Xu, Q., 2006, Temperature dependence of luminescence from a silica glass under in-reactor irradiation. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 250(1-2), 377-381. https://doi.org/10.1016/j.nimb.2006.04.141
  61. Tennent, N.H., 1979, Clear and pigmented epoxy resins for stained glass conservation: light aging studies. Studies in Conservation, 24, 153-164.
  62. Tennent, N.H., 1991, An epoxy resin update, Text of lecture delivered to UKIC ceramics and glass conservation group meeting on adhesives and consolidant. Available from author at Department of Chemistry, University of Glasgow, Glasgow G12 8QQ, UK.
  63. Theophanides, T., 2012, Infrared spectroscopy-materials science. Engineering and Technology, InTech, 267.
  64. Yang, P.S. and Seo, J.H., 2011, A study on the changes process repair and restoration method of ceramic. Journal of Conservation Science, 27(1), 49-59. (in Korean with English abstract).
  65. Yoon, S.H., 2004, Study of degradation of epoxy and urethane coatings by UV irradiation. Master's thesis, Pukyong National University, Busan, 1-7. (in Korean with English abstract).
  66. Yoshino, K., Yin, X.H., Tada, K., Kawai, T., Hamaguchi, M., Araki, H., Sugimoto, R., Uchikawa, N., Asanuma, T., Kawahigashi, M. and Kato, H. 1996, Novel properties of new type conducting and insulating polymers and their composites. IEEE Transactions on DEI, 3(3), 331-344. https://doi.org/10.1109/94.506204