Abstract
This research explores how intrinsic factors such as constituents and degradation state can impact the modifications incurred in aged papers during and after X-ray examination. To this end laboratory model papers, artificially aged, and eighteenth and nineteenth century archival documents, with and without additives (gelatin, calcium carbonate) and iron gallate ink, were exposed to Synchrotron X-ray radiation at doses commonly applied (7 Gy to 4 kGy). The threshold dose of 210 Gy previously shown to incur damage in unaged cotton papers falls in this range. Glycosidic scissions, hydroxyl free radicals, UV luminescence and yellowing were measured immediately after the irradiation, and were monitored over a period of three years. Cellulose depolymerization was lower in the aged papers, as well as in the papers containing calcium carbonate and gelatin, than in the unaged fully cellulosic papers. Compared to the papers with no additives, there were more hydroxyl free radicals in the papers with calcium carbonate and slightly less in the gelatin sized papers. UV luminescence and yellowing both appeared post-irradiation, with a delay of several weeks to months. The papers with iron gallate ink showed limited degradation in the low doses range, most probably due to recombination of the free radicals produced. Doses below 4 kGy did not cause yellowing or UV luminescence of the archival papers within the whole monitoring period. The archival papers in good conservation state depolymerized to the same extent as the model papers, while the most degraded archival papers were less impacted than the latter.
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References
T 573 sp-15 (2015) Accelerated temperature aging of printing and writing paper by dry oven exposure apparatus. Technical Association of the Pulp and Paper Industry
Adamo M, Brizzi M, Magaudda G et al (2001) Gamma radiation treatment of paper in different environmental conditions: chemical, physical and microbiological analysis. Restaurator 22:107–131
Ahn K, Banik G, Potthast A (2012) Sustainability of mass-deacidification. part ii: evaluation of alkaline reserve. Restaurator 33:48–75. https://doi.org/10.1515/res-2012-0003
Ahn K, Rosenau T, Potthast A (2013) The influence of alkaline reserve on the aging behavior of book papers. Cellulose 20:1989–2001. https://doi.org/10.1007/s10570-013-9978-3
Albertin F, Astolfo A, Stampanoni M et al (2015) Ancient administrative handwritten documents: X-ray analysis and imaging. J Synchrotron Radiat 22:446–451. https://doi.org/10.1107/S1600577515000314
Barrett T (1992) Evaluating the effect of gelatin sizing with regard to the permanence of paper. In: The Institute of Paper Conservation: conference papers Manchester 1992. Institute of paper conservation, Manchester, pp 228–233
Barrow WJ (1972) Manuscripts and documents: their deterioration and restoration, 2nd edn. University Press of Virginia, Virginia
Bertrand L, Schöeder S, Anglos D et al (2015) Mitigation strategies for radiation damage in the analysis of ancient materials. TrAC Trends Anal Chem 66:128–145. https://doi.org/10.1016/j.trac.2014.10.005
Bicchieri M, Monti M, Piantanida G, Sodo A (2016) Effects of gamma irradiation on deteriorated paper. Radiat Phys Chem 125:21–26. https://doi.org/10.1016/j.radphyschem.2016.03.005
Bouchard J, Méthot M, Jordan B (2006) The effects of ionizing radiation on the cellulose of woodfree paper. Cellulose 13:601–610. https://doi.org/10.1007/s10570-005-9033-0
Burgess HD (1988) Practical Considerations for Conservation Bleaching. JIIC-CG 13:11–26
Carter HA (1996) The Chemistry of paper preservation: part 1. the aging of paper and conservation techniques. J Chem Educ 73:417–420. https://doi.org/10.1021/ed073p417
Castellan A, Ruggiero R, Frollini E et al (2007) Studies on fluorescence of cellulosics. Holzforschung 61:504–508. https://doi.org/10.1515/HF.2007.090
Creagh D (2007) Chapter 1 synchrotron radiation and its use in art, archaeometry, and cultural heritage studies. Physical Techniques in the Study of Art. Archaeology and Cultural Heritage. Elsevier, Amsterdam, pp 1–95
Duconseille A, Andueza D, Picard F et al (2016) Molecular changes in gelatin aging observed by NIR and fluorescence spectroscopy. Food Hydrocoll 61:496–503. https://doi.org/10.1016/j.foodhyd.2016.06.007
Dupont A-L (2003b) Cellulose in lithium chloride/N, N-dimethylacetamide, optimisation of a dissolution method using paper substrates and stability of the solutions. Polymer 44:4117–4126. https://doi.org/10.1016/S0032-3861(03)00398-7
Dupont A-L, Réau D, Bégin P et al (2018) Accurate molar masses of cellulose for the determination of degradation rates in complex paper samples. Carbohydr Polym 202:172–185. https://doi.org/10.1016/j.carbpol.2018.08.134
Dupont A-L (2003a) Gelatine sizing of paper and its impact on the degradation of cellulose during ageing: a study using size-exclusion chromatography. PhD thesis. Universiteit van Amsterdam
Emery JA, Schroeder HA (1974) Iron-catalyzed oxidation of wood carbohydrates. Wood Sci Technol 8:123–137. https://doi.org/10.1007/BF00351367
Ershov BG (1998) Radiation-chemical degradation of cellulose and other polysaccharides. Russ Chem Rev 67:315. https://doi.org/10.1070/RC1998v067n04ABEH000379
Evans R, Wallis AFA (1987) Comparison of cellulose molecular weights determined by high performance size exclusion chromatography and spectrometry. Proc Fourth Int Symp Wood Pulping Chem Paris 1:201–206
Gervais C, Thoury M, Réguer S et al (2015) Radiation damages during synchrotron X-ray micro-analyses of Prussian blue and zinc white historic paintings: detection, mitigation and integration. Appl Phys A 121:949–955. https://doi.org/10.1007/s00339-015-9462-z
Gimat A, Kasneryk V, Dupont A-L et al (2016) Investigating the DMPO-formate spin trapping method for the study of paper iron gall ink corrosion. New J Chem 40:9098–9110. https://doi.org/10.1039/C6NJ01480A
Gimat A, Dupont A-L, Lauron-Pernot H et al (2017) Behavior of cellobiose in iron-containing solutions: towards a better understanding of the dominant mechanism of degradation of cellulosic paper by iron gall inks. Cellulose 24:5101–5115. https://doi.org/10.1007/s10570-017-1434-3
Gimat A, Schöder S, Thoury M et al (2020) Short- and long-term effects of X-ray synchrotron radiation on cotton paper. Biomacromol 21:2795–2807. https://doi.org/10.1021/acs.biomac.0c00512
Gimat A (2016) Comprehension of cellulose depolymerisation mechanisms induced by iron ions. PhD thesis. Université Pierre et Marie Curie
Glaser L, Deckers D (2014) The Basics of fast-scanning xrf element mapping for iron-gall ink palimpsests. Manuscr Cult 7:104–112
Henniges U, Hasani M, Potthast A et al (2013) Electron beam irradiation of cellulosic materials—opportunities and limitations. Materials 6:1584–1598. https://doi.org/10.3390/ma6051584
IAEA (2016) Trends of synchrotron radiation applications in cultural heritage. Forensics and Materials Science International Atomic Energy Agency, Vienna
Jeong M-J, Dupont A-L, de la Rie ER (2014) Degradation of cellulose at the wet–dry interface. II. Study of oxidation reactions and effect of antioxidants. Carbohydr Polym 101:671–683. https://doi.org/10.1016/j.carbpol.2013.09.080
Kabacińska Z, Yate L, Wencka M et al (2017) Nanoscale effects of radiation (UV, X-ray, and γ) on calcite surfaces: implications for its mechanical and physico-chemical properties. J Phys Chem C 121:13357–13369. https://doi.org/10.1021/acs.jpcc.7b03581.s001
Kocar D, Strlic M, Kolar J et al (2005) Chemiluminescence from paper III: the effect of superoxide anion and water. Polym Degrad Stab 88:407–414. https://doi.org/10.1016/j.polymdegradstab.2004.12.005
Kozachuk M, Suda A, Ellis L et al (2016) Possible radiation-induced damage to the molecular structure of wooden artifacts due to micro-computed tomography, handheld X-ray fluorescence, and X-ray photoelectron spectroscopic techniques. J Conserv Mus Stud 14:2–6. https://doi.org/10.5334/jcms.126
Mantler M, Klikovits J (2004) Analysis of art objects and other delicate samples: Is XRF really nondestructive? Powder Diffr 19:16–19. https://doi.org/10.1154/1.1649962
Missori M, Righini M, Dupont A-L (2006) Gelatine sizing and discoloration: A comparative study of optical spectra obtained from ancient and artificially aged modern papers. Opt Commun 263:289–294. https://doi.org/10.1016/j.optcom.2006.02.004
Moini M, Rollman CM, Bertrand L (2014) Assessing the impact of synchrotron X-ray irradiation on proteinaceous specimens at macro and molecular levels. Anal Chem 86:9417–9422. https://doi.org/10.1021/ac502854d
Nevell TP (1985) Degradation of cellulose by acids, alkalis and mechanicals means. Chapter 9. In: Nevell TP, Zeronian SH (eds) Cellulose chemistry and its applications. Ellis Horwood, Chichester, pp 223–242
Poggi G, Sistach MC, Marin E et al (2016) Calcium hydroxide nanoparticles in hydroalcoholic gelatin solutions (GeolNan) for the deacidification and strengthening of papers containing iron gall ink. J Cult Herit 18:250–257. https://doi.org/10.1016/j.culher.2015.10.005
Potthast A, Henniges U, Banik G (2008) Iron gall ink-induced corrosion of cellulose: aging, degradation and stabilization. Part 1: model paper studies. Cellulose 15:849–859. https://doi.org/10.1007/s10570-008-9237-1
Pouyet E, Devine S, Grafakos T et al (2017) Revealing the biography of a hidden medieval manuscript using synchrotron and conventional imaging techniques. Anal Chim Acta 982:20–30. https://doi.org/10.1016/j.aca.2017.06.016
Reissland B (1999) Ink corrosion aqueous and non aqueous treatment of paper objects—state of the art. Restaurator 20:167–180
Röhrling J, Potthast A, Rosenau T et al (2002) A novel method for the determination of carbonyl groups in cellulosics by fluorescence labeling. 2. Valid Appl Biomacromol 3:969–975. https://doi.org/10.1021/bm020030p
Ross-Murphy SB (1985) Properties and uses of cellulose solutions. Chapter 8. In: Nevell TP, Zeronian S (eds) Cellulose Chemistry and its Applications. Ellis Horwood, Chichester, pp 202–222
Rouchon V, Belhadj O (2016) Calcium hydrogen carbonate (bicarbonate) deacidification: what you always wanted to know but never dared asking. J Pap Conserv 17:125–127. https://doi.org/10.1080/18680860.2016.1287406
Rouchon V, Duranton M, Burgaud C et al (2011) Room-temperature study of iron gall ink impregnated paper degradation under various oxygen and humidity conditions: time-dependent monitoring by viscosity and X-ray absorption near-edge spectrometry measurements. Anal Chem 83:2589–2597. https://doi.org/10.1021/ac1029242
Rouchon V, Belhadj O, Duranton M et al (2016) Application of Arrhenius law to DP and zero-span tensile strength measurements taken on iron gall ink impregnated papers: relevance of artificial ageing protocols. Appl Phys A 122:773. https://doi.org/10.1007/s00339-016-0307-1
Selih VS, Strlic M, Kolar J, Pihlar B (2007) The role of transition metals in oxidative degradation of cellulose. Polym Degrad Stab 92:1476–1481. https://doi.org/10.1016/j.polymdegradstab.2007.05.006
Sequeira S, Casanova C, Cabrita EJ (2006) Deacidification of paper using dispersions of Ca(OH)2 nanoparticles in isopropanol. Study of Efficiency J Cult Herit 7:264–272. https://doi.org/10.1016/j.culher.2006.04.004
Shinotsuka H, Tanuma S, Powell CJ, Penn DR (2015) Calculations of electron inelastic mean free paths. X. Data for 41 elemental solids over the 50 eV to 200 keV range with the relativistic full Penn algorithm. Surf Interface Anal 47:1132–1132. https://doi.org/10.1002/sia.5861
T 211 om-02 (2002) Ash in wood, pulp, paper and paperboard: combustion at 525 °C. Technical Association of the Pulp and Paper Industry
T 230 om-19 (1999) Viscosity of pulp (capillary viscometer method). Technical Association of the Pulp and Paper Industry
T 402 sp-08 (2013) Standard conditioning and testing atmospheres for paper, board, pulp handsheets, and related products. Technical Association of the Pulp and Paper Industry
T 509 om-15 (2002) Hydrogen ion concentration (pH) of paper extracts (cold extraction method). Technical Association of the Pulp and Paper Industry
T 553 om-00 (2000) Alkalinity of paper as calcium carbonate (alkaline reserve of paper). Technical Association of the Pulp and Paper Industry
T 430 cm-99 (1999) Copper Number of Pulp, Paper, and Paperboard. Technical Association of the Pulp and Paper Industry
T 502 cm-07 (1998) Equilibrium relative humidity of paper and paperboard. Technical Association of the Pulp and Paper Industry
Whitmore PM, Bogaard J (1994) Determination of the cellulose scission route in the hydrolytic and oxidative degradation of paper. Restaurator 15:26–45. https://doi.org/10.1515/rest.1994.15.1.26
Yova D, Hovhannisyan V, Theodossiou T (2001) Photochemical effects and hypericin photosensitized processes in collagen. J Biomed Opt 6:52–57. https://doi.org/10.1117/1.1331559
Acknowledgments
We are grateful to synchrotron Soleil for the access to the PUMA beamline within the proposal 20181723 and to Tülin Okbinoglu for technical help on the beamline. We thank Samia Rebaa and Naomi Nganzami Ebale, undergraduate chemistry students (Sorbonne Université), for help with photography and spectroscopy. We also thank Sabrina Paris Lacombe and Oulfa Belhadj for technical help with Size Exclusion Chromatography and Scanning Electron Microscopy, respectively.
Funding
This research was supported by Paris Seine Graduate School of Humanities, Creation, Heritage, Investissements d’Avenir ANR-17-EURE-0021-Foundation for Cultural Heritage Science.
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Conception of the research and methodology: AG, ALD, MT, SC; PUMA Irradiation Experiment: AG, SC; physico-chemical characterizations: AG, Writing-original draft preparation: AG, ALD; Writing-review and editing: AG, ALD, MT, SC; Supervision: ALD, MT, SC.
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Gimat, A., Schöder, S., Thoury, M. et al. Degradation of historical paper induced by synchrotron X-ray technical examination. Cellulose 29, 4347–4364 (2022). https://doi.org/10.1007/s10570-022-04552-3
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DOI: https://doi.org/10.1007/s10570-022-04552-3