Clays as Inhibitors of Polyurethane Foams’ Flammability
Abstract
:1. Introduction
2. Polyurethanes—Production and Market Size
3. Polyurethanes—Flammability
3.1. General Information
3.2. Flame Retardancy of Polyurethanes
3.2.1. Mechanisms of Action of Flame Retardants
Chemical Mechanism
Physical Mechanism
3.3. Classification of Flame Retardants for Polyurethanes
3.3.1. Nitrogen-Based Flame Retardants
3.3.2. Phosphorus-Based Flame Retardants
3.3.3. Inorganic Flame Retardants
3.3.4. Expandable Graphite
3.3.5. Clays
4. Reduction of Polyurethane Foams’ Flammability by Clays
4.1. Impact on Thermal Decomposition Onset
4.2. Impact on Limiting Oxygen Index
4.3. Impact on the Results of Combustion Tests
4.4. Impact on the Cone Calorimetry Results
5. Clay-Based Coatings for Polyurethane Foams
6. Conclusions
- a better understanding of the synergy effects between clays and flame retardants, especially novel types of halogen-free, and possibly bio-based ones;
- chemical modifications of clays, which would enhance their flame retardancy activity;
- possible applications of clays as precursors for manufacturing of flame retardants and flame-retardant polyols;
- modifications of clays, which, except for the flame retardancy, could provide other properties to foams, e.g., electrical conductivity;
- the flammability of polyurethane/clay composites based on the novel, green raw materials;
- the manufacturing of fully bio-based clay coatings without the use of additional synthetic compounds;
- simplification of the coating process;
- development of multi-purpose coatings, which could combine flame retardancy with other benefits for foams; and
- evaluation of the novel techniques for coating polyurethane foams.
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
Abbreviations
APP | ammonium polyphosphate |
ATH | aluminum hydroxide |
CASE | coatings, adhesives, sealants, and elastomers |
EHC | effective heat of combustion |
HRR | heat-release rate |
LbL | layer-by-layer assembly |
LDH | layered double hydroxide |
LOI | limiting oxygen index |
MDH | magnesium hydroxide |
MMT | montmorillonite |
PA | polyamide |
PAA | poly(acrylic acid) |
PEI | polyethyleneimine |
PET | poly(ethylene terephthalate) |
pHRR | peak value of heat-release rate |
PP | polypropylene |
PUR | polyurethane |
PVC | poly(vinyl chloride) |
SPB | sodium polyborate |
SPR | smoke production rate |
TDI | p-toluyleneisocyanate |
THR | total heat released |
TSR | total smoke released |
VMT | vermiculite |
XRD | X-ray diffraction |
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Combustion Product | Concentration, ppm | Effect on Humans after the Exposition | Ref. |
---|---|---|---|
Carbon oxide, CO | 35 | Headache and dizziness within 6 to 8 h of constant exposure | [64] |
100 | Slight headache in 2 to 3 h | ||
200 | Slight headache within 2 to 3 h; loss of judgment | ||
400 | Frontal headache within 1 to 2 h | ||
800 | Dizziness, nausea, and convulsions within 45 min; insensible within 2 h | ||
1600 | Headache, tachycardia, dizziness, and nausea within 20 min; death in less than 2 h | ||
3200 | Headache, dizziness, and nausea in 5 to 10 min; death within 30 min | ||
6400 | Headache and dizziness in 1 to 2 min; convulsions, respiratory arrest, and death in less than 20 min | ||
12,800 | Unconsciousness after 2–3 breaths; death in less than 3 min | ||
Carbon dioxide, CO2 | <40,000 | Dilatation of cerebral vessels, increased pulmonary ventilation, and increased oxygen delivery to the tissues after 30 min | [65] |
40,000–70,000 | Headache, hearing and visual disturbances, increased blood pressure, dyspnea, difficult breathing, depressions, and tremors | ||
70,000–100,000 | Unconsciousness, headache, visual and hearing dysfunction, depression, shortness of breath, and sweating after few minutes | ||
100,000–150,000 | Unconsciousness, severe muscle twitching, and dizziness after several minutes | ||
>170,000 | Loss of controlled activity, unconsciousness, convulsions, coma, and death within 1 min of initial inhalation | ||
Hydrogen cyanide, nitriles, R-CN | 20–40 | Headache, drowsiness, vertigo, weak and rapid pulse, rapid breathing, bright-red color in the face, nausea, and vomiting | [66] |
100 | Fatal (1 h) | ||
135 | Fatal (30 min) | ||
180 | Fatal (10 min) | ||
270 | Rapidly fatal | ||
Nitrogen oxides, NxOy | 25 | Respiratory irritation, chest pain after 1 h | [67] |
50 | Respiratory irritation, chest pain after 15 min; pulmonary edema possible subacute after 1 h | ||
75 | Pulmonary edema, possible subacute, and chronic lesions in the lungs after 30 min | ||
100 | Pulmonary edema, possible subacute, chronic lesions in the lungs after 15 min; death after 1 h | ||
150 | Pulmonary edema and death after 30 min | ||
200 | Possible subacute and chronic lesions in the lungs after 5 min; pulmonary edema, and death after 15 min | ||
400 | Pulmonary edema and death after 5 min | ||
Ammonia, NH3 | 50 | Irritation to eyes, nose, and throat after 2 h | [68] |
100 | Rapid eye and respiratory tract irritation | ||
250 | Tolerable by most persons (30–60 min exposure) | ||
700 | Immediately irritating to eyes and throat | ||
>1500 | Pulmonary edema, coughing, and laryngospasm | ||
2500–4500 | Fatal (30 min) | ||
5000–10,000 | Rapidly fatal due to airway obstruction | ||
Benzene, C6H6 | 500 | Symptoms of illness after 1 h, slight irritation of mucous membranes | [69] |
1500 | Serious symptoms | ||
3000 | Endurable | ||
7500 | Fatal (1 h), death associated with asphyxiation, respiratory arrest, and central nervous system depression | ||
20,000 | Fatal (5–10 min) |
Foam Type | Clay | Modification of Clay | Flame Retardant | Clay Content, % | ΔTini, °C | Δresidue, % | Ref. |
---|---|---|---|---|---|---|---|
Rigid foams | Bentonite | - | - | 6 | 32 | - | [146] |
9 | 7 | - | [147] | ||||
Cloisite 30B | methyl tallow bis-2-hydroxyethyl ammonium | - | 3 | 16 | - | [147] | |
6 | 35 | - | [146] | ||||
9 | 33 | - | [147] | ||||
aluminium phosphinate, 10% | 5 | 14 | 16.8 | [144,145] | |||
Dellite HPS | - | aluminium phosphinate, 10% | 5 | 13 | 17.0 | ||
[CH3OOCCH2(Ph)2PCH2CH2P(Ph)2CH2COOCH3]Br2 | 5 | 17 | 13.2 | ||||
Halloysite | - | - | 1 | 5 | - | [143] | |
3 | 3 | - | |||||
Laponite RD | - | - | 3 | 14 | - | [147] | |
6 | 39 | - | [146] | ||||
MMT K10 | - | - | 1 | 16 | - | [148] | |
Nanocor | PEG 600 | - | 2 | 25 | 1.0 | [149] | |
PEG 1000 | 2 | 7 | 3.0 | ||||
PEG 1500 | 2 | 20 | 2.0 | ||||
Flexible foams | Cloisite 30B | methyl tallow bis-2-hydroxyethyl ammonium | - | 1 | 44 | 15.0 | [150] |
3 | 53 | 16.0 | |||||
5 | 76 | 26.0 | |||||
1 | 14 | 0.7 | [151] | ||||
2 | 21 | 1.2 | |||||
3 | 24 | 2.0 | |||||
1 | 6 | - | [152] | ||||
3 | 12 | - | |||||
5 | 33 | - | |||||
1 | 45 | 6.0 | [153] | ||||
3 | 49 | 8.0 | |||||
5 | 55 | 11.0 | |||||
Hydro- talcite | - | - | 1.9 | −1 | 1.6 | [154,155] | |
potassium phosphate monobasic | 1.9 | 2 | 1.2 | ||||
Exolit OP560, 5% | 1.9 | 2 | 1.2 | ||||
Exolit OP560, 10% | 1.9 | −7 | 2.7 | ||||
bis(2-ethylhexyl) hydrogen phosphate | - | 1.9 | 4 | 0.3 | |||
Exolit OP560, 5% | 1.9 | 3 | 3.1 | ||||
Exolit OP560, 10% | 1.9 | −8 | 3.1 | ||||
Nanofil 116 | - | Fyrol PNX, 1.5% | 1.5 | 7 | 2.0 | [156] | |
Fyrol PNX, 3.0% | 3 | −19 | 5.0 | ||||
Fyrol PNX | - | 3 | 0 | 1.0 | |||
6 | −1 | 3.0 |
Foam Type | Clay | Modification of Clay | Flame Retardant | Clay Content, % | ΔLOI, % | Ref. | |
---|---|---|---|---|---|---|---|
Rigid foams | Cloisite 30B | methyl tallow bis-2-hydroxyethyl ammonium | - | 3 | 0.9 | [147] | |
9 | 1.6 | ||||||
aluminium phosphinate, 10% | 5 | 5.9 | [144] | ||||
Dellite HPS | - | aluminium phosphinate, 10% | 5 | 5.1 | |||
[CH3OOCCH2(Ph)2PCH2CH2P (Ph)2CH2COOCH3]Br2 | aluminium phosphinate, 10% | 5 | 6.1 | ||||
MMT | octadecyl bis-hydroxyethyl methyl ammonium chloride | ammonium phosphate, 8% | 5 | 6.5 | [163] | ||
dimethyl methyl phosphonate, 8% | 5 | 7.5 | |||||
ammonium phosphate, 8% + dimethyl methyl phosphonate, 8% | 5 | 9.5 | |||||
Na MMT | hexadecyltrimethyl ammonium bromide | - | 2 | 0.4 | [164] | ||
Diethyl bis(2-hydroxyethyl)aminomethylphosphonate | 10% | 2 | 4.1 | ||||
20% | 2 | 8.4 | |||||
30% | 2 | 10.7 | |||||
Nanofil 2 | - | - | 1.2 | 1.7 | [165] | ||
zinc stannate, 1.2% | 1.2 | 2.3 | |||||
zinc stannate, 1.1% + expandable graphite, 2.2% | 1.1 | 3.4 | |||||
zinc stannate, 1.1% + expandable graphite, 6.5% | 1.1 | 5.0 | |||||
Flexible foams | Cloisite 30B | methyl tallow bis-2-hydroxyethyl ammonium | - | 1 | 2 | [152] | |
3 | 7 | ||||||
5 | 9 | ||||||
1 | 5 | [153] | |||||
3 | 7 | ||||||
5 | 10 |
Clay | Modification of Clay | Flame Retardant | Clay Content, % | ΔpHRR, % | ΔTHR, % | ΔTSR, % | Δchar, % | Ref. |
---|---|---|---|---|---|---|---|---|
Cloisite 30B | methyl tallow bis-2-hydroxyethyl ammonium | aluminum tris-diethylphosphinate, 10% | 3 | 40.9 | 30.3 | - | - | [176] |
5 | 35.5 | 27.3 | - | - | ||||
aluminum tris-diethylphosphinate + melamine cyanurate, 10% | 3 | 40.2 | 33.3 | - | - | |||
5 | 44.4 | 27.3 | - | - | ||||
aluminium phosphinate, 10% | 5 | 27.2 | 12.9 | 4.8 | 10.7 | [144] | ||
Dellite HPS | - | aluminium phosphinate, 10% | 5 | 22.1 | 14.2 | 10.5 | 8.7 | |
[CH3OOCCH2(Ph)2PCH2CH2P(Ph)2CH2COOCH3]Br2 | 5 | 35.9 | 18.2 | 4.3 | 5.9 | |||
MMT | - | - | 5 | 0.0 | 3.3 | - | 18.7 | [177,178] |
10 | 3.0 | 11.5 | - | 26.9 | ||||
15 | 0.0 | 24.4 | - | 31.0 | ||||
ammonium polyphosphate + pentaerythritol (2:1 ratio), 5% | 5 | 5.1 | 9.2 | - | 15.8 | |||
ammonium polyphosphate + pentaerythritol (2:1 ratio), 10% | 5 | 17.9 | 29.7 | - | 23.8 | |||
octadecyl bis-hydroxyethyl methyl ammonium chloride | ammonium phosphate, 8% + dimethyl methyl phosphonate, 8% | 5 | 42.5 | - | - | - | [163] | |
- | 5 | 12.4 | - | 1.0 | - | [174] | ||
ammonium polyphosphate, 8% + triphenyl phosphate, 4% | 5 | 33.7 | - | 28.0 | - | |||
octadecyl trimethyl ammonium | - | 0.8 | 15.9 | - | - | - | [173] | |
Na MMT | octadecyl primary ammonium | - | 0.8 | 30.2 | - | - | - | |
decanediamine | 0.8 | 26.4 | - | - | - | |||
hexadecyltrimethyl ammonium bromide | 2 | 19.1 | 6.2 | 5.7 | 6.3 | [164] | ||
Diethyl bis(2-hydroxyethyl)aminomethylphosphonate, 30% | 2 | 50.5 | 43.8 | 16.5 | 20.3 |
Hydrotalcite Modification | Content of Exolit OP560 in Polyol Mixture, % | pHRR, W/g | THR, kJ/g |
---|---|---|---|
Reference foam (no hydrotalcite) | 0 | 144.7 ± 6.5 | 28.2 ± 0.6 |
- | 0 | 136.4 ± 5.5 | 26.9 ± 0.4 |
5 | 132.7 ± 6.5 | 26.1 ± 0.5 | |
10 | 114.7 ± 7.3 | 25.9 ± 0.2 | |
potassium phosphate monobasic | 0 | 138.4 ± 6.5 | 26.5 ± 0.5 |
5 | 136.0 ± 5.5 | 26.2 ± 0.2 | |
10 | 138.8 ± 6.2 | 25.6 ± 0.5 | |
bis(2-ethylhexyl) hydrogen phosphate | 0 | 133.2 ± 11.0 | 27.4 ± 0.8 |
5 | 121.4 ± 6.0 | 26.2 ± 0.5 | |
10 | 131.0 ± 7.4 | 25.9 ± 0.3 |
Type of Coating | Coating Sequence | Content | Coating Mass, % | Nanoparticle Content, % | ΔpHRR, % | ΔTHR, % | |||
---|---|---|---|---|---|---|---|---|---|
PAA | PEI | LDH | MMT | ||||||
Bilayer | PAA/PEI + LDH | 0.2 | 0.2 | 0.5 | - | 25.0 | 54 | 40 | 14 |
PAA/PEI + LDH | 1.0 | - | 30.0 | 58 | 39 | 19 | |||
PAA + MMT/PEI | - | 0.5 | 11.0 | 32 | 22 | 0 | |||
PAA + MMT/PEI + LDH | 0.5 | 0.5 | 11.0 | 32 | 27 | 7 | |||
Trilayer | PAA/PEI + LDH/MMT | 0.5 | 0.5 | 11.0 | 43 | 28 | 9 | ||
PAA/PEI + LDH/MMT | 1.0 | 1.0 | 7.5 | 64 | 29 | 16 | |||
Quadlayer | PAA/LDH/PEI/MMT | 0.5 | 0.5 | 13.0 | 29 | 33 | 5 | ||
PAA/LDH/PEI/MMT | 1.0 | 1.0 | 8.4 | 56 | 31 | 21 |
Coating and Number of Bilayers | ΔpHRR, % | ΔTHR, % | Δresidue, % | ΔTSR, % |
---|---|---|---|---|
MMT 1 | 27.8 | 4.1 | 6.0 | −7.5 |
MMT 2 | 53.3 | 1.5 | 4.0 | 11.0 |
MMT 4 | 59.5 | 11.8 | 8.0 | 50.7 |
VMT 1 | 53.9 | 8.2 | 13.0 | 30.8 |
VMT 2 | 56.2 | 12.3 | 11.0 | 58.2 |
Starch Content, wt% | SPB Content, wt% | MMT Content, wt% | ΔpHRR, % | Open-Flame Test Results |
---|---|---|---|---|
1.5 | 5.8 | - | 42 | Self-extinguished < 40 s |
5.8 | 2.0 | 60 | Self-extinguished < 20 s | |
11.5 | - | 64 | Self-extinguished < 20 s | |
11.5 | 2.0 | 66 | No ignition | |
3.0 | 5.8 | - | 53 | Self-extinguished < 20 s |
5.8 | 2.0 | 63 | Self-extinguished < 20 s | |
11.5 | - | 66 | No ignition | |
11.5 | 2.0 | 66 | No ignition | |
23.0 | - | 75 | No ignition |
Number of Bilayers | Sepiolite Content, wt% | ΔpHRR, % | ΔTHR, % | ΔSPR, % | ΔTSR, % |
---|---|---|---|---|---|
3 | 0.0 | 25.4 | 4.9 | 33.3 | 9.8 |
6 | 39.4 | 12.9 | 41.7 | 19.5 | |
3 | 0.5 | 60.6 | 14.4 | 58.3 | 22.0 |
6 | 70.4 | 19.3 | 58.3 | 29.3 | |
3 | 1.0 | 76.1 | 24.2 | 58.3 | 24.4 |
6 | 76.1 | 23.9 | 58.3 | 26.8 |
Alginate (A) and Clay (C) Content, wt% | Coating Thickness, mm | ΔpHRR, % | ΔTHR, % | ΔTSR, % | Δresidue, % |
---|---|---|---|---|---|
A5C5 | 1.5 | 55.4 | −5 | 39.2 | 14.7 |
A5C10 | 1.5 | 65.9 | 20 | 62.0 | 43.6 |
A7.5C7.5 | 0.2 | 31.0 | 5 | 46.5 | 9.3 |
0.7 | 31.9 | 5 | 36.9 | 19.6 | |
1.5 | 60.4 | 5 | 46.3 | 33.9 |
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Hejna, A. Clays as Inhibitors of Polyurethane Foams’ Flammability. Materials 2021, 14, 4826. https://doi.org/10.3390/ma14174826
Hejna A. Clays as Inhibitors of Polyurethane Foams’ Flammability. Materials. 2021; 14(17):4826. https://doi.org/10.3390/ma14174826
Chicago/Turabian StyleHejna, Aleksander. 2021. "Clays as Inhibitors of Polyurethane Foams’ Flammability" Materials 14, no. 17: 4826. https://doi.org/10.3390/ma14174826