Toward Sustainability through Bio-Based Materials at the Interfaces with Living Systems

A special issue of Coatings (ISSN 2079-6412). This special issue belongs to the section "Surface Coatings for Biomedicine and Bioengineering".

Deadline for manuscript submissions: closed (10 October 2023) | Viewed by 29746

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Department of Surgery, University of Pittsburgh, Pittsburgh, PA 15213, USA
Interests: regenerative medicine; bioresorbable biomaterials; targeted delivery and nanocarriers
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Special Issue Information

Dear Colleagues,

Advances in technologies have improved many aspects of human life over the centuries through the materials functioning at the interface with living systems. However, many novel materials produced at large scale are consumed and discarded in a single stream, threatening a new grand challenge of the 21st century, environmental sustainability. For example, the WHO projected that frontline health workers needed 89 million facial masks monthly during the COVID-19 pandemic. Micro- and nanofabrication of bio-based materials has emerged as a technical solution to transform current materials-based technologies to become recyclable, biodegradable, and less energy intensive. Many bio-based materials (e.g., papers and silk textiles) have been used for thousands of years, proving their sustainability. Recent advances in science and engineering have revealed new functionality and applications of these traditional materials by regeneration, recombination, and modification of their structures and components. For example, a silk-based seed coating technology developed by my colleagues at the Massachusetts Institute of Technology encapsulates biofertilizer (nitrogen-fixing Rhizobium bacteria), which may alleviate CO2 release and water usage from the Haber–Bosch process for nitrogen fertilizer production.

This Special Issue focuses on the future of bio-based materials’ applications at the interfaces with the living systems (e.g., human body, plant, soil microbiome, food). We invite research and review articles reporting new developments and improvements of bio-based materials that contribute to building a sustainable environment. New perspectives on bio-based materials, such as how we should define bio-based materials and access their sustainability, are welcome to be discussed.

The scope of this Special Issue will serve as a forum for papers on the following concepts, but manuscripts on other relevant topics are also welcome:

  • Development of new bio-based materials and exploration of their new applications.
  • Surface modification and functionalization of bio-based materials.
  • Application of bio-based materials for biomedical engineering, packaging, agri-food, environmental remediation, etc.
  • Theoretical and experimental research studying physical, chemical, and mechanical properties of bio-based materials.
  • Sustainability assessment of bio-based materials.
  • New perspectives on bio-based materials.
  • Reviews on recent developments in bio-based materials.

Dr. Seungil Kim
Guest Editors

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Keywords

  • bio-based materials
  • bioresorbable biomaterials
  • sustainable materials
  • surface modification
  • nature-derived materials
  • biodegradable packaging

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Published Papers (10 papers)

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Research

Jump to: Review

15 pages, 3824 KiB  
Article
Assessing the Bioreceptivity of Biobased Cladding Materials
by Karen Butina Ogorelec, Ana Gubenšek, Faksawat Poohphajai and Anna Sandak
Coatings 2023, 13(8), 1413; https://doi.org/10.3390/coatings13081413 - 11 Aug 2023
Cited by 2 | Viewed by 1889
Abstract
Materials exposed to the outdoors are prone to various deterioration processes. Architectural coatings are designed to protect surfaces against environmental and biotic degradation and to provide a decorative layer. The objective of this work was to examine the early colonisers on a diverse [...] Read more.
Materials exposed to the outdoors are prone to various deterioration processes. Architectural coatings are designed to protect surfaces against environmental and biotic degradation and to provide a decorative layer. The objective of this work was to examine the early colonisers on a diverse set of coated and non-coated biobased façade materials. A set of 33 wood-based cladding materials were exposed to four cardinal directions and monitored in outdoor conditions. The surfaces were sampled using a wet swab and plated on DG-18 agar, which prevents the growth of bacteria and limits the growth of fast-growing fungi. Pure cultures were then isolated and identified through PCR amplification and Sanger sequencing of specific DNA regions/genes. The response of cladding materials to weathering and fungal infestation was assessed. The proposed techniques enabled the identification of features that promote/inhibit fungal colonisation and revealed the preference of certain fungi for specific materials. Both the material type and the climate condition at the exposure site influence fungal colonisation. This study is a starting point for more exhaustive assays that aim to develop a novel coating system based on controlled and optimized fungal biofilm formation, and is proposed as a nature-inspired alternative for the protection of architectonic surfaces. Full article
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23 pages, 6523 KiB  
Article
Influence of Cu Substitution on the Properties of Hydroxyapatite Targets and Deposited Coatings
by Konstantin Prosolov, Vladimir Lastovka, Margarita Khimich, Ivan Glukhov, Alexander Kashin, Nikita Luginin and Yurii Sharkeev
Coatings 2023, 13(8), 1410; https://doi.org/10.3390/coatings13081410 - 11 Aug 2023
Cited by 1 | Viewed by 1133
Abstract
In addressing the issue of optimizing the mechanical and electrochemical properties of hydroxyapatite (CaP) materials for biomedical applications, this research explored the incorporation of copper (Cu) into the material and scrutinized its impact through various processing stages, from powders to ceramics and finally [...] Read more.
In addressing the issue of optimizing the mechanical and electrochemical properties of hydroxyapatite (CaP) materials for biomedical applications, this research explored the incorporation of copper (Cu) into the material and scrutinized its impact through various processing stages, from powders to ceramics and finally to coatings. Our investigation indicated that the integration of CuO into CaP significantly changed the lattice parameters of hydroxyapatite from manufactured powders to sintered targets, indicating a structural evolution. Simultaneously, the change in the elemental composition and Ca/P ratio was also followed by each step from manufactured powders to deposited coatings. Mechanical testing revealed an impressive increase in the hardness of coatings to a high of 37 GPa for the 0.2CuO-CaP sample, a substantial improvement when compared to 13 GPa for pure Ti. The corrosion resistance of the coatings also improved, evidenced by the decrease in corrosion current density (Icorr) from 60.2 ± 5.2 nA/cm2 for pure Ti to a lower 3.9 ± 0.5 nA/cm2 for the CaP coating. Our study has revealed that the structural, mechanical, and electrochemical properties of CaP materials can be finely adjusted through the addition of Cu, promising advances in the realm of biomedical applications. Moreover, these results hint at the potential to tune the electrophysical characteristics of CaP coatings, an avenue for future exploration. Full article
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12 pages, 5236 KiB  
Article
Mechanisms of Premature Fracture in Modular Neck Stems Made of CoCrMo/Ti6Al4V and Ti6Al4V/Ti6Al4V Alloy
by Drago Dolinar, Miro Gorenšek, Klemen Avsec, Barbara Šetina Batič, Matej Hočevar, Matjaž Godec, Borut Žužek, Mojca Debeljak, Monika Jenko, John T. Grant and Boštjan Kocjančič
Coatings 2023, 13(7), 1255; https://doi.org/10.3390/coatings13071255 - 16 Jul 2023
Viewed by 1438
Abstract
In this paper, we present the mechanisms of premature fracture of modular neck stems in two case studies: (I) when the neck and stem are both made of the same Ti6Al4V alloy, and (II) when the neck and stem are made from two [...] Read more.
In this paper, we present the mechanisms of premature fracture of modular neck stems in two case studies: (I) when the neck and stem are both made of the same Ti6Al4V alloy, and (II) when the neck and stem are made from two different alloys, CoCrMo and Ti6Al4V alloy. Our study integrates two orthopedic patients who have undergone primary uncemented THA for usual indications in two orthopedic centers (Community Health Centre and University Medical Centre). Both centers are part of the national public health care system. Both surgeries were performed by two skilled orthopedic surgeons with more than 10 years of experience in THA. The survivorship of the modular neck of cast CoCrMo alloy was 24 months. The survivorship of the modular neck from Ti6Al4V alloy was 84 months. Multivariate analyses were performed to assess the differences in the fretting, corrosion, and fatigue of the two prematurely failed modular neck stems: stereo light microscopy (SLM), scanning electron microscopy (SEM), X-ray energy-dispersive spectroscopy (EDS), and electron backscatter diffraction (EBSD). Patient demographic information, including sex, age, body mass index, survivorship of implants, and reason for the revision, was collected from medical records. We found that fretting and fatigue occurred on both neck-stem retrievals due to additional galvanic corrosion, but the CoCrMo/Ti6Al4V alloy system suffered more corrosion due to additional galvanic corrosion and fractured earlier than the Ti6Al4V/Ti6Al4V metal alloy system. Both metallic alloy systems used in this application are known to be highly corrosion-resistant, but the bio-tribo-corrosion processes need to be understood in detail and characterized so that appropriate improvements in design and materials can be made. Full article
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12 pages, 6196 KiB  
Article
Permeability of Skin-Mimicking Cell Coatings by Polymers of Complex Architecture Based on Polyoxazolines
by Gia Storti, Giulia Romano, Kristen Gilmore, Nicholas Sadowski, Andrii Tiiara, Igor Luzinov and Alexander Sidorenko
Coatings 2023, 13(6), 1007; https://doi.org/10.3390/coatings13061007 - 29 May 2023
Cited by 2 | Viewed by 2267
Abstract
In the scope of drug delivery, the transdermal route is desirable because it provides attainable therapeutic concentrations and has minimal systemic side effects. To make the skin a feasible route for the delivery of therapeutic agents, the biggest challenge is overcoming its natural [...] Read more.
In the scope of drug delivery, the transdermal route is desirable because it provides attainable therapeutic concentrations and has minimal systemic side effects. To make the skin a feasible route for the delivery of therapeutic agents, the biggest challenge is overcoming its natural coating. In this paper, we investigate the effect of the architectures (homopolymer vs. block copolymer vs. hybrid block–graft copolymer) of several amphiphilic polymeric derivatives of poly(2-oxazoline) on skin permeability. The block copolymers are composed of a hydrophobic poly(2-oxazoline) block and a hydrophilic PEG block. The hybrid block–graft copolymers are obtained by grafting hydrophobic side chains of polycaprolactone to a poly(2-oxazoline) backbone. We used the commercially available EpiDerm™ by MatTek, composed of human epidermal cells, as a model of human skin. Two parameters of skin permeation are reported: penetration rate and lag time. We hypothesize that the skin permeation characteristics correlate with the critical micelle concentration and particle size of the studied polymers, while both parameters are a function of the complex architectures of the presented macromolecular constructs. While homopolymer poly(2-oxazolines) show the least permeation, the block copolymers demonstrate partial permeation. The hybrid block–graft copolymers exhibited full penetration through the model skin samples. Full article
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18 pages, 3153 KiB  
Article
Ciprofloxacin-Loaded Composite Granules Enriched in Silver and Gallium Ions—Physicochemical Properties and Antimicrobial Activity
by Kamil Pajor, Łukasz Pajchel, Anna Zgadzaj, Paulina Kowalska, Anna Kowalczuk and Joanna Kolmas
Coatings 2023, 13(3), 494; https://doi.org/10.3390/coatings13030494 - 23 Feb 2023
Cited by 2 | Viewed by 1913
Abstract
Various calcium phosphates (hydroxyapatite, α- and β-tricalcium phosphate, and brushite) containing silver or gallium ions were synthesized via standard methods and subjected to physicochemical analysis by Fourier transform infrared spectroscopy (FT-IR), powder X-ray diffractometry (PXRD), and atomic absorption spectrometry (AAS). In the next [...] Read more.
Various calcium phosphates (hydroxyapatite, α- and β-tricalcium phosphate, and brushite) containing silver or gallium ions were synthesized via standard methods and subjected to physicochemical analysis by Fourier transform infrared spectroscopy (FT-IR), powder X-ray diffractometry (PXRD), and atomic absorption spectrometry (AAS). In the next step, the obtained calcium phosphate powders, sodium alginate, and chondroitin were used to produce composite granules. Ciprofloxacin, a broad-spectrum antibiotic that can be used in local delivery systems targeting bone tissue, was loaded into the granules. The release of silver and gallium ions as well as ciprofloxacin was then examined by inductively coupled plasma mass spectrometry (ICP-MS) and high-performance liquid chromatography (HPLC), respectively. The cytotoxicity of the granules was studied using a neutral red uptake (NRU) test and mouse embryonic fibroblasts. Moreover, preliminary antibacterial activity against Staphylococcus aureus and Escherichia coli was measured. The study showed that the type of calcium phosphates enriched in silver or gallium significantly affects the release profile of these ions. Biphasic calcium phosphates also have an impact on the morphology of the granules. Most of the granules turned out to be non-toxic to mammalian cells. Microbiological tests showed high antibacterial activity against both strains of bacteria. Full article
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16 pages, 4595 KiB  
Article
Studies of New Layer Formation on the Surface of Zinc Doped Hydroxyapatite/Chitosan Composite Coatings in Biological Medium
by Mikael Motelica-Heino, Mihai Valentin Predoi, Steluta Carmen Ciobanu, Simona Liliana Iconaru and Daniela Predoi
Coatings 2023, 13(2), 472; https://doi.org/10.3390/coatings13020472 - 19 Feb 2023
Cited by 11 | Viewed by 1808
Abstract
Usually, before being used in biomedical applications, a biomaterials’ bioactivity is tested by in vitro methods that simulate similar conditions to those found in the human body. In this work, we report on the synthesis of zinc-doped hydroxyapatite–chitosan (ZnHApC) composite coatings by the [...] Read more.
Usually, before being used in biomedical applications, a biomaterials’ bioactivity is tested by in vitro methods that simulate similar conditions to those found in the human body. In this work, we report on the synthesis of zinc-doped hydroxyapatite–chitosan (ZnHApC) composite coatings by the vacuum deposition method. The surface microstructure and the chemical and molecular modification of the coatings before and after soaking in DMEM (Dulbecco’s Modified Eagle’s Medium) were studied. For this objective, techniques such as attenuated total reflection (ATR), Fourier transform infrared (FTIR) spectroscopy, metallographic microscopy (MM), and scanning electron microscopy (SEM) were applied used. Also, water contact angle measurements and swelling studies were made on ZnHApC composite coatings before and after soaking in a biological medium. The coatings’ adherence to the substrate was also studied. The results of antifungal studies on ZnHApC composite coatings against the Candida albicans microbial strain reveal their good antifungal activity. The biocompatibility of the composite coatings was tested using a primary osteoblast cell line. Our results suggest that zinc-doped hydroxyapatite–chitosan samples could be used as a bioimplant material due to their enhanced bioactivity and biocompatibility. Full article
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14 pages, 1680 KiB  
Article
Study of Argon and Oxygen Mixtures in Low Temperature Plasma for Improving PLA Film Wettability
by Joanna Izdebska-Podsiadły
Coatings 2023, 13(2), 279; https://doi.org/10.3390/coatings13020279 - 26 Jan 2023
Cited by 6 | Viewed by 2373
Abstract
Oxygen (O2) and argon (Ar) plasma give a significant improvement in the wettability of PLA films. This study investigates the effectiveness of plasma activation with a mixture of these two gases. The study includes contact angle measurements with water and diiodomethane [...] Read more.
Oxygen (O2) and argon (Ar) plasma give a significant improvement in the wettability of PLA films. This study investigates the effectiveness of plasma activation with a mixture of these two gases. The study includes contact angle measurements with water and diiodomethane and calculation of surface free energy (SFE) together with its polar and dispersion components. In addition, a chemical analysis of the surface, surface roughness, weight loss and the change in tensile strength were examined. As a result of the study, it was found that the use of a mixture of oxygen and argon during the plasma activation of the polylactide film gives better improvement in wettability than the use of pure gases. Moreover, the use of a mixture of these gases in equal proportions turned out to be the most effective, providing the highest value of the SFE and its polar component, as well as the lowest value of the water contact angle. Furthermore, plasma activation with this gas mixture results in reduced surface etching compared to other gas compositions, which manifests itself in lower weight reduction and an insignificant change in tensile strength. Full article
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11 pages, 3195 KiB  
Article
Activity of Colloidal Silver Solution against Microorganisms Implicated in Ocular Infections
by Anna Rita Blanco, Andreana Marino, Manuela D’Arrigo and Antonia Nostro
Coatings 2023, 13(2), 265; https://doi.org/10.3390/coatings13020265 - 23 Jan 2023
Cited by 2 | Viewed by 8328
Abstract
Endophthalmitis most likely originates from both planktonic bacteria suspended in the tear film and bacteria adherent to the conjunctiva and the eyelid. This study aimed to expand the research on the effectiveness of a colloidal silver solution (Silverix®) against ocular microorganisms. [...] Read more.
Endophthalmitis most likely originates from both planktonic bacteria suspended in the tear film and bacteria adherent to the conjunctiva and the eyelid. This study aimed to expand the research on the effectiveness of a colloidal silver solution (Silverix®) against ocular microorganisms. The activity of Silverix® was evaluated against methicillin-resistant Staphylococcus aureus, S. epidermidis, ofloxacin-resistant Pseudomonas aeruginosa, and Candida albicans strains, previously characterized for their antibiotic resistance and biofilm-forming capabilities. The microbial killing was estimated at various times in the presence and absence of colloidal silver solution against planktonic and biofilm-embedded cells. The results documented the efficacy of Silverix® on planktonic cells of S. aureus and S. epidermidis (2.49–2.87 Log CFU/mL reduction) and P. aeruginosa strains (3–4.35 Log CFU/mL reduction). On the contrary, C. albicans showed mild susceptibility. Regarding early biofilm, the ocular isolates were harder to kill (2–2.6 Log CFU/mL reduction) than the reference strains, whereas a similar decrease (3.1 Log CFU/mL reduction) was estimated for P. aeruginosa strains. The light microscope images of biofilms treated with colloidal solution confirmed the ability of Silverix® to destroy the biofilm. Full article
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15 pages, 5830 KiB  
Article
A Novel Low-Profile Self-Expanding Biodegradable Percutaneous Heart Valve Frame That Grows with a Child
by Mohamed Ibrahim, Kara X. Nghiem, Kaitlin Chung, Moataz Elsisy, Uma J. Gosai, Seungil Kim, Sangho Ye, William R. Wagner and Youngjae Chun
Coatings 2023, 13(1), 184; https://doi.org/10.3390/coatings13010184 - 14 Jan 2023
Viewed by 2947
Abstract
According to rough estimates, one in every 125 newborns born in the United States has a congenital cardiac abnormality that must be repaired. With the recent development of new biomaterials and innovative treatment methods, percutaneous cardiac valve replacement has been considered as an [...] Read more.
According to rough estimates, one in every 125 newborns born in the United States has a congenital cardiac abnormality that must be repaired. With the recent development of new biomaterials and innovative treatment methods, percutaneous cardiac valve replacement has been considered as an alternative to surgical procedures. While percutaneous heart valve replacement is a relatively new procedure with a few commercially available devices, the devices are not sufficiently low-profile, and do not grow with the child. To address this issue, a novel low-profile growing percutaneous pediatric heart valve frame made of two types of unique metallic biomaterials (supere lastic nitinol and biodegradable iron) has been developed through this study. The developed pediatric heart valve frame has an innovative mechanism that will expand its diameter by disconnecting biodegradable metals, enabling the growth of the device with the surrounding tissue in the cardiac space. The thermally treated iron wires show stable and gradual degradation characteristics, showing approximately 7.66% for both wires treated under 350 and 450 °C. Polymer-coated wires show a degradation range of 4.96 to 5.55% depending on the type of coating. Degradation test results show the predicted 9–23 months of degradation depending on the type of surface treatment (e.g., thermal treatment, polymer coating), which is a suitable range when compared with the theoretical arterial vessel remodeling process period in the human vascular system. Radial forces calculated by finite element analysis and measured by mechanical testing matched well, showing 5–6 N with a 20% diameter reduction considering the deployed valve frame in the heart. Biocompatibility study results demonstrated superior cell viability in thermally treated iron wires after 3 days of cell culture and showed rarely found platelets on the surface after 3-h blood exposure tests. Prototype devices were successfully fabricated using optimized advanced joining processes for dissimilar metallic materials such as nitinol and iron. This study represents the first demonstration of self-expanding and biodegradable percutaneous heart valve frames for pediatric patients that grow with a child. Full article
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Review

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24 pages, 1633 KiB  
Review
Whether Carbon Nanotubes Are Capable, Promising, and Safe for Their Application in Nervous System Regeneration. Some Critical Remarks and Research Strategies
by Andrzej Zieliński and Beata Majkowska-Marzec
Coatings 2022, 12(11), 1643; https://doi.org/10.3390/coatings12111643 - 30 Oct 2022
Cited by 6 | Viewed by 4121
Abstract
Carbon nanotubes are applied in or considered for different fields of medicine. Among them is the regeneration or rebuilding of nervous system components, which still lack substantial progress; this field is supported by carbon nanotubes to a great extent as the principal material. [...] Read more.
Carbon nanotubes are applied in or considered for different fields of medicine. Among them is the regeneration or rebuilding of nervous system components, which still lack substantial progress; this field is supported by carbon nanotubes to a great extent as the principal material. The limited research on this issue has involved PU/silk/MWCNTs, PCL/silk/MWCNTs, PCL/PGS/CNTs, chitin/CNTs, PGF/CNTs, CNTs/PGFs/PLDLA, MWCNTs/chitosan, MWCNTs/PPy, PLA/MWCNTs, PU/PAA/MWCNts, GelMA/SACNTs, and CNTs alone, which have been subjected to different surface modifications and applied in the form of solid materials or scaffolds that are degradable or nondegradable. So far, these attempts have shown that the use of surface-modified MWCNTs is a promising way to improve the functions of nervous systems as a whole, even though some drawbacks, such as the potential cytotoxicity or the weak adhesion of CNTs to other components, may appear and be eliminated by their proper functionalization. The present review presents an idea of a nonbiodegradable scaffold structure composed of a chosen conductive polymer that is able to create a scaffold structure, a selected nanocarbon form (with MWCNTs as the first candidate), and a corrosion-resistant metal as a conductor. Other substances are also considered for their ability to increase the mechanical strength and adhesion of CNTs and their biological and electrical properties. The novelty of this approach is in the simultaneous use of nanocarbon and conductive metallic fibers in a polymer scaffold structure. Full article
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