Bioprocess-Inspired Room-Temperature Synthesis of Enamel-like Fluorapatite/Polymer Nanocomposites Controlled by Magnesium Ions.

Tooth enamel is composed of arrayed fluorapatite (FAP) or hydroxyapatite nanorods modified with Mg-rich amorphous layers. Although it is known that Mg2+ plays an important role in the formation of enamel, there is limited research on the regulatory role of Mg2+ in the synthesis of enamel-like materials. Therefore, we focus on the regulatory behavior of Mg2+ in the fabrication of biomimetic mineralized enamel-like structural materials. In the present study, we adopt a bioprocess-inspired room-temperature mineralization technique to synthesize a multilayered array of enamel-like columnar FAP/polymer nanocomposites controlled by Mg2+ (FPN-M). The results reveal that the presence of Mg2+ induced the compaction of the array and the formation of a unique Mg-rich amorphous-reinforced architecture. Therefore, the FPN-M array exhibits excellent mechanical properties. The hardness (2.42 ± 0.01 GPa) and Young's modulus (81.5 ± 0.6 GPa) of the as-prepared FPN-M array are comparable to those of its biological counterparts; furthermore, the enamel-like FPN-M array is translucent. The hardness and Young's modulus of the synthetic array of FAP/polymer nanocomposites without Mg2+ control (FPN) are 0.51 ± 0.04 and 43.5 ± 1.6 GPa, respectively. The present study demonstrates a reliable bioprocess-inspired room-temperature fabrication technique for the development of advanced high-performance composite materials.

[1]  Prasanna V. Balachandran,et al.  Chemical Gradients in Human Enamel Crystallites. , 2020, Nature.

[2]  Lidong Li,et al.  Amorphous Alumina Nanosheets/Polylactic Acid Artificial Nacre , 2019, Matter.

[3]  Liwen Lei,et al.  Bioprocess‐Inspired Microscale Additive Manufacturing of Multilayered TiO2/Polymer Composites with Enamel‐Like Structures and High Mechanical Properties , 2019, Advanced Functional Materials.

[4]  Xurong Xu,et al.  Crosslinking ionic oligomers as conformable precursors to calcium carbonate , 2019, Nature.

[5]  H. Pan,et al.  Repair of tooth enamel by a biomimetic mineralization frontier ensuring epitaxial growth , 2019, Science Advances.

[6]  Jingjing Xie,et al.  Bioprocess-inspired fabrication of materials with new structures and functions , 2019, Progress in Materials Science.

[7]  Dimitri D. Deheyn,et al.  On the Nature of the Transparent Teeth of the Deep-Sea Dragonfish, Aristostomias scintillans , 2019, Matter.

[8]  P. Baglioni,et al.  Effect of pH and Mg2+ on Amorphous Magnesium-Calcium Phosphate (AMCP) stability. , 2018, Journal of colloid and interface science.

[9]  A. Mata,et al.  Protein disorder–order interplay to guide the growth of hierarchical mineralized structures , 2018, Nature Communications.

[10]  H. Pan,et al.  Total morphosynthesis of biomimetic prismatic-type CaCO3 thin films , 2017, Nature Communications.

[11]  C. X. Resende,et al.  Effect of Mg 2+ on acidic calcium phosphate phases grown by electrodeposition , 2017 .

[12]  H. Christenson,et al.  The Effect of Additives on the Early Stages of Growth of Calcite Single Crystals , 2017, Angewandte Chemie.

[13]  K. Onuma,et al.  Artificial enamel induced by phase transformation of amorphous nanoparticles , 2017, Scientific Reports.

[14]  A. Waas,et al.  Abiotic tooth enamel , 2017, Nature.

[15]  Bram Cantaert,et al.  Use of Amorphous Calcium Carbonate for the Design of New Materials. , 2017, ChemPlusChem.

[16]  Lei Liu,et al.  Synthetic nacre by predesigned matrix-directed mineralization , 2016, Science.

[17]  Shuhong Yu,et al.  Anisotropic nanowire growth via a self-confined amorphous template process: A reconsideration on the role of amorphous calcium carbonate , 2016, Nano Research.

[18]  J. Cairney,et al.  Atomic-scale compositional mapping reveals Mg-rich amorphous calcium phosphate in human dental enamel , 2016, Science Advances.

[19]  S. Coppersmith,et al.  Nanoscale Transforming Mineral Phases in Fresh Nacre. , 2015, Journal of the American Chemical Society.

[20]  J. Banfield,et al.  Crystallization by particle attachment in synthetic, biogenic, and geologic environments , 2015, Science.

[21]  K. Macrenaris,et al.  Amorphous intergranular phases control the properties of rodent tooth enamel , 2015, Science.

[22]  Y. Ikuhara,et al.  Fluorine in shark teeth: its direct atomic-resolution imaging and strengthening function. , 2014, Angewandte Chemie.

[23]  Dwayne Arola,et al.  Nanoscopic dynamic mechanical properties of intertubular and peritubular dentin. , 2012, Journal of the mechanical behavior of biomedical materials.

[24]  Doris Vollmer,et al.  Candle Soot as a Template for a Transparent Robust Superamphiphobic Coating , 2012, Science.

[25]  Peter Fratzl,et al.  Enamel-like apatite crown covering amorphous mineral in a crayfish mandible , 2012, Nature Communications.

[26]  Poonam Sharma,et al.  FTIR, powder XRD, TEM and dielectric studies of pure and zinc doped nano‐hydroxyapatite , 2011 .

[27]  Derk Joester,et al.  Nanoscale chemical tomography of buried organic–inorganic interfaces in the chiton tooth , 2011, Nature.

[28]  Xurong Xu,et al.  Magnesium-aspartate-based crystallization switch inspired from shell molt of crustacean , 2009, Proceedings of the National Academy of Sciences.

[29]  Xurong Xu,et al.  Controls of Tricalcium Phosphate Single-Crystal Formation from Its Amorphous Precursor by Interfacial Energy , 2009 .

[30]  Y. Oaki,et al.  Nanosegregated Amorphous Composites of Calcium Carbonate and an Organic Polymer , 2008 .

[31]  S. Weiner,et al.  Amorphous calcium phosphate is a major component of the forming fin bones of zebrafish: Indications for an amorphous precursor phase , 2008, Proceedings of the National Academy of Sciences.

[32]  M. Antonietti,et al.  Amorphous layer around aragonite platelets in nacre. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[33]  Markus Antonietti,et al.  Mesocrystals: inorganic superstructures made by highly parallel crystallization and controlled alignment. , 2005, Angewandte Chemie.

[34]  R. Lakes,et al.  Deformation of extreme viscoelastic metals and composites , 2004 .

[35]  Stephen Mann,et al.  Higher-order organization by mesoscale self-assembly and transformation of hybrid nanostructures. , 2003, Angewandte Chemie.

[36]  J. García‐Ruiz,et al.  Model of textural development of layered crystal aggregates , 2000 .

[37]  R.Z. Legfros,et al.  Magnesium and Carbonate in Enamel and Synthetic Apatites , 1996, Advances in dental research.

[38]  M. Swain,et al.  Understanding the mechanical behaviour of human enamel from its structural and compositional characteristics. , 2008, Journal of the mechanical behavior of biomedical materials.

[39]  L. Estroff.  Introduction: Biomineralization. , 2008, Chemical reviews.