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      Collagen intrafibrillar mineralisation as a result of the balance between osmotic equilibrium and electroneutrality

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          Abstract

          Mineralisation of fibrillar collagen with biomimetic process-directing agents has enabled scientists to gain insight into the potential mechanisms involved in intrafibrillar mineralisation. Here, by using polycation- and polyanion-directed intrafibrillar mineralisation, we challenge the popular paradigm that electrostatic attraction is solely responsible for polyelectrolyte-directed intrafibrillar mineralisation. Because there is no difference when a polycationic or a polyanionic electrolyte is used to direct collagen mineralisation, we argue that additional types of long-range non-electrostatic interactions are responsible for intrafibrillar mineralisation. Molecular dynamics simulations of collagen structures in the presence of extrafibrillar polyelectrolytes show that the outward movement of ions and intrafibrillar water through the collagen surface occurs irrespective of the charges of polyelectrolytes, resulting in the experimentally verifiable contraction of the collagen structures. The need to balance electroneutrality and osmotic equilibrium simultaneously to establish Gibbs-Donnan equilibrium in a polyelectrolyte-directed mineralisation system establishes a new model for collagen intrafibrillar mineralisation that supplements existing collagen mineralisation mechanisms.

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          Most cited references 44

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                Author and article information

                Journal
                101155473
                30248
                Nat Mater
                Nat Mater
                Nature materials
                1476-1122
                1 October 2016
                07 November 2016
                March 2017
                07 May 2017
                : 16
                : 3
                : 370-378
                Affiliations
                [1 ]State Key Laboratory of Military Stomatology & National Clinical Research Center for Oral Diseases & Shaanxi Key Laboratory of Oral Diseases, Department of Prosthodontics, School of Stomatology, The Fourth Military Medical University, Xi’an, China
                [2 ]School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia, USA
                [3 ]Department of Biological Structure, University of Washington, Seattle, Washington, USA
                [4 ]Frontier Institute of Science and Technology, State Key Laboratory for Mechanical behavior of Materials, Xi’an Jiaotong University, Xi’an, China
                [5 ]Department of Biomedical and Neuromotor Sciences, DIBINEM, University of Bologna, Bologna, Italy
                [6 ]The Dental College of Georgia, Augusta University, Augusta, Georgia, USA
                Author notes
                Co-corresponding authors: Franklin R. Tay, The Dental College of Georgia, Augusta University, Augusta, Georgia, 30912-1129, USA. TEL: (706) 7212031, ftay@ 123456augusta.edu ; Ji-hua Chen, School of Stomatology, The Fourth Military Medical University, Xi’an, China, jhchen@ 123456fmmu.edu.cn ; Seung Soon Jang, School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia, USA, seungsoon.jang@ 123456mse.gatech.edu

                Correspondence and requests for materials should be addressed to F.R.T. at ftay@ 123456augusta.edu .

                [*]

                These authors contributed equally to this work

                Article
                NIHMS819975
                10.1038/nmat4789
                5321866
                27820813

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                Materials science

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