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Properties of water confined in hydroxyapatite nanopores as derived from molecular dynamics simulations

Abstract

Bone tissue is characterized by nanopores inside the collagen-apatite matrix where fluid can exist and flow. The description of the fluid flow within the bone has however mostly relied on a macroscopic continuum mechanical treatment of the system, and, for this reason, the role of these nanopores has been largely overlooked. However, neglecting the nanoscopic behaviour of fluid within the bone volume could result in large errors in the overall description of the dynamics of fluid. In this work, we have investigated the nanoscopic origin of fluid motion by conducting atomistic molecular dynamics simulations of water confined between two parallel surfaces of hydroxyapatite (HAP), which is the main mineral phase of mammalian bone. The polarizable core–shell interatomic potential model used in this work to simulate the HAP–water system has been extensively assessed with respect to ab initio calculations and experimental data. The structural (pair distribution functions), dynamical (self-diffusion coefficients) and transport (shear viscosity coefficients) properties of confined water have been computed as a function of the size of the nanopore and the temperature of the system. Analysis of the results shows that the dynamical and transport properties of water are significantly affected by the confinement, which is explained in terms of the layering of water on the surface of HAP as a consequence of the molecular interactions between the water molecules and the calcium and phosphate ions at the surface. Using molecular dynamics simulations, we have also computed the slip length of water on the surface of HAP, the value of which has never been reported before.

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References

  1. Narasaraju TSB, Phebe DE (1996) J Mater Sci 31(1):1

    Article  CAS  Google Scholar 

  2. Fratzl P, Gupta HS, Paschalis EP, Roschger P (2004) J Mater Chem 14(14):2115

    Article  CAS  Google Scholar 

  3. Kenny SM, Buggy M (2003) J Mater Sci Mater Med 14(11):923

    Article  CAS  Google Scholar 

  4. Oddou C, Lemaire T, Pierre J, David B (2011) In: Vafai K (ed) Porous media: applications in biological systems and biotechnology. CRC Press, Boca Raton, pp 75–119

  5. Robinson RA, Elliott SR (1957) J Bone Joint Surg 39(1):167

    Google Scholar 

  6. Timmins PA, Wall JC (1977) Calcif Tissue Res 23(1):1. doi:10.1007/BF02012759

    Article  CAS  Google Scholar 

  7. Tate MLK (2003) J Biomech 36(10):1409

    Article  Google Scholar 

  8. Cowin SC, Gailani G, Benalla M (2009) Philos Trans R Soc A 367:3401

    Article  Google Scholar 

  9. Rohan E, Naili S, Cimrman R, Lemaire T (2012) J Mech Phys Solids 60(5):857

    Article  Google Scholar 

  10. Lemaire T, Capiez-Lernout E, Kaiser J, Naili S, Rohan E, Sansalone V (2011) Bull Math Biol 73:2649

    Article  CAS  Google Scholar 

  11. Rohan E, Naili S, Cimrman R, Lemaire T (2012) Comptes Rendus Mecanique 340(10):688

    Article  Google Scholar 

  12. Norrish K (1954) Disc Faraday Soc 18:120

    Article  CAS  Google Scholar 

  13. Karniadakis G, Beskok A, Aluru NR (2006) Microflows and nanoflows: fundamentals and simulation, vol 29. Springer, Berlin

    Google Scholar 

  14. Stephen W, Wolfie T (1986) FEBS Lett 206(2):262. doi:10.1016/0014-5793(86)80993-0. http://www.sciencedirect.com/science/article/pii/0014579386809930

  15. Sudarsanan K, Young RA (1969) Acta Crystallogr Sect B 25(8):1534. doi:10.1107/S0567740869004298

    Article  CAS  Google Scholar 

  16. de Leeuw NH, Parker SC (1998) Phys Rev B 58:13901. doi:10.1103/PhysRevB.58.13901

    Article  Google Scholar 

  17. de Leeuw NH (2004) Phys Chem Chem Phys 6:1860. doi:10.1039/B313242K

    Article  Google Scholar 

  18. Dick BG, Overhauser AW (1958) Phys Rev 112:90. doi:10.1103/PhysRev.112.90

    Article  CAS  Google Scholar 

  19. Errington JR, Debenedetti PG (2001) Nature 409:318

    Article  CAS  Google Scholar 

  20. Essmann U, Perera L, Berkowitz ML, Darden T, Lee H, Pedersen LG (1995) J Chem Phys 103(19):8577. doi:10.1063/1.470117. http://scitation.aip.org/content/aip/journal/jcp/103/19/10.1063/1.470117

  21. Todorov IT, Smithand W, Trachenko K, Dove MT (2006) J Mater Chem 16:1911. doi:10.1039/B517931A

    Article  CAS  Google Scholar 

  22. Nosé S (1984) J Chem Phys 81(1):511. doi:10.1063/1.447334. http://scitation.aip.org/content/aip/journal/jcp/81/1/10.1063/1.447334

  23. Wolthers M, Di Tommaso D, Du Z, de Leeuw NH (2012) Phys Chem Chem Phys 14:15145. doi:10.1039/C2CP42290E

    Article  CAS  Google Scholar 

  24. Ruiz-Hernandez S, Grau-Crespo NR, Almora-Barrios R, Wolthers M, Ruiz-Salvador AR, Fernandez N, de Leeuw NH (2012) Chem Eur J 18:9828

    Article  CAS  Google Scholar 

  25. de Leeuw NH, Parker SC (2001) Phys Chem Chem Phys 3:3217

    Article  Google Scholar 

  26. Bako I, Hutter J, Palinkas G (2002) J Chem Phys 117(21):9838. doi:10.1063/1.1517039. http://scitation.aip.org/content/aip/journal/jcp/117/21/10.1063/1.1517039

  27. Odutola JA, Dyke TR (1980) J Chem Phys 72(9):5062. doi:10.1063/1.439795. http://scitation.aip.org/content/aip/journal/jcp/72/9/10.1063/1.439795

  28. Chandra A (2000) Phys Rev Lett 85:768. doi:10.1103/PhysRevLett.85.768. http://link.aps.org/doi/10.1103/PhysRevLett.85.768

  29. Wright K, Cygan RT, Slater B (2001) Phys Chem Chem Phys 3:839. doi:10.1039/B006130L

    Article  CAS  Google Scholar 

  30. Kerisit S, Parker SC, Harding JH (2003) J Phys Chem B 107(31):7676. doi:10.1021/jp034201b

    Article  CAS  Google Scholar 

  31. Kerisit S, Parker SC (2004) J Am Chem Soc 126(32):10152. doi:10.1021/ja0487776. http://dx.doi.org/10.1021/ja0487776

  32. Cooke DJ, Elliott JA (2007) J Chem Phys 127(10):104706. doi:10.1063/1.2756840. http://scitation.aip.org/content/aip/journal/jcp/127/10/10.1063/1.2756840

  33. Perry T IV, Cygan RT, Mitchell R (2007) Geochimica et Cosmochimica Acta 71(24):5876. doi:10.1016/j.gca.2007.08.030. http://www.sciencedirect.com/science/article/pii/S0016703707005182

  34. Raiteri P, Gale JD, Quigley D, Rodger PM (2010) J Phys Chem C 114(13):5997. doi:10.1021/jp910977a

    Article  CAS  Google Scholar 

  35. Gale JD, Raiteri P, van Duin ACT (2011) Phys Chem Chem Phys 13:16666. doi:10.1039/C1CP21034C

    Article  CAS  Google Scholar 

  36. Villegas-Jimenez A, Mucci A, Whitehead MA (2009) Langmuir 25(12):6813. doi:10.1021/la803652x

    Article  CAS  Google Scholar 

  37. Lardge JS, Duffy DM, Gillan MJ, Watkins M (2010) J Phys Chem C 114(6):2664. doi:10.1021/jp909593p

    Article  CAS  Google Scholar 

  38. Heberling F, Trainor TP, Lützenkirchen J, Eng P, Denecke MA, Bosbach D (2011) J Colloid Interface Sci 354(2):843. doi:10.1016/j.jcis.2010.10.047. http://www.sciencedirect.com/science/article/pii/S0021979710012336

  39. Hiemstra T, Venema P, Van Riemsdijk WH (1996) J Colloid Interface Sci 184(2):680. doi:10.1006/jcis.1996.0666. http://www.sciencedirect.com/science/article/pii/S0021979796906669

  40. Fenter P, Geissbühler P, Dimasi E, Srajer G, Sorensen LB, Sturchio NC (2000) Geochimica et Cosmochimica Acta 64(7):1221. doi:10.1016/S0016-7037(99)00403-2. http://www.sciencedirect.com/science/article/pii/S0016703799004032

  41. Bruneval F, Donadio D, Parrinello M (2007) J Phys Chem B 111(42):12219. doi:10.1021/jp0728306

    Article  CAS  Google Scholar 

  42. Freeman CL, Harding JH, Cooke DJ, Elliott JA, Lardge JS, Duffy DM (2007) J Phys Chem C 111(32):11943. doi:10.1021/jp071887p

    Article  CAS  Google Scholar 

  43. Beveridge DL, DiCapua FM (1989) Ann Rev Biophys Biophys Chem 18:431

    Article  CAS  Google Scholar 

  44. David F, Vokhmin V, Ionova G (2001) J Mol Liquids 90:45–62

    Article  CAS  Google Scholar 

  45. Hofer TS, Tran HT, Schwenk CF, Rode BM (2004) J Comput Chem 90:211–217

    Article  Google Scholar 

  46. Di Tommaso NH, de Leeuw D (2010) Crystal Growth Design 10:4292–4302

    Article  Google Scholar 

  47. Dang LX, Smith DE (1993) J Chem Phys 99:4229

    Article  Google Scholar 

  48. Berendsen HJC, Grigera JR, Straatsma TP (1987) J Phys Chem 91:6269

    Article  CAS  Google Scholar 

  49. Pan H, Tao J, Wu T, Tang R (2007) Front Chem China 2(2):156. doi:10.1007/s11458-007-0032-6

    Article  Google Scholar 

  50. Sit PHL, Marzari N (2005) J Chem Phys 122:204510

    Article  Google Scholar 

  51. Arismendi-Arrieta D, Medina JS, Fanourgakis GS, Prosmiti R, Delgado-Barrio G (2014) Appl Radiat Isotopes 83(Part B):115. doi:10.1016/j.apradiso.2013.01.020. http://www.sciencedirect.com/science/article/pii/S0969804313000213

  52. Medina JS, Prosmiti R, Villarreal P, Delgado-Barrio G, Winter G, Gonzalez B, Aleman JV, Collado C (2011) Chem Phys 388(1–3):9. doi:10.1016/j.chemphys.2011.07.001. http://www.sciencedirect.com/science/article/pii/S0301010411002813

  53. Soper AK, Phillips MG (1986) Chem Phys 107(1):47. doi:10.1016/0301-0104(86)85058-3. http://www.sciencedirect.com/science/article/pii/0301010486850583

  54. Di Tommaso D, de Leeuw NH (2008) J Phys Chem B 112(23):6965. doi:10.1021/jp801070b. http://pubs.acs.org/doi/abs/10.1021/jp801070b

  55. Tang E, Di Tommaso D, de Leeuw NH (2009) J Chem Phys 130(23):234502. doi:10.1063/1.3143952. http://scitation.aip.org/content/aip/journal/jcp/130/23/10.1063/1.3143952

  56. Einstein A (1956) Investigations on the theory of the Brownian movement. Dover, New York

    Google Scholar 

  57. Dünweg B, Kremer K (1993) J Chem Phys 99(9):6983. doi:10.1063/1.465445. http://scitation.aip.org/content/aip/journal/jcp/99/9/10.1063/1.465445

  58. Yeh IC, Hummer G (2004) J Phys Chem B 108(40):15873. doi:10.1021/jp0477147. http://pubs.acs.org/doi/abs/10.1021/jp0477147

  59. Todd BD, Evans DJ, Daivis PJ (1995) Phys Rev E 52:1627. doi:10.1103/PhysRevE.52.1627. http://link.aps.org/doi/10.1103/PhysRevE.52.1627

  60. Botan A, Rotenberg B, Marry V, Turq P, Noetinger B (2011) J Phys Chem C 115(32):16109. doi:10.1021/jp204772c. http://pubs.acs.org/doi/abs/10.1021/jp204772c

  61. Kestin J, Sokolov M, Wakeham WA (1978) J Phys Chem Ref Data 7(3):941. doi:10.1063/1.555581. http://scitation.aip.org/content/aip/journal/jpcrd/7/3/10.1063/1.555581

  62. Bird RB, Warren ES, Edwin NL (2007) Transport phenomena, revised, 2nd edn. Wiley, New York

    Google Scholar 

  63. Markesteijn AP, Hartkamp R, Luding S, Westerweel J (2012) J Chem Phys 136(13):134104. doi:10.1063/1.3697977. http://scitation.aip.org/content/aip/journal/jcp/136/13/10.1063/1.3697977

  64. Fanourgakis GS, Medina JS, R P (2012) J Phys Chem A 116:2564–2570

    Article  CAS  Google Scholar 

  65. Guevara-Carrion G, Vrabec J, Hasse H (2011) J Chem Phys 134(7):074508. doi:10.1063/1.3515262. http://scitation.aip.org/content/aip/journal/jcp/134/7/10.1063/1.3515262

  66. Gonzalez MA, Abascal JLF (2010) J Chem Phys 132(9):096101. doi:10.1063/1.3330544. http://scitation.aip.org/content/aip/journal/jcp/132/9/10.1063/1.3330544

  67. Fanourgakis GS, Medina JS, Prosmiti R (2012) J Phys Chem A 116(10):2564. doi:10.1021/jp211952y. http://pubs.acs.org/doi/abs/10.1021/jp211952y

  68. Wensink EJW, Hoffmann AC, van Maaren PJ, van der Spoel D (2003) J Chem Phys 119(14):7308. doi:10.1063/1.1607918. http://scitation.aip.org/content/aip/journal/jcp/119/14/10.1063/1.1607918

  69. Bertolini D, Tani A (1995) Phys Rev E 52:1699. doi:10.1103/PhysRevE.52.1699. http://link.aps.org/doi/10.1103/PhysRevE.52.1699

  70. Wu Y, Tepper HL, Voth GA (2006) J Chem Phys 124(2):024503. doi:10.1063/1.2136877. http://scitation.aip.org/content/aip/journal/jcp/124/2/10.1063/1.2136877

  71. Slusher JT (2000) Mol Phys 98(5):287. doi:10.1080/00268970009483292

    Article  CAS  Google Scholar 

  72. Jorgensen WL (1986) J Phys Chem 90(7):1276. doi:10.1021/j100398a015. http://pubs.acs.org/doi/abs/10.1021/j100398a015

  73. Glattli A, Daura X, van Gunsteren WF (2002) J Chem Phys 116(22):9811. doi:10.1063/1.1476316. http://scitation.aip.org/content/aip/journal/jcp/116/22/10.1063/1.1476316

  74. Hess B (2002) J Chem Phys 116(1):209. doi:10.1063/1.1421362. http://scitation.aip.org/content/aip/journal/jcp/116/1/10.1063/1.1421362

  75. Balasubramanian S, Mundy CJ, Klein ML (1996) J Chem Phys 105(24):11190. doi:10.1063/1.472918. http://scitation.aip.org/content/aip/journal/jcp/105/24/10.1063/1.472918

  76. Guo GJ, Zhang YG (2001) Mol Phys 99(4):283. doi:10.1080/00268970010011762

    Article  CAS  Google Scholar 

  77. Smith PE, van Gunsteren WF (1993) Chem Phys Lett 215(4):315. doi:10.1016/0009-2614(93)85720-9. http://www.sciencedirect.com/science/article/pii/0009261493857209

  78. Harris KR, Woolf LA (2004) J Chem Eng Data 49(4):1064. doi:10.1021/je049918m. http://pubs.acs.org/doi/abs/10.1021/je049918m

  79. Ellis JS, Thompson M (2004) Phys Chem Chem Phys 6:4928

    Article  CAS  Google Scholar 

  80. Bocquet L, Charlaix E (2010) Chem Soc Rev 39:1073

    Article  CAS  Google Scholar 

  81. Sendner C, Horinek D, Bocquet L, Netz RR (2009) Langmuir 25(18):10768

    Article  CAS  Google Scholar 

  82. Joschek S, Nies B, Krotz R, Gopferich A (2000) Biomaterials 21(16):1645

    Article  CAS  Google Scholar 

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Acknowledgments

N.H. de Leeuw is grateful to ‘Université Paris-Est Créteil’ (UPEC) for financial support received during the course of this research. T.T. Pham is grateful to the ‘Institut des sciences de l’ingénierie et des systèmes’ (INSIS) of the ‘Centre national de la recherche scientifique’ (CNRS) for financial support received during the course of this research. D. Di Tommaso would like to thank the Royal Society, UK, for the award of a Royal Society Industry Fellowship.

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The authors declare that they have no conflict of interest.

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Pham, T.T., Lemaire, T., Capiez-Lernout, E. et al. Properties of water confined in hydroxyapatite nanopores as derived from molecular dynamics simulations. Theor Chem Acc 134, 59 (2015). https://doi.org/10.1007/s00214-015-1653-3

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Keywords

  • Water properties
  • Nanopores
  • Hydroxyapatite
  • Bone fluid flow