We have recently reported the repair of carious enamel using a full-length amelogeninchitosan hydrogel through guided stabilization and growth of mineral clusters. The objective of this study was to further evaluate the enamel repair potential of smaller amelogenin peptides like LRAP (leucine-rich amelogenin peptide) and compare their efficiency with their full-length counterpart. The demineralized tooth slices treated with a single application of LRAP-chitosan hydrogel for 3 days showed a dense mineralized layer consisting of highly organized enamel-like apatite crystals. Focus-ion beam technique showed a seamless growth at the interface between the repaired layer and native enamel. There was a marked improvement in the surface hardness after treatment of the demineralized sample with almost 87% recovery of the hardness value to that of sound enamel sections. This current approach can inspire the design of smaller peptide analogues based on naturally occurring amelogenin as a competent, low-cost, and safe strategy for enamel biomimetics to curb the high prevalence of incipient dental caries.
Amelogenin-chitosan (CS-AMEL) hydrogel has shown great potential for the prevention, restoration, and treatment of defective enamel. As a step prior to clinical trials, this study aimed to examine the efficacy of CS-AMEL hydrogel in biomimetic repair of human enamel with erosive or caries-like lesions in pH-cycling systems. Two models for enamel defects, erosion and early caries, were addressed in this study. Two pH-cycling systems were designed to simulate the daily cariogenic challenge as well as the nocturnal pH conditions in the oral cavity. After pH cycling and treatment with CS-AMEL hydrogel, a synthetic layer composed of oriented apatite crystals was formed on the eroded enamel surface. CS-AMEL repaired the artificial incipient caries by re-growing oriented crystals and reducing the depth of the lesions by up to 70% in the pH-cycling systems. The results clearly demonstrate that the CS-AMEL hydrogel is effective at the restoration of erosive and carious lesions under pH-cycling conditions.
Bioinspired synthesis of hierarchically structured calcium phosphate (CaP) material is a highly promising strategy for developing improved bone substitute materials. However, synthesis of CaP materials with outstanding mechanical properties still remains an ongoing challenge. Inspired by the formation of lamellar structure in nacre, we designed an organic matrix composed of chitosan and cis-butenediolic acid (maleic acid, MAc) that could assemble into a layered complex and further guide the mineralization of monetite crystals, resulting in the formation of organized and parallel arrays of monetite platelets with a brick-and-mortar structure. Using the layered monetite-chitosan composite as a precursor, we were able to synthesize hydroxyapatite (HAp) with multiscale hierarchically ordered structure via a topotactic phase transformation process. On the nanoscale, needlelike HAp crystallites assembled into organized bundles that aligned to form highly oriented plates on the microscale. On the large-scale level, these plates with different crystal orientations were stacked together to form a layered structure. The organized structures and composite feature yielded CaP materials with improved mechanical properties close to those of bone. Our study introduces a biomimetic approach that may be practical for the design of advanced, mechanically robust materials for biomedical applications.
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