Abstract
Fast field cycling (FFC) NMR relaxometry has been used to study the conformational properties of aqueous solutions of hyaluronan (HYA) at three concentrations in the range 10 to 25 mg mL–1. Results revealed that, irrespective of the solution concentration, three different hydration layers surround hyaluronan. The inner layer consists of water molecules strongly retained in the proximity of the HYA surface. Because of their strong interactions with HYA, water molecules in this inner hydration layer are subject to very slow dynamics and have the largest correlation times. The other two hydration layers are made of water molecules which are located progressively further from the HYA surface. As a result, decreasing correlation times caused by faster molecular motion were measured. The NMRD profiles obtained by FFC-NMR relaxometry also showed peaks attributable to 1H–14N quadrupole interactions. Changes in intensity and position of the quadrupolar peaks in the NMRD profiles suggested that with increasing concentration the amido group is progressively involved in the formation of weak and transient intramolecular water bridging adjacent hyaluronan chains. In this work, FFC-NMR was used for the first time to obtain deeper insight into HYA–water interactions and proved itself a powerful and promising tool in hyaluronan chemistry.
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References
Garg HG, Hales CA (2004) Chemistry and biology of hyaluronan. Elsevier Ltd, Oxford
De Angelis PL (2002) Glycobiology 12:9R–16R
McDonald JA, Camenisch TD (2003) Glycoconjugate J 19:331–339
Kogan G, Šoltéz L, Stern R, Gemener P (2007) Biotechnol Lett 29:17–25
Rinaudo M (2008) Polym Int 57:397–430
Leach JB, Schmidt CE (2004) In: Encyclopedia of Biomaterials and Biomedical Engineering, 1st edn. Marcel Dekker, pp 779–789
Taglienti A, Sequi P, Valentini M (2009) Carbohydr Res 344:245–249
Cowman MK, Matsuoka S (2005) Carbohydr Res 340:791–809
Blundell CD, Reed MAC, Almond A (2006) Carbohydr Res 341:2803–2815
Almond A (2007) Cell Mol Life Sci 64:1591–1596
Giannotti MI, Rinaudo M, Vancso GJ (2007) Biomacromolecules 8:2648–2652
Deschrevel B, Tranchepain F, Vincent J-C (2008) Matrix Biol 27:475–485
Hargittai I, Hargittai M (2008) J Struct Chem 19:697–717
Tømmeraas K, Melander C (2008) Biomacromolecules 9:1535–1540
Matteini P, Dei L, Carretti E, Volpi N, Goti A, Pini R (2009) Biomacromolecules 10:1516–1522
Blundell CD, Reed MAC, Almond A (2006) Carbohydr Res 341:2803–2815
Giannotti MI, Rinaudo M, Vancso GJ (2007) Biomacromolecules 8:2648–2652
Haxaire K, Maréchal Y, Milas M, Rinaudo M (2003) Biopolymers 72:10–20
Haxaire K, Maréchal Y, Milas M, Rinaudo M (2003) Biopolymers 72:149–161
Maréchal Y, Milas M, Rinaudo M (2003) Biopolymers 72:162–173
Hatakeyama T, Hatakeyama H (1998) Thermochim Acta 308:3–22
Lui J, Cowman MK (2000) J Therm Anal Calorim 59:547–557
Pogány P, Kovács A (2009) Carbohydr Res 344:1745–1752
Rinaudo M (2006) Macromol Symp 245–246:549–557
Conte P, Bubici S, Palazzolo E, Alonzo G (2009) Spectrosc Lett 42:235–239
Bertram HC, Wiking L, Nielsen JH, Andersen HJ (2005) Int Dairy J 15:1056–1063
Davenel A, Schuck P, Mariette F, Brulé G (2002) Lait 82:465–473
Gianferri R, Maioli M, Delfini M, Brusio E (2007) Int Dairy J 17:167–176
Hernández-Sánchez N, Hills BP, Barreiro P, Marigheto N (2007) Postharvest Biol Technol 44:260–270
Tang HR, Zhao BL, Belton PS, Sutcliffe LH, Ng A (2000) Magn Reson Chem 38:765–770
Prestes RA, Colnago LA, Forato LA, Vizzotto L, Novotny EH, Carrilho E (2007) Anal Chim Acta 596:325–329
Casieri C, Bubici S, Viola I, De Luca F (2004) Solid State Nucl Magn Reson 26:65–73
Kausik R, Fatkullin N, Hüsing N, Kimmich R (2007) Magn Reson Imaging 25:489–497
Melton JR, Kantzas A, Langford CH (2007) Anal Chim Acta 605:46–52
Halle B, Johannesson H, Venu K (1998) J Magn Reson 135:1–13
Wang YL, Belton PS (2000) Chem Phys Lett 325:33–38
Kimmich R, Anoardo E (2004) Prog Nucl Magn Reson Spectrosc 44:257–320
Ferrante G, Sykora S (2005) Adv Inorg Chem 57:405–470
Laghi L, Cremonini MA, Placucci G, Sykora S, Wright K, Hills B (2005) Magn Reson Imaging 23:01–510
Dobies M, Kuśmia S, Jurga S (2005) Acta Phys Pol A 108:33–46
Takahashi M, Hatakeyama T, Hatakeyama H (2000) Carbohydr Polym 41:91–95
Lauffer RB (1987) Chem Rev 87:901–927
Bakhmutov VI (2005) Pratical NMR relaxation for chemists. John Wiley & Sons Ltd, Chichester
Bertini I, Luchinat C (1986) In: Gray ABP, Deries HB (eds) NMR of paramagnetic molecules in biological systems. The Benjamin/Cummings Publishing Company Inc, California
Fouissac E, Milas M, Rinaudo M (1993) Macromol 26:6945–6951
Almond A, Sheehan JK, Brass A (1997) Glycobiology 7:597–604
Almond A (2007) Cell Mol Life Sci 64:1591–1596
Wolfe J, Bryant G, Koster KL (2002) CryLetters 23:157–166
Hardingham T (2004) In: Garg HG, Hales CA (eds) Chemistry and biology of hyaluronan. Elsevier Ltd, Oxford
Acknowledgments
This work was partially funded by Ce.R.T.A. s.c.r.l. (Centri Regionali per le Tecnologie Alimentari; http://www.certa.it/default.asp) and by the Ministry of Education, Youth and Sport of the Czech Republic, project no. 0021630501. A.P. acknowledges an Erasmus project which enabled her to work at the Università degli Studi di Palermo. The authors kindly acknowledge Dr. Vladimír Velebný (CPN company, Dolní Dobrouč, Czech Republic) for providing the hyaluronan sample.
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Průšová, A., Conte, P., Kučerík, J. et al. Dynamics of hyaluronan aqueous solutions as assessed by fast field cycling NMR relaxometry. Anal Bioanal Chem 397, 3023–3028 (2010). https://doi.org/10.1007/s00216-010-3855-9
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DOI: https://doi.org/10.1007/s00216-010-3855-9