Chitosan/calcium nanoparticles as advanced antimicrobial coating for paper documents
Graphical abstract
Introduction
In recent years, advances in nanotechnology have pioneered new research fields such as the conservation of paper-based artifacts using nanomaterials. The preservation of paper-based historical artifacts is a critical process, primarily based on neutralizing the acidity level of the artifact. The increase in the acidity of the artifacts over time causes deformations in the cellulose structure of the paper, thus causing the paper to deteriorate and lose its integrity. There has been an intense effort to prepare various micro/nanoformulations as deacidification agents developed by nanotechnology. Various deacidification agents such as magnesium hydroxide, calcium hydroxide, or calcium carbonate are used to remove the acidity of the paper [1], [2], [3], [4]. These agents all have diminished the acidity of paper-based materials and strengthened them. Although these approaches are useful and effective, they mainly focus on the papers' neutralization through specific alkali agents.
The presence of bacteria and fungi on paper-based materials also plays an important role in increasing acidity. The extracellular secretions of these microorganisms increase the acidity level in the cellulose structure and eventually lead to disruption of the paper [5]. Removing the bacteria and fungi colonies from the artifact can also be considered as an effective approach that will indirectly strengthen the cellulose structure and prevent increased acidity. Usage of well-investigated antimicrobial agents such as benzimidazole and sulfonamid derivatives can be an effective strategy to prevent microorganism growth [6], [7], [8], [9], [10]. Moreover, this antimicrobial activity can be improved either by using antimicrobial nanomaterials alone or coupled with specific antimicrobial agents [10], [11], [12]. In the sense of paper conservation, Ponce-Jimenez et al. proved that chitosan provides effective protection for the papers against deterioration [13]. Jia et al. prepared chitosan nanoparticles (CS NPs) around 75 nm using the ball milling method and demonstrated that CS NPs can provide a safe environment acting as antimicrobial agents as well as reinforcement materials [14]. These efforts indicate a strong need to develop novel nanostructures that can provide enhanced protection for paper-based documents.
In addition to the studies mentioned above, our approach is based on increasing the effectiveness of CS NPs by calcium decoration. Here, we prepared calcium/chitosan nanoparticles (Ca/CS NPs) to preserve paper-based library and archival materials. Following the fabrication of the nanoparticles, they were characterized by dynamic light scattering to determine their average size, zeta potential, and dispersity index. Also, morphological and chemical makeup analyses were performed by Scanning Electron Microscopy (SEM), Fourier-Transform Infrared Spectroscopy (FTIR), and Energy dispersive X-ray (EDX) spectroscopy, respectively. The deacidification effect of the nanoparticles was investigated via periodic pH level measurements on paper-based samples, and their antimicrobial activity was confirmed through the minimum inhibitory concentration (MIC) assay for specific bacteria and fungi strains. Moreover, the antimicrobial activity of chitosan and Ca/CS NPs at the molecular level was investigated. At the molecular level, DNA gyrase and dihydrofolate reductase (DHFR) are preferred as essential targets to elucidate the antimicrobial properties of the materials [15], [16], [17]. The binding modes and energies of the antibacterial DNA gyrase and antifungal Candida albicans dihydrofolate reductase receptors and the inhibition activities at the active sites of these receptors were determined through molecular docking technique. Finally, this antimicrobial effect was also tested after the nanoparticle coating on the paper-based samples. The resulting nanoparticles displayed a microorganism-free environment for up to 10 days for the paper-based sample.
Section snippets
Materials
Chitosan (75–85 % deacetylated, low molecular weight, CAS no. 9012-76-4), sodium tripolyphosphate (TPP, CAS no. 7758-29-4), and calcium hydroxide (CAS no.1305-62-0) were from Sigma–Aldrich. Acetic acid (CAS no. 64-19-7) was purchased from Merck. For antimicrobial tests, the nutrient broth (CAS no. 70122) was purchased from Sigma-Aldrich. The strains of Micrococcus luteus (ATCC 15307), Bacillus megaterium (ATCC 14581), Bacillus subtilis (ATCC 6051), Aspergillus niger (CRM-16404), Aspergillus
Physicochemical characterization of CS NPs and Ca/CS NPs
DLS results of the nanoparticles are presented in Table 1. The average particle size and PdI values of both CS NPs and Ca/CS NPs are <100 nm in size and have homogeneous dispersion. The association of calcium ions with the blank chitosan nanostructures resulted in a small increase in average particle size from 61.5 ± 0.4 nm to 66.7 ± 0.7 nm and PdI value from 0.1 to 0.2. Besides, the zeta potential value of Ca/CS was reported as 11.7 ± 0.9 mV, whereas it was 16.9 ± 0.6 mV for bare CS NPs These
Conclusion
CS NPs successfully prepared and decorated with calcium ions for the preservation of paper-based artifacts. Antifungal and antibacterial assays revealed that calcium decoration increased the antimicrobial activity of the nanoparticles, by lowering the required dosage and increasing the inhibitory effect. This antimicrobial activity also enabled pH stability to the paper-based artifacts.
The molecular docking results were also in accordance with the antimicrobial activity results. In particular,
CRediT authorship contribution statement
All authors made a significant contribution to the work reported, whether that is in the conception, study design, execution, acquisition of data, analysis and interpretation, or in all these areas; took part in drafting, revising or critically reviewing the article; gave final approval of the version to be submitted to IJBIOMAC.
Acknowledgment
In this study, the support of The Scientific and Technological Research Council of Turkey (TUBITAK) (Project number: 2180454) was used. The authors would thank TUBITAK for their support. We would like to thank Anuipraya Kumar for allowing the Small Molecular Docking program. E.M. would like to acknowledge the support from the National Institute of Biomedical Imaging and Bioengineering (5T32EB009035).
References (45)
- et al.
Benzimidazole analogues as efficient arsenals in war against methicillin-resistance Staphylococcus aureus (MRSA) and its SAR studies
Bioorg. Chem.
(2021) - et al.
Antibacterial activities of sulfonyl or sulfonamide containing heterocyclic derivatives and its structure-activity relationships (SAR) studies: a critical review
Bioorg. Chem.
(2020) - et al.
Biomaterials: antimicrobial surfaces in biomedical engineering and healthcare
Curr. Opin. Biomed. Eng
(2022) - et al.
Engineered nanomaterials for antimicrobial applications: a review
Appl. Mater. Today
(2020) - et al.
Innovative nano-carriers in anticancer drug delivery-a comprehensive review
Bioorg. Chem.
(2019) - et al.
Recent advances and challenges in silicon carbide (SiC) ceramic nanoarchitectures and their applications
Mater.TodayCommun.
(2021) - et al.
Synthesis, characterization, biological activities and molecular docking of Epilobium parviflorum aqueous extract loaded chitosan nanoparticles
Int. J. Biol. Macromol.
(2020) - et al.
Formation mechanism of monodisperse, low molecular weight chitosan nanoparticles by ionic gelation technique
Colloids Surf. B: Biointerfaces
(2012) - et al.
X-ray crystallographic studies of Candida albicans dihydrofolate reductase: high resolution structures of the holoenzyme and an inhibited ternary complex
J. Biol. Chem.
(1997) - et al.
Comparison of scanning electron microscopy, dynamic light scattering and analytical ultracentrifugation for the sizing of poly(butyl cyanoacrylate) nanoparticles
Eur. J. Pharm. Biopharm.
(2004)
Detection of silica and calcium carbonate deposits in granulomatous areas of skin sarcoidosis by μFourier transform infrared spectroscopy and field emission scanning electron microscopy coupled with energy dispersive X-ray spectroscopy analysis
C R Chim.
Antibacterial activity of calcium hydroxide combined with chitosan solutions and the outcomes on the bond strength of RealSeal sealer to radicular dentin
J. Biomed. Res.
Design, synthesis and molecular docking study of thienopyrimidin-4(3H)-thiones as antifungal agents
J. Saudi Chem. Soc.
A key review on oxadiazole analogs as potential methicillin-resistant Staphylococcus aureus (MRSA) activity: structure-activity relationship studies
Eur. J. Med. Chem.
Role of BP*C@AgNPs in bap-dependent multicellular behavior of clinically important methicillin-resistant Staphylococcus aureus (MRSA) biofilm adherence: a key virulence study
Microb. Pathog.
Synthesis of novel benzodioxane midst piperazine moiety decorated chitosan silver nanoparticle against biohazard pathogens and as potential anti-inflammatory candidate: a molecular docking studies
Int. J. Biol. Macromol.
Nanoparticles for cultural heritage conservation: calcium and barium hydroxide nanoparticles for wall painting consolidation
Chem. Eur. J
Colloid and materials science for the conservation of cultural heritage: cleaning, consolidation, and deacidification
Langmuir
Nanomaterials in art conservation
Nat. Nanotechnol.
Newly developed nano-calcium carbonate and nano-calcium propanoate for the deacidification of library and archival materials
J. Anal. Methods Chem.
Effect of fungi on the destruction of historical parchment and paper documents
Pol. J. Environ. Stud.
Combating a master manipulator: Staphylococcus aureus immunomodulatory molecules as targets for combinatorial drug discovery
ACS Comb. Sci.
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