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. 2022 Jul 31:2022:6331465.
doi: 10.1155/2022/6331465. eCollection 2022.

Layer-by-Layer Fabrication of PAH/PAMAM/Nano-CaCO3 Composite Films and Characterization for Enhanced Biocompatibility

Naemi Tonateni Shifeta  1   2 , Shindume Lomboleni Hamukwaya  2   3 , Qi An  2 , Huiying Hao  2 , Melvin Mununuri Mashingaidze  3
Affiliations

Layer-by-Layer Fabrication of PAH/PAMAM/Nano-CaCO3 Composite Films and Characterization for Enhanced Biocompatibility

Naemi Tonateni Shifeta et al. Int J Biomater. .

Abstract

Nanoparticle production and functionalization for various biomedical uses are still challenging. Polymer composites constituted of poly(amidoamine) (PAMAM), polyallylamine hydrochloride (PAH), and calcium carbonate (CaCO3) nanoparticles have good biocompatibility with physiological tissue and fluids, making them excellent candidates for biomedical applications. This study investigated the characteristics of polymeric/nano-CaCO3 composite films based on a PAH/PAMAM matrix, which were fabricated through layer-by-layer synthesis on quartz glass substrates. It was found that the as-prepared elastic moduli of the resultant (PAH/PAMAM) n -CaCO3 (where n represents the number of bilayers) composite films varied from 1.40 to 23.70 GPa for different degrees of cross-linking when 0.1 M nano-CaCO3 particles were incorporated into the polymer matrix. The highly cross-linked (PAH/PAMAM)15-CaCO3 composite film had the highest recorded elastic modulus of 23.70 GPa, while it was observed that for all the composite films fabricated for the present study, the addition of the nano-CaCO3 particles approximately doubled the elastic modulus regardless of the degree of polymerization. Live/Dead assays were used to determine whether the produced composite films were compatible with human lung fibroblast cells. The findings indicate that the (PAH/PAMAM)7.5-CaCO3 composite film had the most positive effect on cell growth and proliferation, with the (PAH/PAMAM)15-CaCO3 composite film demonstrating significant ion transport behavior with low impedance, which was considered good for in vivo rapid cell-to-cell communication. Therefore, the (PAH/PAMAM)7.5-CaCO3 and (PAH/PAMAM)15-CaCO3 composite films are potential tissue engineering biomaterials, but further studies are essential to generate more data to evaluate the suitability of these composites for this and other biomedical functions.

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Conflict of interest statement

The authors declare that they have no conflicts of interest.

Figures

Figure 1
Figure 1
Allotropic structural cells of calcium carbonate: (a) vaterite, (b) calcite, and (c) aragonite. The neighboring environment of the cation and the cation-oxygen distances are also shown (copyright: Royal Society of Chemistry 2014, order number 1198792 [19]).
Scheme 1
Scheme 1
Schematic diagram of LbL fabrication process of cross-linked (PAH/PAMAM)7.5 multilayers, biomineralization of CaCO3, and cell culture using HLFC.
Figure 2
Figure 2
SEM images of calcium carbonate of (a1–a3) noncross-linked, (b1–b3) low cross-linked, (c1–c3) medium cross-linked, and (d1–d3) highly cross-linked (PAH/PAMAM)7.5 multilayers.
Figure 3
Figure 3
SEM and EDX analysis of (PAH/PAMAM)7.5-CaCO3 composite. Elemental mapping of calcium, carbon, and oxygen from all the components on the cross section multilayers of (a) noncross-linked, (b) low cross-linked, (c) medium cross-linked, and (d) highly cross-linked films.
Figure 4
Figure 4
TEM and SAED of (a, b) amorphous calcium carbonate, (c, d) vaterite, and (e, f) calcite obtained from the medium cross-linked of (PAH/PAMAM)7.5-CaCO3 from PVDF-HFP substrate.
Figure 5
Figure 5
(a) XRD patterns and (b) FT-IR obtained from all cross-linked samples of PAH/PAMAM7.5-CaCO3 on a quartz glass substrate.
Figure 6
Figure 6
(a) Raman spectrum of all cross-linkages and Raman mapping of (b) noncross-linked (c) low cross-linked, (d) medium cross-linked, and (e) highly cross-linked (PAH/PAMAM)7.5-CaCO3. (f) PAH/PAMAM)7.5 -CO32− (control) (dimension of mapping area = 5 μm × 5 μm).
Figure 7
Figure 7
Film thickness representation before and after mineralization. (a) AFM of film thickness before mineralization of (PAH/PAMAM)7.5 and (b) SEM cross section of the films after mineralization of (PAH/PAMAM)7.5 -CaCO3.
Figure 8
Figure 8
Output voltage-time curve of PVDF-HFP, PVDF-HFP/(PAH/PAMAM)7.5, and PVDF-FP/(PAH/PAMAM)7.5-CaCO3 after finger-pressing.
Figure 9
Figure 9
Electrical properties (a), cyclic voltammograms, and (b) Nyquist plot (at a scan rate of 5 mVs−1) of different films in 0.1 M PBS.
Figure 10
Figure 10
The release profile of MB from the medium crossed-linked (PAH/PAMAM)7.5 film and (PAH/PAMAM)7.5-CaCO3 film at various pH values.
Figure 11
Figure 11
Fluorescent images of HLFCs cultured (a1–a4) 24 h, (b1–b4) 48 h, and (c1–c4) 72 h on substrates with different bilayers. Control experiment, no CaCO3.
See this image and copyright information in PMC

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