Progress in Biodegradable Flame Retardant Nano-Biocomposites
Abstract
:1. Introduction
2. Biodegradability of Biocomposites
- Disintegration—namely fragmentation and loss of visibility of the compostable material in the finished compost. It is measured in a pilot composting test (EN 14045) in which specimens of the test material are composted with biowaste for 3 months. After this time, the mass of test material residues has to amount to less than 10% of the original mass.
- Biodegradability—namely the capability of the compostable material to be converted into CO2 under the action of microorganisms. The standard contains a mandatory threshold of at least 90% biodegradation that must be reached in less than 6 months (laboratory test method EN 14046) [96].
- Ecotoxicity—the amount of heavy metals has to be below given maximum values. The final compost must not be affected negatively (no reduction of agronomic value and no ecotoxicological effects on plant growth)
- Absence of negative effects on the composting process.
Biodegradation Mechanism
3. Flame Retardant Chemistry
3.1. Nanofillers Classification and Chemistry
3.2. FR Nanofillers
3.2.1. Clay Based Nano FRs
3.2.2. Layered Double Hydroxides
3.2.3. Carbon Based Nano FRs
3.2.4. Metal Oxides
3.2.5. Other Flame Retandant Nanofillers
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Biobased Polymer | Description |
---|---|
PLA (Polylactide) | Renewable, biocompatible and biodegradable polymer. Obtained by ring opening polymerization of lactide or by direct polycondensation of lactic acid. Its thermal stability and impact resistance are inferior to those of conventional polymers used for thermoplastic applications. PLA matrix is used to improve the composite stiffness, permeability, crystallinity, and thermal stability. Targeted markets include packaging, textiles and biomedical applications. |
PHA (Polyhydroxyalkanoates) | Renewable, biocompatible and biodegradable polyesters synthesized by microorganisms from various carbon sources. They are very sensitive to temperature and shear. Additives, blends and natural fibre reinforced composites are capable of overcoming negative drawbacks of individual components. |
STARCH | Bioplastic composed of both linear and branched polysaccharides (amylose and amylopectin). Thermoplastic starch (TPS) can be obtained from starch by disrupting its molecular interactions, using plasticizers and/or complex operations as devolatilization, melt-melt mixing and morphology control. Extreme moisture sensitivity of starch leads to limited practical application. Therefore, blending of TPS with other less sensitive polymers and additives is required. |
CELLULOSE | Renewable, biocompatible and biodegradable polymers obtained from wood, cotton or extracted from agricultural byproducts such as bagasse, stalks and cropstraws. Cellulose based materials are used in two forms on an industrial scale—Regenerated cellulose used for fibre and film production and Cellulose esters used in coatings, biomedical uses and other usual plastic applications. |
CHITIN & CHITOSAN | They are renewable, biocompatible and biodegradable polymers with excellent adsorption properties. Chitin is a natural polysaccharide used as a supporting material in many invertebrate animals such as insects and crustaceans. The deacetylated chitin is known as chitosan. Chitosan has been explored for films and fibres and has generated great interest and usage for biomedical applications. |
PROTEINS | They are biodegradable polymers based on renewable sources obtained from original proteins which can be classified as plant and animal proteins. Water, glycerols, fatty acids and oils are commonly used plasticizers for proteins. Wet and dry processing methods are used to obtain biomaterials from proteins. Such biomaterials are used in food and pharmaceutical applications, as well as in tissue engineering applications. |
BIO-PBS (Bio-Polybutylene succinate) | Renewable, biodegradable and even compostable material obtained by direct polymerization of biobased succinic acid and 1,4-butanediol. This material is mainly used for product containers and packaging since it is food-contact approved. |
PBAT/PLA (Poly(butylene adipate-co-terephtalate) | Polybutyrate is a biodegradable and compostable biopolymer with properties similar to low density polyethylene (LDPE). PBAT bioplastic is made from fossil resources. Its compounds (starch, PLA) have a biobased carbon content of up to 30%. Typical application is for flexible film for packaging, e.g., compostable shopping bags. |
Plant Fibre | Matrix | Source |
---|---|---|
Flax | Starch, PBT, PP, PLA | [24,25,26,27,28,29,30] |
Hemp | Epoxy, PBS, PP | [31,32,33,34,35] |
Jute | Epoxy, PP, PLA | [36,37,38,39,40,41,42] |
Kenaf | PLA, PET, PP | [43,44,45,46,47,48,49] |
Ramie | PCL, PBS, PP, Starch, Epoxy | [50,51,52,53,54,55] |
Spanish Broom | PLA, PP | [56,57,58] |
Sisal | Bioepoxy, PES, | [45,59,60,61,62,63] |
Coir | PLA, starch, Epoxy, PP, PE | [64,65,66,67,68,69] |
Banana | PVA, PP, Epoxy, PU | [70,71,72,73,74,75,76] |
Bamboo | Starch, PLA, Epoxy | [60,77,78,79,80,81,82] |
Miscanthus Giganteus | PP, PLA, PBS/PBAT | [83,84,85,86,87] |
Plate Like (1D) | Nanofibres/Nanowhiskers (2D) | Nanoparticles (3D) |
---|---|---|
• Layered Silicates (Montmorilonite-MMT, Hectorite, Saponite) | • Carbon Nanotubes (Single-walled and Multi-walled) | • Silica Particles (SiO2) |
• Layered Double HydroxIdes—LDHs | • Cellulose Nanofibrils | • Metal Oxides (TiO2, Al2O3, MgO, ZnO, Fe2O3, Fe3O4) |
• Graphene Nano Sheets/ExPanded Graphite | • Cellulose Nanocrystals | • Metal Hydroxides (Nanomagnesium Hydroxide) |
• Layered MoS2 Nano Sheets | • Bacterial Cellulose | • Metal Nanoparticles (Ag, Au, Cu, Fe) |
• Layerd Nano α-Zirconium Phosphate | • Sepiolite Nano Rods | • Polyhedral Oligomeric Silsesquioxane (POSS) |
• Pseudo-Boehmit (AlOOH) | • Halloysite Nanotubes | • Fullerene |
• Black Phosphorus | • Gold or Silver Nanotubes | • Carbon Black |
• MXenes Nano Sheets (Matal Carbides and/or Carbonitrides) | • Wormlike Rubber | • Spherical Nano Rubber |
• Hexagonal Boron Nitride | • Boron Nitride Nanotubes | • Quantum Dots |
Matrix/Reinforcement | FR Agent | Loading | Flammability | References Year |
---|---|---|---|---|
PLA | Two Organo-modified Layered Silicates (OMLS) | 3% | PHRR 42% ↓ | [143] 2010 |
PLA/Hemp | • Sepiolite Nanoclay • MWCNT | 10% 2% | PHRR 45% ↓ | [144] 2010 |
PU | • Chitosan • MMT Nano Clay | 0.1% 1% | PHRR 52% ↓ | [145] 2012 |
PLA/Spanish Broom | • MMT Nano Clay | 5% | THR 13.5% ↓ | [56] 2015 |
PP/Kenaf | • Halloysite Nano-tubes (HNTs) • Montmorillonite (MMT) Nanoclay | 3% 3% | THR 20% ↓ | [146] 2016 |
PLA | • Nano Fibrous Sepiolite SEP-DOPO | 10% | UL-94 V-0 | [147] 2019 |
PLA/Flax | • Sepiolite nNnorods • Chitosan • APP | 1% 0.5% 1% | PHRR 33% ↓ | [24] 2020 |
PP | • Nano Kaolin | 1.5% | LOI 35.5% | [148] 2020 |
Matrix/Reinforcement | FR Agent | Loading | Flammability | References Year |
---|---|---|---|---|
PHB | • Organically Modified LDH Sodium Stearate | 5% | THR 13.2% ↓ | [153] 2012 |
Epoxy | • Eugenol Derivative Based LDH | 8% | UL-94 V-0 | [154] 2014 |
Cotton | • Mg–Al Nano-LDH | 1.5% | LOI 20.8% | [155] 2016 |
Cotton | • Inorganic Hydrotalcite Nanoparticles (HT) | 0.1% | THR 27% ↓ | [156] 2017 |
Bamboo | • MgAl-LDH | 5% | THR 33.3% ↓ | [157] 2019 |
Silicon Rubber SR/PBS | • Mg4.5Al2(OH)3(CO3)6⋅5H2O (LDH) | 5% | PHRR 54.4% ↓ | [158] 2019 |
PP | • Sodium Alginates LDH (SA@LDHs) | 30% | UL-94 V-0 | [159] 2020 |
Leather | • LDH/Zanthoxylum Bungeanum Seed Oil | 10% | LOI 28.3% | [160] 2020 |
Matrix/Reinforcement | FR Agent | Loading | Flammability | References Year |
---|---|---|---|---|
PP/Flax | • Expandable Graphite (EG) | 25% | LOI 30% | [167] 2003 |
PLA | • Sepiolite Nanorods • Multiwalled Carbon Nanotubes (MWNT) | 10% 2% | PHRR 45% ↓ | [144] 2010 |
PP/Carbon fibre | • Carbon Black | 5% | THR 16% ↓ | [168] 2015 |
Polyimide PI | • Graphene Oxide Nanosheet (GO) • MMT | 5% 10% | LOI 55% | [169] 2017 |
Epoxy/Fruit fibres | • EG | 7% | THR 25.5% ↓ | [170] 2017 |
PU | • Chitosan • GO | 0.5% 1% | THR 13% ↓ | [171] 2019 |
Epoxy/Curaua | • GO | 0.1% | DTA Increase in Thermal Stability | [172] 2019 |
cotton | • Polyamidoamines Containing Disulphide Groups (SS-PAA) • Nano GO | 12% 1% | PHRR 53% ↓ | [173] 2019 |
ABS | • Mo5/PN-rGO | 1% | THR 20% ↓ Total Smoke Production (TSP) 45% ↓ | [174] 2020 |
Hydroxyethyl Cellulose (HEC) + Lactic Acid (LA) + PU | • Graphene Nanoplatelets (GNPs) | 0.3% | TGA Enhancement in Thermal Stability by Nearly 15–20 °C With a Weight Loss of 50%. | [175] 2020 |
Elium® 150 Thermoplastic Resin | • EG • Alumina Trihydrate (ATH) | 4–10% 10–30% | UL-94 V-0 | [50] 2020 |
PLA | • Carbon Nanotubes (CNTs) • CaMg-Ph | 1% 19% | PHRR 35% ↓ | [176] 2020 |
Cotton | • Phytic acid • Biochar | 8% 8% | No Ignition | [177] 2020 |
Matrix/ Reinforcement | FR Agent | Loading | Flammability | References Year |
---|---|---|---|---|
PMMA | • TiO2 • Fe2O3 • OMMT (Cloisite 15A) | 10% 10% 10% | PHRR 29% ↓ | [190] 2005 |
Kenaf/PHBV/ PBAT | • Exolit OP 1240 • Antimony Oxide NPs Sb2O3 | 8% 2% | PHRR 47% ↓ | [188] 2013 |
Unsaturated Polyester PES | • Exolit OP 1240 • Nano Al2O3 | 10–15% 2.5% | UL-94 V-1 | [191] 2015 |
Sisal | • Nano ZnO | 1% | LOI 34% | [185] 2017 |
Jute | • Nano ZnO • Polyhydroxymethyl Amino Silicone (PHAMS) | 0.01% 10% | LOI 35% | [187] 2017 |
Cotton | • Nano-TiO2@DNA | 3% | Do Not Ignite | [192] 2019 |
HDPE | • Cellulose Nano Crystals + ZnO NPs | 0.4% | PHRR 18% ↓ | [193] 2019 |
Zinc Alginate (ZnAlg) | • Nano-cuprous Oxide (Cu2O) | / | LOI 58% | [194] 2019 |
Epoxy +PA | • Intumescent Fire-retardant (APP+pentaerythritol+Melamine) • Clamshells CS Bio Filler • Nano TiO2 | 52% 3% 1% | Smoke Density Rating (SDR) 37.5% ↓ | [195] 2020 |
Cotton | • pentaerythritol phosphate Urea Salt (PEPAS) • 2-(4-(4,6-dichloro- 1,3,5-triazin-2-ylamino) phe- nylsulfonyl) ethyl sulphate sodium (CYPA) • nano-SiO2 | 300 g/L 125g/L / | LOI 31.8% | [189] 2020 |
Wood | • chitosan/sodium phytate/TiO2-ZnO nanoparticle | 1% | LOI 32.8% | [196] 2020 |
Legislation principles of greener flame retardance |
not PBT (Persistent, Bio-accumulating, Toxic) |
not POPs (Persistent Organic Pollutant) |
REACH/CLP: No/Few Hazard (H) or Risk (R) |
not CMR (Carcinogenic, Mutagenic, Toxic to Reproduction) |
not EDC (Endocrine Disrupting) |
Matrix/ Reinforcement | FR Agent | Loading | Flammability | References Year |
---|---|---|---|---|
Waste PP +Kenaf | • Nano CaCO3 • Sodium polyphosphate (NaPP) | 7% 13% | PHRR 18% ↓ | [199] 2012 |
PP PA PE | • Cyclodextrin Nanosponges | 10% | THR 11% ↓ | [208] 2012 |
Cotton | • POSS | 20 bilayers (BLs) | PHRR 20%↓ | [136,209] 2015 |
PP | • POSS • Intumescent Flame Retardant | 0.5% 19.5% | UL 94 V-0 LOI 29.9% | [205] 2018 |
Epoxy/Kenaf | • Nano Oil Palm Empty Fruit Bunch (OPEFB) Filler | 3% | LOI 30% | [210] 2019 |
PLA | • Lignin Nanoparticles diethyl (2-(triethoxysilyl) ethyl) phosphonate (SiP) | 5% | PHRR 11% ↓ | [203] 2019 |
PLA/Flax | • Nano hydroxyapatite Ca10(PO4)6 (OH)2 | 40% | UL-94 V-1 | [207] 2019 |
PLA | • Nanoplate-like Hydroxyapatite (HA) | 10% | TGA Improved Thermal Sstability | [206] 2020 |
epoxy | • Chicken Feather Nano HA From Conch Shells | 15% 3% | HRC Heat Release Capacity 36% ↓ | [211] 2020 |
PU | • HA • Sodium Alginate (SA) • Chitosan (CH) | 1% 0.5% 0.5% | PHRR 77.7% ↓ | [212] 2020 |
PAN | • Tannic Acid-MoS2 Nanosheets | 2% | PHRR 38.1% ↓ | [213] 2020 |
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Kovačević, Z.; Flinčec Grgac, S.; Bischof, S. Progress in Biodegradable Flame Retardant Nano-Biocomposites. Polymers 2021, 13, 741. https://doi.org/10.3390/polym13050741
Kovačević Z, Flinčec Grgac S, Bischof S. Progress in Biodegradable Flame Retardant Nano-Biocomposites. Polymers. 2021; 13(5):741. https://doi.org/10.3390/polym13050741
Chicago/Turabian StyleKovačević, Zorana, Sandra Flinčec Grgac, and Sandra Bischof. 2021. "Progress in Biodegradable Flame Retardant Nano-Biocomposites" Polymers 13, no. 5: 741. https://doi.org/10.3390/polym13050741