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Title: In Situ Evaluation of Calcium Phosphate Nucleation Kinetics and Pathways during Intra- and Extrafibrillar Mineralization of Collagen Matrices

Abstract

Calcium phosphate (CaP) nanocrystals nucleate and grow in intrafibrillar and/or extrafibrillar spaces of collagen fibrils during the mineralization of bones and teeth. Little is known about the early stages of CaP nucleation and distribution in fibrillar matrices, despite their significant influence on the physical and chemical structures of tissue-level constructs. Using in situ small angle X-ray scattering (SAXS), we examined the nucleation and growth of CaP within collagen matrices and elucidated how a nucleation inhibitor, polyaspartic acid (pAsp), governs mineralization kinetics and pathways at multiple length scales. In situ SAXS analysis clearly revealed that nucleation sites, kinetically-controlled by the nucleation inhibitor, determined the pathways of CaP morphological transformation. Mineralization with pAsp led to intrafibrillar CaP plates with a spatial distribution gradient through the depth of the matrix. Mineralization without pAsp led initially to spherical aggregates of CaP in the entire extrafibrillar spaces. With time, the spherical aggregates transformed into plates at the outermost surface of the collagen matrix, preventing intrafibrillar mineralization inside. The results illuminate mineral nucleation kinetics and real-time nanoparticle distributions within organic matrices in solutions containing body fluid components. Because the macroscale mechanical properties of collagen matrices depend on their mineral content, phase, and arrangement at the nanoscale,more » this study contributes to better design and fabrication of biomaterials for regenerative medicine.« less

Authors:
 [1];  [2];  [3];  [1]
  1. Department of Energy, Environmental &, Chemical Engineering, Washington University, St. Louis, Missouri 63130, United States
  2. X-ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
  3. Department of Orthopedic Surgery, Columbia University, New York, New York 10032-3072, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Institutes of Health (NIH)
OSTI Identifier:
1429899
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Crystal Growth and Design; Journal Volume: 16; Journal Issue: 9
Country of Publication:
United States
Language:
English

Citation Formats

Kim, Doyoon, Lee, Byeongdu, Thomopoulos, Stavros, and Jun, Young-Shin. In Situ Evaluation of Calcium Phosphate Nucleation Kinetics and Pathways during Intra- and Extrafibrillar Mineralization of Collagen Matrices. United States: N. p., 2016. Web. doi:10.1021/acs.cgd.6b00864.
Kim, Doyoon, Lee, Byeongdu, Thomopoulos, Stavros, & Jun, Young-Shin. In Situ Evaluation of Calcium Phosphate Nucleation Kinetics and Pathways during Intra- and Extrafibrillar Mineralization of Collagen Matrices. United States. doi:10.1021/acs.cgd.6b00864.
Kim, Doyoon, Lee, Byeongdu, Thomopoulos, Stavros, and Jun, Young-Shin. Thu . "In Situ Evaluation of Calcium Phosphate Nucleation Kinetics and Pathways during Intra- and Extrafibrillar Mineralization of Collagen Matrices". United States. doi:10.1021/acs.cgd.6b00864.
@article{osti_1429899,
title = {In Situ Evaluation of Calcium Phosphate Nucleation Kinetics and Pathways during Intra- and Extrafibrillar Mineralization of Collagen Matrices},
author = {Kim, Doyoon and Lee, Byeongdu and Thomopoulos, Stavros and Jun, Young-Shin},
abstractNote = {Calcium phosphate (CaP) nanocrystals nucleate and grow in intrafibrillar and/or extrafibrillar spaces of collagen fibrils during the mineralization of bones and teeth. Little is known about the early stages of CaP nucleation and distribution in fibrillar matrices, despite their significant influence on the physical and chemical structures of tissue-level constructs. Using in situ small angle X-ray scattering (SAXS), we examined the nucleation and growth of CaP within collagen matrices and elucidated how a nucleation inhibitor, polyaspartic acid (pAsp), governs mineralization kinetics and pathways at multiple length scales. In situ SAXS analysis clearly revealed that nucleation sites, kinetically-controlled by the nucleation inhibitor, determined the pathways of CaP morphological transformation. Mineralization with pAsp led to intrafibrillar CaP plates with a spatial distribution gradient through the depth of the matrix. Mineralization without pAsp led initially to spherical aggregates of CaP in the entire extrafibrillar spaces. With time, the spherical aggregates transformed into plates at the outermost surface of the collagen matrix, preventing intrafibrillar mineralization inside. The results illuminate mineral nucleation kinetics and real-time nanoparticle distributions within organic matrices in solutions containing body fluid components. Because the macroscale mechanical properties of collagen matrices depend on their mineral content, phase, and arrangement at the nanoscale, this study contributes to better design and fabrication of biomaterials for regenerative medicine.},
doi = {10.1021/acs.cgd.6b00864},
journal = {Crystal Growth and Design},
number = 9,
volume = 16,
place = {United States},
year = {Thu Aug 04 00:00:00 EDT 2016},
month = {Thu Aug 04 00:00:00 EDT 2016}
}