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

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

References

[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. USA113(12), 3159 (2016)

[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)

[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)

[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)

[5] D.Klemm, B.Philipp, T.Heinze , U.Heinze, and W.Wagenknecht, Volume I: Fundamentals and Analytical Methods, Weinheim: WILEY-VCH Verlag GmbH, 1998

[6] A. C.O’Sullivan , The structure slowly unravels, Cellulose4(3), 173(1997)

[7] X.Qiuand S.Hu, “Smart” materials based on cellulose: A review of the preparations, properties, and applications, Materials (Basel)6(3), 738(2013)

[8] J.Kim, Cellulose as a smart material, in: R. Malcolm Brown Jr. and Inder M. Saxena (Eds.), Cellulose: Molecular and Structural Biology, Springer Netherlands, 323–343 (2007)

[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)

[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. E77(4), 041801(2008)

[11] K. L.Katoand R. E. Cameron, A review of the relationship between thermally-accelerated ageing of paper and hornification, Cellulose6(1), 23(1999)

[12] G.Banikand I.Brückle, Structure and properties of dry and wet paper, in: Paper and Water: A Guide for Conservators, Amsterdam: Elsevier, 81–105(2011)

[13] L.Teodonio, M.Missori, D.Pawcenis , J.Lojewska, and F.Valle, Nanoscale analysis of degradation processes of cellulose fibers, Micron91, 75(2016)

[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)

[15] D.Hunter, Papermaking: The History and Technique of an Ancient Craft, New York: Dover Publications, 1978

[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)

[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, Macromolecules35(14), 5536(2002)

[18] C.Federici, P.Mufanò, and M. S.Storace , Ancient paper and its NMR characterization, Sci. Technol. Cult. Herit. 5, 37(1996)

[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)

[20] J.Kolar, Mechanism of autoxidative degradation of cellulose, Restaurator (Copenh.)18(4), 163(1997)

[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)

[22] T.jewski, P.Miskowiec, M.Missori , A.Lubanska, L. M.Proniewicz, andJ.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)

[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)

[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. A100(3), 873(2010)

[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, Biomacromolecules9(9), 2546(2008)

[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, Talanta89, 301(2012)

[27] S.Belton, NMR studies of hydration in low water content biopolymer systems, Magn. Reson. Chem. 49, S127(2011)

[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 B252(1), 112(2015)

[29] M.Missori, Optical spectroscopy of ancient paper and textiles, Nuovo Cimento C39, 293(2016)

[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. B89(5), 054201(2014)

[31] A.Mosca Conte, O.Pulci, M. C.Misiti , J.Lojewska, L.Teodonio, C.Violante , andM.Missori,Visual degradation in Leonardo da Vinci’s iconic self-portrait: A nanoscale study,Appl. Phys. Lett.104(22), 224101(2014)

[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, Cellulose18(6), 1623(2011)

[33] A.Abragam, The Principles of Nuclear Magnetism, London: Oxford University Press, 1961

[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)

[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)

[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)

[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)

[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)

[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)

[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 C39, 309(2016)

[41] J. H.Chenand 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)

[42] J. C.Lindon, E.Holmes, and J. K.Nicholson , Metabolonomics in pharmacheutical R&D, FEBS J. 274(5), 1140(2007)

[43] E. R.Andrew, A.Bradbury, and R. G.Eades , Removal of bipolar broadening of nuclear magnetic resonance spectra of solids by specimen rotation, Nature183(4678), 1802(1959)

[44] B.Blicharskaand M.Kluza, NMR relaxation in cellulose pulp, Colloids Surf. A Physicochem. Eng. Asp. 115, 137(1996)

[45] D.Topgaardand O.Söderman, Changes of cellulose fiber wall structure during drying investigated using NMR self-diffusion and relaxation experiments, Cellulose9(2), 139(2002)

[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)

[47] K.Modig, B. G.Pfrommer, and B.Halle , Temperaturedependent hydrogen-bond geometry in liquid water, Phys. Rev. Lett.90(7), 075502(2003)

[48] D.Sebastianiand M.Parrinello, Ab-initio study of NMR chemical shifts of water under normal and supercritical conditions, ChemPhysChem3(8), 675(2002)

[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. USA105(35), 12725(2008)

[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. B112(34), 10449(2008)

[51] M. F.Froixand R.Nelson, The interaction of water with cellulose from nuclear magnetic resonance relaxation times, Macromolecules8(6), 726(1975)

[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. B112(13), 3927(2008)

[53] M.Paci, C.Federici, D.Capitani , N.Perenze, and A. L. Segre, NMR study of paper, Carbohydr. Polym. 26(4), 289(1995)

[54] S.Hayashiand E.Akiba, Nuclear spin-lattice relaxation mechanisms in kaolinite confirmed by magic-angle spinning, Solid State Nucl. Magn. Reson. 4(6), 331(1995)

[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. C120(42), 24088(2016)

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