Frontiers of Physics

, 13:138202 | Cite as

NMR investigation of degradation processes of ancient and modern paper at different hydration levels

  • Domenico Mallamace
  • Sebastiano Vasi
  • Mauro Missori
  • Francesco Mallamace
  • Carmelo Corsaro
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Part of the following topical collections:
  1. Water and Water Systems

Abstract

The degradation process of cellulose-made materials was investigated by means of nuclear magnetic resonance (NMR) spectroscopy, with particular emphasis on the role of water and on the hydration mechanism of cellulose fibrils. To accomplish this, the structure and dynamics of water within ancient and modern samples with different aging histories were investigated. The results mainly indicated that hydrolytic and oxidative reactions provoked the formation of acidic by-products. Furthermore, degradation processes were enhanced by higher amounts of water giving a progressive consumption of the amorphous regions of the cellulose. We propose NMR experiments as a benchmark for characterization of the degradation state of paper, as well as for investigating the effectiveness of restoration treatments.

Keywords

ancient paper degradation NMR hydration solvent dynamics 
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Notes

Acknowledgements

The authors acknowledge the Consiglio Nazionale delle Ricerche and the Istituto Centrale per il Restauro e la Conservazione del Patrimonio Archivistico e Librario (Roma, Italy) for their support. J. Łojewska is kindly acknowledged for providing the P2 samples. D.M.’s activity was carried out within the framework of the NANORESTART project, which has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No. 646063.

References

  1. 1.
    F. Mallamace, C. Corsaro, D. Mallamace, S. Vasi, C. Vasi, P. Baglioni, S. V. Buldyrev, S. H. Chen, and H. E. Stanley, Energy landscape in protein folding and unfolding, Proc. Natl. Acad. Sci. USA 113(12), 3159 (2016)ADSCrossRefGoogle Scholar
  2. 2.
    F. Mallamace, C. Corsaro, D. Mallamace, S. Vasi, C. Vasi, and G. Dugo, The role of water in protein’s behavior: The two dynamical crossovers studied by NMR and FTIR techniques, Comput. Struct. Biotechnol. J. 13, 33 (2015)CrossRefMATHGoogle Scholar
  3. 3.
    F. Mallamace, P. Baglioni, C. Corsaro, S. H. Chen, D. Mallamace, C. Vasi, and H. E. Stanley, The influence of water on protein properties, J. Chem. Phys. 141(16), 165104 (2014)ADSCrossRefGoogle Scholar
  4. 4.
    F. Mallamace, C. Corsaro, D. Mallamace, S. Vasi, C. Vasi, H. E. Stanley, and S. H. Chen, Some thermodynamical aspects of protein hydration water, J. Chem. Phys. 142(21), 215103 (2015)ADSCrossRefMATHGoogle Scholar
  5. 5.
    D. Klemm, B. Philipp, T. Heinze, U. Heinze, and W. Wagenknecht, Volume I: Fundamentals and Analytical Methods, Weinheim: WILEY-VCH Verlag GmbH, 1998Google Scholar
  6. 6.
    A. C. O’Sullivan, The structure slowly unravels, Cellulose 4 (3), 173 (1997)CrossRefGoogle Scholar
  7. 7.
    X. Qiu and S. Hu, “Smart” materials based on cellulose: A review of the preparations, properties, and applications, Materials (Basel) 6 (3), 738 (2013)ADSCrossRefGoogle Scholar
  8. 8.
    J. Kim, Cellulose as a smart material, in: R. Malcolm Brown and Inder M. Saxena (Eds.), Cellulose: Molecular and Structural Biology, Springer Netherlands, 323–343 (2007)CrossRefGoogle Scholar
  9. 9.
    M. Missori, C. Mondelli, M. De Spirito, C. Castellano, M. Bicchieri, R. Schweins, G. Arcovito, M. Papi, and A. C. Castellano, Modifications of the mesoscopic structure of cellulose in paper degradation, Phys. Rev. Lett. 97(23), 238001 (2006)ADSCrossRefGoogle Scholar
  10. 10.
    M. De Spirito, M. Missori, M. Papi, G. Maulucci, J. Teixeria, C. Castellano, and G. Arcovito, Modifications in solvent clusters embedded along the fibers of a cellulose polymer network cause paper degradation, Phys. Rev. E 77(4), 041801 (2008)ADSCrossRefGoogle Scholar
  11. 11.
    K. L. Kato and R. E. Cameron, A review of the relationship between thermally-accelerated ageing of paper and hornification, Cellulose 6 (1), 23 (1999)CrossRefGoogle Scholar
  12. 12.
    G. Banik and I. Brückle, Structure and properties of dry and wet paper, in: Paper and Water: A Guide for Conservators, Amsterdam: Elsevier, 81–105 (2011)Google Scholar
  13. 13.
    L. Teodonio, M. Missori, D. Pawcenis, J. Lojewska, and F. Valle, Nanoscale analysis of degradation processes of cellulose fibers, Micron 91, 75 (2016)CrossRefGoogle Scholar
  14. 14.
    C. Corsaro, D. Mallamace, J. Lojewska, F. Mallamace, L. Pietronero, and M. Missori, Molecular degradation of ancient documents revealed by 1H HR-MAS NMR spectroscopy, Sci. Rep. 3, 2896 (2013)ADSCrossRefGoogle Scholar
  15. 15.
    D. Hunter, Papermaking: The History and Technique of an Ancient Craft, New York: Dover Publications, 1978Google Scholar
  16. 16.
    D. Capitani, A. L. Segre, D. Attanasio, B. Blicharska, B. Focher, and G. Capretti, 1H NMR relaxation study of paper as a system of cellulose and water, Tappi J. 79, 113 (1996)Google Scholar
  17. 17.
    D. Capitani, N. Proietti, F. Ziarelli, and A. L. Segre, NMR study of water-filled pores in one of the most widely used polymeric material: The paper, Macromolecules 35 (14), 5536 (2002)Google Scholar
  18. 18.
    C. Federici, P. Mufanò, and M. S. Storace, Ancient paper and its NMR characterization, Sci. Technol. Cult. Herit. 5, 37 (1996)Google Scholar
  19. 19.
    M. Missori, M. Righini, and A. L. Dupont, Gelatine sizing and discoloration: A comparative study of optical spectra obtained from ancient and artificially aged modern papers, Opt. Commun. 263(2), 289 (2006)ADSCrossRefGoogle Scholar
  20. 20.
    J. Kolar, Mechanism of autoxidative degradation of cellulose, Restaurator (Copenh.) 18(4), 163 (1997)Google Scholar
  21. 21.
    S. Zervos, Natural and accelerated ageing of cellulose and paper: A literature review, in: A. Lejeune and T. Deprez (Eds.), Cellulose: Structure and Properties, Derivatives and Industrial Uses, Nova Publishing, 155–203 (2010)Google Scholar
  22. 22.
    T. jewski, P. Miskowiec, M. Missori, A. Lubanska, L. M. Proniewicz, and J. Lojewska, FTIR and UV/vis as methods for evaluation of oxidative degradation of model paper: DFT approach for carbonyl vibrations, Carbohydr. Polym. 82 (2), 370 (2010)CrossRefGoogle Scholar
  23. 23.
    A. Mosca Conte, A. Knapik, J. Bagniuk, R. Del Sole, J. Lojewska, and M. Missori, Role of cellulose oxidation in the yellowing of ancient paper, Phys. Rev. Lett. 108(15), 158301 (2012)ADSCrossRefGoogle Scholar
  24. 24.
    T. jewski, T. Sawoszczuk, J. M. Lagan, K. Zieba, A. Baranski, and J. Lojewska, Furfural as a marker of cellulose degradation. A quantitative approach, Appl. Phys. A 100(3), 873 (2010)ADSCrossRefGoogle Scholar
  25. 25.
    Z. Souguir, A. L. Dupont, and E. R. de la Rie, Formation of brown lines in paper: Characterization of cellulose degradation at the wet-dry interface, Biomacromolecules 9 (9), 2546 (2008)CrossRefGoogle Scholar
  26. 26.
    A. L. Dupont, A. Seemann, and B. Lavédrine, Capillary electrophoresis with electrospray ionization-mass spectrometry for the characterization of degradation products in aged papers, Talanta 89, 301 (2012)CrossRefGoogle Scholar
  27. 27.
    S. Belton, NMR studies of hydration in low water content biopolymer systems, Magn. Reson. Chem. 49, S127 (2011)CrossRefGoogle Scholar
  28. 28.
    C. Violante, L. Teodonio, A. Mosca Conte, O. Pulci, I. Kupchak, and M. Missori, An ab-initio approach to cultural heritage: The case of ancient paper degradation, Phys. Status Solidi B 252(1), 112 (2015)ADSCrossRefGoogle Scholar
  29. 29.
    M. Missori, Optical spectroscopy of ancient paper and textiles, Nuovo Cimento C 39, 293 (2016)ADSGoogle Scholar
  30. 30.
    M. Missori, O. Pulci, L. Teodonio, C. Violante, I. Kupchak, J. Bagniuk, J. jewska, and A. M. Conte, Optical response of strongly absorbing inhomogeneous materials: Application to paper degradation, Phys. Rev. B 89(5), 054201 (2014)ADSCrossRefGoogle Scholar
  31. 31.
    A. Mosca Conte, O. Pulci, M. C. Misiti, J. Lojewska, L. Teodonio, C. Violante, and M. Missori, Visual degradation in Leonardo da Vinci’s iconic self-portrait: A nanoscale study, Appl. Phys. Lett. 104(22), 224101 (2014)ADSCrossRefGoogle Scholar
  32. 32.
    T. Rosenau, A. Potthast, K. Krainz, Y. Yoneda, T. Dietz, Z. P. I. Shields, and A. D. French, Chromophores in cellulosic, VI: First isolation and identification of residuals chromophores from aged cotton linters, Cellulose 18(6), 1623 (2011)CrossRefGoogle Scholar
  33. 33.
    A. Abragam, The Principles of Nuclear Magnetism, London: Oxford University Press, 1961Google Scholar
  34. 34.
    S. Moestue, B. Sitter, T. Frost Bathen, M. B. Tessem, and I. S. Gribbestad, HR MAS MR spectroscopy in metabolic characterization of cancer, Curr. Top. Med. Chem. 11 (1), 2 (2011)CrossRefGoogle Scholar
  35. 35.
    A. Torre, F. Trischitta, C. Corsaro, D. Mallamace, and C. Faggio, Digestive cells from Mytilus galloprovincialis show a partial regulatory volume decrease following acute hypotonic stress through mechanisms involving inorganic ions, Cell Biochem. Funct. 31(6), 489 (2013)CrossRefGoogle Scholar
  36. 36.
    O. Beckonert, M. Coen, H. C. Keun, Y. Wang, T. M. D. Ebbels, E. Holmes, J. C. Lindon, and J. K. Nicholson, High-resolution magic-anglespinning NMR spectroscopy for metabolic profiling of intact tissues, Nat. Protoc. 5(6), 1019 (2010)CrossRefGoogle Scholar
  37. 37.
    C. Corsaro, D. Mallamace, S. Vasi, V. Ferrantelli, G. Dugo, and N. Cicero, 1H HR-MAS NMR spectroscopy and the metabolite determination of typical foods in mediterranean diet, J. Anal. Methods Chem. 2015, 1 (2015)CrossRefGoogle Scholar
  38. 38.
    N. Cicero, C. Corsaro, A. Salvo, S. Vasi, S. V. Giofré, V. Ferrantelli, V. Di Stefano, D. Mallamace, and G. Dugo, The metabolic profile of lemon juice by proton HR-MAS NMR: The case of the PGI Interdonato Lemon of Messina, Nat. Prod. Res. 29(20), 1894 (2015)CrossRefGoogle Scholar
  39. 39.
    C. Corsaro, D. Mallamace, S. Vasi, L. Pietronero, F. Mallamace, and M. Missori, The role of water in the degradation process of paper using 1H HR-MAS NMR spectroscopy, Phys. Chem. Chem. Phys. 18(48), 33335 (2016)CrossRefGoogle Scholar
  40. 40.
    D. Mallamace, S. Vasi, M. Missori, and C. Corsaro, New insight into hydration and aging mechanisms of paper by the line shape analysis of proton NMR spectra, Il Nuovo Cimento C 39, 309 (2016)ADSGoogle Scholar
  41. 41.
    J. H. Chen and S. Singer, High-resolution magic-anglespinning NMR spectroscopy, in: J. C. Lindon, J. K. Nickolson, and E. Holmes (Eds.), The Handbook of Metabolonomics and Metabolomics, New York: Elsevier, 113–147 (2007)CrossRefGoogle Scholar
  42. 42.
    J. C. Lindon, E. Holmes, and J. K. Nicholson, Metabolonomics in pharmacheutical R&D, FEBS J. 274(5), 1140 (2007)CrossRefGoogle Scholar
  43. 43.
    E. R. Andrew, A. Bradbury, and R. G. Eades, Removal of bipolar broadening of nuclear magnetic resonance spectra of solids by specimen rotation, Nature 183 (4678), 1802 (1959)ADSCrossRefGoogle Scholar
  44. 44.
    B. Blicharska and M. Kluza, NMR relaxation in cellulose pulp, Colloids Surf. A Physicochem. Eng. Asp. 115, 137 (1996)CrossRefGoogle Scholar
  45. 45.
    D. Topgaard and O. Söderman, Changes of cellulose fiber wall structure during drying investigated using NMR self-diffusion and relaxation experiments, Cellulose 9 (2), 139 (2002)CrossRefGoogle Scholar
  46. 46.
    N. Matubayasi, C. Wakai, and M. Nakahara, NMR study of water structure in super- and subcritical conditions, Phys. Rev. Lett. 78 (13), 2573 (1997)ADSCrossRefGoogle Scholar
  47. 47.
    K. Modig, B. G. Pfrommer, and B. Halle, Temperaturedependent hydrogen-bond geometry in liquid water, Phys. Rev. Lett. 90(7), 075502 (2003)ADSCrossRefGoogle Scholar
  48. 48.
    D. Sebastiani and M. Parrinello, Ab-initio study of NMR chemical shifts of water under normal and supercritical conditions, ChemPhysChem 3(8), 675 (2002)CrossRefGoogle Scholar
  49. 49.
    F. Mallamace, C. Corsaro, M. Broccio, C. Branca, N. Gonzalez-Segredo, J. Spooren, S. H. Chen, and H. E. Stanley, NMR evidence of a sharp change in a measure of local order in deeply supercooled confined water, Proc. Natl. Acad. Sci. USA 105 (35), 12725 (2008)ADSCrossRefGoogle Scholar
  50. 50.
    C. Corsaro, J. Spooren, C. Branca, N. Leone, M. Broccio, C. Kim, S. H. Chen, H. E. Stanley, and F. Mallamace, Clustering dynamics in water/methanol mixtures: A nuclear magnetic resonance study at 205 K < T < 295 K, J. Phys. Chem. B 112(34), 10449 (2008)CrossRefGoogle Scholar
  51. 51.
    M. F. Froix and R. Nelson, The interaction of water with cellulose from nuclear magnetic resonance relaxation times, Macromolecules 8(6), 726 (1975)ADSCrossRefGoogle Scholar
  52. 52.
    D. Majolino, C. Corsaro, V. Crupi, V. Venuti, and U. Wanderlingh, Water diffusion in nanoporous glass: An NMR study at different hydration levels, J. Phys. Chem. B 112(13), 3927 (2008)CrossRefGoogle Scholar
  53. 53.
    M. Paci, C. Federici, D. Capitani, N. Perenze, and A. L. Segre, NMR study of paper, Carbohydr. Polym. 26 (4), 289 (1995)CrossRefGoogle Scholar
  54. 54.
    S. Hayashi and E. Akiba, Nuclear spin-lattice relaxation mechanisms in kaolinite confirmed by magic-angle spinning, Solid State Nucl. Magn. Reson. 4(6), 331 (1995)CrossRefGoogle Scholar
  55. 55.
    E. Scarpellini, M. Ortolani, A. Nucara, L. Baldassarre, M. Missori, R. Fastampa, and R. Caminiti, Stabilization of the tensile strength of aged cellulose paper by Cholinium-Amino acid ionic liquid treatment, J. Phys. Chem. C 120(42), 24088 (2016)CrossRefGoogle Scholar

Copyright information

© Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Domenico Mallamace
    • 1
  • Sebastiano Vasi
    • 2
  • Mauro Missori
    • 3
  • Francesco Mallamace
    • 2
    • 4
    • 5
  • Carmelo Corsaro
    • 2
    • 4
  1. 1.Consorzio interuniversitario per lo sviluppo dei Sistemi a Grande Interfase - CSGISesto Fiorentino, FirenzeItaly
  2. 2.Dipartimento MIFT, Sezione di FisicaUniversità di MessinaMessinaItaly
  3. 3.Istituto dei Sistemi ComplessiConsiglio Nazionale delle RicercheRomaItaly
  4. 4.CNR-IPCF Messina, Istituto per i Processi Chimico-FisiciMessinaItaly
  5. 5.Center for Polymer Studies and Department of PhysicsBoston UniversityBostonUSA

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