Recent Developments and Formulations for Hydrophobic Modification of Carrageenan Bionanocomposites
Abstract
:1. Introduction
2. Research Strategy and Data Collection
3. Factors Affecting Hydrophobicity of Carrageenan Bionanocomposites
3.1. Role of Matrix/Carrageenan Type
3.1.1. Kappa vs. Iota
3.1.2. Refined vs. Semi-Refined
3.2. Role of Plasticisers
3.3. Effect of Nanofillers
3.3.1. Polysaccharide-Based Nanofillers
3.3.2. Nanoclay/Bioceramic/Mineral Nanoparticles
3.3.3. Metal Oxide Nanoparticles, Nanotubes and Carbon Dots
3.3.4. Bioactive Agents
3.3.5. Synergistic Effects in Hybrid Bionanocomposites
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Search Terms/Keywords | Carrageenan Bionanocomposites Hydrophobic modification Nanofillers Bioactive Agents |
Databases | Google Scholar Science Direct Bielefeld Academic Search Engine (BASE) Semantic Scholar PubMed.gov |
Publication types included | Research papers Work articles Conference proceedings |
Publication types excluded | Review articles Book chapters |
Language | English |
Search period | 2018–2023 |
No. | Type of Carrageenan | Nanofillers | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Iota-carrageenan (Semi-refined) | Silicon dioxide and zinc oxide (SiO2 and ZnO) | Incorporation of nanoparticles (NPs) significantly decreased the water vapour permeability (WVP). | Increased ultraviolet (UV) screening and enhanced antimicrobial activity with the addition of NPs. | [2] |
2. | Kappa-carrageenan (Semi-refined) | ZnO | Increased solubility (up to 92%) with 0.5% ZnO, followed by a reduction at higher ZnO% (up to 75%). | Tensile strength increased up to 32 MPa with 0.5% ZnO, but then reduced up to 23 MPa with increasing ZnO%. Elongation at break exhibited a reducing trend, with an insignificant difference. | [5] |
No. | Type of Carrageenan | Nanofillers | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Refined and semi-refined kappa-carrageenan | Nanocellulose fibrils (NCF) | Lower moisture content (up to 23% for SRC and 25% for RC), higher water solubility (ranging between 38% and 60%), moisture uptake (between 47 and 67%), contact angle (between 38 and 100°) and WVP (between 8 and 16 g·mm·cm−2·h−1·Pa−1) for SRC + NCF than RC + NCF. | Overall properties of both semi-refined carrageenan (SRC) and refined carrageenan (RC) films were enhanced. | [51] |
2. | Kappa-carrageenan | Cellulose nanocrystals (CNC) derived from Indian gooseberry pomace | Decreased WVP from 3.21 to 2.25 g·mm/m2·day·kPa with increasing CNC concentration from 1 to 7%. | No structural changes with added CNC. Increased tensile strength and crystallinity with increasing CNC concentration. | [39] |
3. | Carrageenan | Agar, zinc sulphide nanoparticles (ZnS NP) and nanocellulose-based tea tree essential oil Pickering emulsion (TPE) | Addition of ZnSNP and TPE, alone or in combination slightly improved the water vapour barrier (WVP reduced from 0.66 to 0.52 × 10−9 g·m/m2·Pa·s) and water resistance of the films (WCA increased from 62 to 67°). | ZnSNPs improved mechanical strength, whereas PET slightly decreased the strength. However, the combined addition maintained the mechanical strength with slightly improved flexibility and thermal stability. Distinct antioxidant and antibacterial activity. | [52] |
4. | Kappa-carrageenan | Cellulose nanocrystals | Decreased water uptake (from 15 to 10%) and water sorption (128 to 115%) properties, increased water contact angle (from 47 to 90°). | Not specified. | [53] |
5. | Kappa-carrageenan | Cellulose nanocrystals | Better water barrier properties (water absorbency decreased from 886 to 562; film solubility decreased from 61 to 48; work of adhesion from 140 to 96), increased water contact angle (from 23 to 72°) and decreased water vapour permeation (from 8.9 to 4.7 × 10−11 g·m−1·s−1·Pa−1). | Superior mechanical, thermal, and UV barrier properties. | [36] |
6. | Kappa-carrageenan | Cellulose nanocrystals (CNCs) and organically modified montmorillonite (OMMT) | Significant reduction in water uptake (from ~160 to ~85%), both with individual fillers and with their synergistic effect. | Enhanced mechanical properties. | [4] |
No. | Type of Carrageenan | Nanofiller | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Semi-refined kappa-carrageenan | Three types of nanoclays (Hydrophilic bentonite (HB), Cloisite 10A, Cloisite® 30B) | Decreased WVP (12.6 to 12.2 × 10−8/g·mm·cm−2·h−1·Pa−1) with more hydrophobic nanoclay filler. | Semi-refined carrageenan more compatible with hydrophilic nanoclay, resulting in higher tensile and thermal properties. Hydrophobic nanoclay caused higher stiffness. | [54] |
2. | Kappa-carrageenan | Bentonite nanoclay (BT) | Decrease of water contact angle (from 76 to 27°), water uptake (from 12 to 9%) and water sorption ability 128 to 121%) with increasing BT content. | Increased surface roughness. Did not induce exfoliation of bentonite layers into the matrix, but there was an intercalation of polymer chains between the clay sheets. | [43] |
3. | Kappa-carrageenan | Nanoclay, Zataria multiflora plant extract (ZME) and glycerol (as plasticiser) | Increment in WVP with increasing ZME concentration according to Procedure 1 (1.21 to 2.21 × 10−10 g·m−1·s−1·Pa−1), and vice versa for Procedure 2 (2.83 to 1.54 × 10−10 g·m−1·s−1·Pa−1). | Incorporation of ZME resulted in strong UV screening effects. Increased film thickness and elongation at break (EB) values with increasing ZME concentration according to Procedure 1, and vice versa for Procedure 2. Tensile strength augmented with increasing ZME in both procedures. | [55] |
4. | Kappa-carrageenan | Nanoclay (montmorillonite) and rosemary extract | Significant reduction in water vapour permeability (5.3 to 2.1 × 10−10 g/m·s·Pa). | Increased tensile strength and elongation at break. More than 99% inhibition against B. cereus, E. coli, P. aeruginosa and S. aureus. | [37] |
No. | Type of Carrageenan | Nanofillers | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Semi-refined kappa-carrageenan | ZnO nanoparticles | Increased solubility (up to 92%) with 0.5% ZnO, followed by reduction at higher ZnO% (up to 75%). | Tensile strength increased with 0.5% ZnO, but then reduced with increasing ZnO%. Elongation at break exhibited a reducing trend, with insignificant difference. | [5] |
2. | Kappa-carrageenan | Sodium carboxymethyl cellulose (NaCMC) and Mg1−xZnxO nanoparticles | Higher swelling ratio in the presence of Zn, but inversely proportional to its concentration (Figure 6 in the cited article). | Enhanced thermal stability, springiness, adhesion, and consistency. Reduced hardness. | [41] |
3. | Kappa-carrageenan | ZnONPs/rosemary essential oil (RE)-incorporated zein nanofibres | Increased surface hydrophobicity (WCA increased from 33.8 to 77.7°) with the addition of ZnO and RE, both separately and together (additive effect). | Enhanced thermal and mechanical properties. Increased cell viability, antimicrobial activity and DPPH scavenging activity. | [56] |
4. | Carrageenan | ZnO NP and m-ZnO NPs (capped/stabilized by melanin) | Increased water contact angle (63.8 to 73.7°) and increasing trend in WVP values (ranging between 1.58 and 1.22 × 10−9 g·m/m2·Pa·s). | Lesser transparency. Higher UV-blocking property, thermal stability, mechanical properties, and antibacterial activity. | [57] |
Film Type | WVP (g·m−1·s−1·Pa−1 × 10−10) via P1 | WVP (g·m−1·s−1·Pa−1 × 10−10) via P2 |
---|---|---|
Neat film (KC alone) | 1.21 | 2.83 |
KC + 1% ZME | 1.49 | 1.81 |
KC + 2% ZME | 2.11 | 1.54 |
KC + 3% ZME | 2.21 | 1.76 |
Sample Code | Water Absorbency | Film Solubility | WVP (×10−11 g·m−1·s−1·Pa−1) | Water Contact Angle (°) | Work of Adhesion |
---|---|---|---|---|---|
CNC0 | 885.94 | 60.94 | 8.93 | 23.30 | 139.69 |
CNC1 | 825.00 | 54.63 | 7.37 | 23.70 | 139.38 |
CNC3 | 821.43 | 53.97 | 6.25 | 46.45 | 122.97 |
CNC5 | 778.05 | 51.22 | 5.36 | 55.65 | 113.88 |
CNC7 | 761.54 | 49.23 | 4.69 | 57.75 | 111.60 |
CNC9 | 561.79 | 47.97 | 9.15 | 71.80 | 95.54 |
No. | Form of Composites and End Use Applications | Components | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Scaffolds for bone tissue engineering | Kappa-carrageenan and nano-hydroxyapatite and chitosan | Appropriate swelling ability. | Rough surface morphology, better interaction between the components, favourable crystallinity, and higher mechanical properties. Increased deposition of apatite layer and greater cell viability. Enhanced protein adsorption and favourable degradation rate. | [71] |
2. | Hydrogels as potential drug delivery system | Kappa-carrageenan, polyvinyl alcohol and hydroxyapatite (bioceramic) nanoparticles | Lesser degree of swelling in presence of hydroxyapatite NPs (Decreased from 19.6 to 9.7 g/g). | Remarkable effect on antibacterial activity and in vitro release rate of ciprofloxacin. | [67] |
3. | Films for active food packaging applications | Kappa-carrageenan and silver loaded aminosilane modified halloysite nanotubes | Enhanced WCA (55.3 to 69.7°) and reduced WVP (1.6 to 1.4 × 10−9 g·m/m2·Pa·s) | Increased UV-light barrier property and antibacterial activity. | [3] |
Films | Thickness (μm) | TS (MPa) | EB (%) | EM (GPa) | WCA (deg) | WVP (×10−9 g·m/m2·Pa·s) |
---|---|---|---|---|---|---|
Carrageenan | 53.3 ± 0.7 a | 45.5 ± 3.5 a | 3.3 ± 2.4 a | 1.9 ± 0.2 a | 59.6 ± 2.6 a | |
Car/TiO2 | 54.5 ± 1.3 a | 47.4 ± 1.9 a | 4.4 ± 1.1 a | 2.6 ± 0.3 a,b | 60.4 ± 1.6 a | 1.32 ± 0.25 a |
Car/TNT | 62.8 ± 1.8 b | 55.8 ± 4.7 b | 4.2 ± 1.5 b | 3.1 ± 0.1 b | 62.3 ± 2.4 a | 1.19 ± 0.26 a |
Car/TNT−CuO | 67.1 ± 4.1 b | 54.6 ± 2.1 b | 5.6 ± 1.3 a | 2.5 ± 0.4 a,b | 66.2 ± 3.3 b | 1.15 ± 0.01 a |
No. | Form of Composites & End Use Applications | Components | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Green halochromic smart and active packaging films | Kappa-carrageenan, gelatin, TiO2 nanoparticle and anthocyanin | Significant improvement in moisture resistance. | Enhanced UV–Visible light barrier property, increment in mechanical and bacteriostatic properties, inhibition of oxidative reactions. Decomposed within ∼30 days under simulated environmental conditions. | [74] |
2. | Antimicrobial packaging films | Kappa-carrageenan and silver nanoparticles (AgNPs) prepared using pine needle extract-mediated synthesis | WVP and WCA significantly increased with added Ag NPs, but no significant increase as a function of increasing nanofiller concentration (except for 3% loading on WVP). | Film thickness, tensile strength. and elongation at break increased with added nanofiller, but independent of the loading concentration. Elastic modulus remained unchanged with 1% nanofiller loading, but increased with 2% and 3%. Significant improvement in UV blocking properties, antioxidant activity and potent antibacterial activity. Total colour difference (△E) of nanocomposite films increased significantly. | [45] |
3. | Pseudo-pasteurization films for kumquat preservation | Kappa-carrageenan, ZnO-doped carbon nanoparticles (ZnO/C) | Improved hydrophobicity and barrier ability. | Outstanding antibacterial properties, enhanced preservation capacity, slight loss of colour and transparency of films, improved tensile strength, thermal stability to varying degrees, qualified safety of films (verified through haemolysis and cell cytotoxicity experiments). | [75] |
4. | Films for active food packaging | Kappa-carrageenan, TiO2 nanotube (TNT), and CuO-doped TNT (TNT−CuO) | Increased surface hydrophobicity and water vapour barrier properties. | Imparted UV-blocking properties and increased mechanical strength. Significantly higher antibacterial activity for doped TNT than native TNT. | [42] |
5. | Films for active food packaging applications | Carrageenan, gelatin, and Enoki mushroom-derived carbon dots (mCDs) | No significant changes in water vapour permeability and hydrophobicity. | Significant improvement in mechanical properties, strong antioxidant activity. | [76] |
6. | Hydrogels to apply in biomedical research | Kappa carrageenan, NaCMC and Mg1-xZnxO nanoparticles | Higher swelling ratio in the presence of Zn, but inversely proportional to its concentration. | Enhanced thermal stability, springiness, adhesion, and consistency, reduced hardness. | [41] |
7. | Films for food packaging | Carrageenan and sulphur-coated iron oxide nanoparticles (Fe3O4@SNP) | Decreased WVP and increased water contact angle. | Effective UV blocking property and stronger antibacterial activity. | [40] |
8. | Films for active packaging | Kappa-carrageenan and silver ion loaded 3-aminopropyl trimethoxysilane-modified Fe3O4 nanoparticles | Addition of Fe3O4 significantly reduced the WCA of films, while the addition of Fe3O4-Ag and Fe3O4@NH2-Ag reduced it to a lesser extent. | Stronger antimicrobial activity, improved thermal stability, and UV blocking properties. | [77] |
9. | Films for active food packaging applications | Kappa-carrageenan and hybrid nanoparticles (HNPs) of Fe3O4@SiO2@PAMAM@AgNPs {PAMAM: Polyamidoamine} | Significant decrease in water contact angle, slight decrease in WVP. | Significant reduction in UV and visible light transmittance, clear antibacterial activity, increased thermal stability, slight increase in tensile strength (TS) and rigidity (EM), slight decrease in flexibility (EB). | [44] |
10. | Films for applications in food and non-food industries as UV shielding packaging materials | Kappa-carrageenan, xanthan gum, gellan gum and TiO2 | Increased contact angle, decreased moisture content and WVP upon increasing TiO2 content. | Tensile strength, tensile modulus, Tg and thermal stability greatly enhanced. Partial microbial activity against S. aureus and decreased UV light transmittance. The hydrophobic nature of TiO2 agglomerates reduces the integrity of the film structure. | [78] |
11. | Nanocomposite coating on oxygen plasma surface modified polypropylene for food packaging | Kappa-carrageenan, silver nanoparticles and Laponite | Decreased water vapour transmission rate (WVTR). | Increased tensile and adhesion strength of the coated film, reduced OTR, strong antimicrobial activity. | [1] |
12. | Films (Application not specified) | Kappa-carrageenan, gelatin and nano-SiO2 | Decreased water vapour permeability, moisture content, and water solubility. | Film thickness not affected. Significant increase in tensile strength and Young’s modulus. Decreased oxygen permeability and increased turbidity. | [79] |
No. | Form of Composites and End Use Applications | Components | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Films for safe and efficient antibacterial food packaging | Kappa-carrageenan, sodium carboxymethylcellulose and berberine−baicalin nanoparticles (BB NPs) | Significant increase in contact angle (from 99.7 to 117.8°) and slight decrease in WVP (∼7.92 × 10−11 g·m·m−2·Pa−1·s−1, with p > 0.05) (Figure 7). | Superior inhibition of bacterial growth, high ROS generation efficiency, enhanced transparency, UV-blocking performance, strong mechanical strength, thermal stability and oxygen barrier properties. | [80] |
2. | Layer by layer coating for surface modifications in biomedical and food industry applications | Kappa-carrageenan and quercetin-loaded lecithin/chitosan nanoparticles | Oscillative behaviour in contact angles, with higher values on quercetin NP coated layers (~50°) and lower WCA values on carrageenan coated layers (~25°) (Figure 2 in the cited article). | Antioxidant capacity and DPPH radical scavenging activity. Devoid of cell toxicity. | [81] |
3. | Films for active packing in food packing industry | Kappa-carrageenan, (fixed % of) nanoclay (montmorillonite) and (different % of) rosemary extract | Significant reduction in water vapour permeability (5.3 to 2.1 × 10−10 g/m·s·Pa). | Increased tensile strength and elongation at break. More than 99% inhibition against B. cereus, E. coli, P. aeruginosa, and S. aureus. | [37] |
No. | Form of Composites and End Use Applications | Components | Effect on Hydrophilicity of Composites | Effect on Other Properties of Composites | References |
---|---|---|---|---|---|
1. | Films for minced chicken packaging | Semi-refined kappa-carrageenan, sorbitol, ZnO, SiO2 and cassava starch. | WVP decreased from 1.05 to 0.84 × 10−6 g−1·h−1·m−1·Pa−1, WCA increased from 98° to 133° and critical surface tension (CST) increased from 20 to 29 mN·m−1. | Thickness remained more or less the same, tensile strength slightly increased from 28.63 to 32.44 MPa and EAB showed an increasing trend. | [83] |
2. | Films for active packaging applications | Carrageenan, agar, zinc sulphide nanoparticles, and nanocellulose-based tea tree essential oil Pickering emulsion (TPE). | Addition of ZnSNP and TPE, alone or in combination slightly improved the water vapour barrier (WVP reduced from 0.66 to 0.52 × 10−9 g·m/m2·Pa·s) and water resistance of the films (WCA increased from 62 to 67°). | ZnS NPs improved the mechanical strength, whereas PET slightly decreased the strength. However, the combined addition maintained the mechanical strength with slightly improved flexibility and thermal stability. Distinct antioxidant and antibacterial activity. | [52] |
3. | Electrospun nanofibres to use as active layer in food packaging systems | Kappa carrageenan and ZnO NPs/rosemary essential oil (RE)-incorporated zein nanofibres. | Increased surface hydrophobicity (WCA increased from 33.8 to 77.7°) with the addition of ZnO and RE, both separately and together (additive effect). | Enhanced thermal and mechanical properties. Increased cell viability, antimicrobial activity and DPPH scavenging activity. | [56] |
4. | Films for food packaging | Kappa carrageenan, cellulose nanocrystals (CNCs) and organically modified montmorillonite (OMMT). | Significant reduction in water uptake (from ~160 to ~ 85%), both with individual fillers and with their synergistic effect. | Enhanced mechanical properties. | [4] |
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Mavelil-Sam, R.; Ouseph, E.M.; Morreale, M.; Scaffaro, R.; Thomas, S. Recent Developments and Formulations for Hydrophobic Modification of Carrageenan Bionanocomposites. Polymers 2023, 15, 1650. https://doi.org/10.3390/polym15071650
Mavelil-Sam R, Ouseph EM, Morreale M, Scaffaro R, Thomas S. Recent Developments and Formulations for Hydrophobic Modification of Carrageenan Bionanocomposites. Polymers. 2023; 15(7):1650. https://doi.org/10.3390/polym15071650
Chicago/Turabian StyleMavelil-Sam, Rubie, Elizabeth Mariya Ouseph, Marco Morreale, Roberto Scaffaro, and Sabu Thomas. 2023. "Recent Developments and Formulations for Hydrophobic Modification of Carrageenan Bionanocomposites" Polymers 15, no. 7: 1650. https://doi.org/10.3390/polym15071650
APA StyleMavelil-Sam, R., Ouseph, E. M., Morreale, M., Scaffaro, R., & Thomas, S. (2023). Recent Developments and Formulations for Hydrophobic Modification of Carrageenan Bionanocomposites. Polymers, 15(7), 1650. https://doi.org/10.3390/polym15071650