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Title: Structural and dynamical studies of acid-mediated conversion in amorphous-calcium-phosphate based dental composites

Our objective was to investigate the complex structural and dynamical conversion process of the amorphous-calcium-phosphate (ACP)-to-apatite transition in ACP based dental composite materials. Composite disks were prepared using zirconia hybridized ACP fillers (0.4 mass fraction) and photo-activated Bis-GMA/TEGDMA resin (0.6 mass fraction). We performed an investigation of the solution-mediated ACP-to-apatite conversion mechanism in controlled acidic aqueous environment with in situ ultra-small angle X-ray scattering based coherent X-ray photon correlation spectroscopy and ex situ X-ray diffraction, as well as other complementary techniques. We established that the ACP-to-apatite conversion in ACP composites is a two-step process, owing to the sensitivity to local structural changes provided by coherent X-rays. Initially, ACP undergoes a local microstructural rearrangement without losing its amorphous character. We established the catalytic role of the acid and found the time scale of this rearrangement strongly depends on the pH of the solution, which agrees with previous findings about ACP without the polymer matrix being present. In the second step, ACP is converted to an apatitic form with the crystallinity of the formed crystallites being poor. Separately, we also confirmed that in the regular Zr-modified ACP the rate of ACP conversion to hydroxyapatite is slowed significantly compared to unmodified ACP, whichmore » is beneficial for targeted slow release of functional calcium and phosphate ions from dental composite materials. Significantly, for the first time, we were able to follow the complete solution-mediated transition process from ACP to apatite in this class of dental composites in a controlled aqueous environment. A two-step process, suggested previously, was conclusively identified.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [2] ;  [2] ;  [3]
  1. National Institute of Standards and Technology, Gaithersburg, MD (United States)
  2. American Dental Assoc. Foundation, Gaithersburg, MD (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
OSTI Identifier:
1263633
Grant/Contract Number:
AC02-06CH11357; NSF/CHE-1346572; DE 13169
Type:
Accepted Manuscript
Journal Name:
Dental Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 10; Journal ID: ISSN 0109-5641
Publisher:
Elsevier
Research Org:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE ACP-based composites; acid-medicated conversion; amorphous calcium phosphate; amorphous conversion; dental composites; dental material; structure