Cutting-edge green nanoclay nanocomposites—fundamentals and technological opportunities for packaging, dye removal, and biomedical sectors

Figures & data

Figure 1. (A) Structure of montmorillonite nanoclay [178]. (Source: Reproduced with permission from Springer.) (B) Transmission electron microscopy images of nanoclay modified isoprene latexes with 5 wt.% nanoclay; (C) 10 wt.% nanoclay; and (D) film formation of the natural rubber/nanoclay modified polyisoprene (NR/Clay-PIP) nanocomposite [68]. NR: natural rubber; PIP: polyisoprene. Source: Reproduced with permission from MDPI.

Figure 2. (A) Chemical structures of (a) PLA, (b) Joncryl, and (c) modified of Cloisite® 20 A; (B) curve fitting between experimental and FEA generated stress–strain curves of PLA and PLA/MMT [75]; (C) DSC thermograms, first heating scan of PLA based nanobiocomposite films after different composting times [76]; and (D) water contact angle for neat PLA and the PLA based biocomposites [77]. DSC: differential scanning calorimetry; FEA: finite element analysis; FEA PLA: finite element analysis derived poly(lactic acid); FEA PLA/MMT: finite element analysis derived poly(lactic acid)/montmorillonite; PLA: poly(lactic acid); PLA/CO: poly(lactic acid)/coconut oil; PLA/CO/S: poly(lactic acid)/coconut oil/sage; PLA/CO/S/1.31 PS: poly(lactic acid)/coconut oil/sage/sage coconut oil nanoclay; PLA/S: poly(lactic acid)/sage; WCA: water contact angle. Source: Reproduced with permission from MDPI.

Figure 3. (A) Scheme of coating application on paper surface with a Mayer bar. The WVTR of PVA and PVA gel coated paper at different temperatures and humidity: (B) 23 °C, 50% RH and (C) 38 °C, 90% RH [89]. PVA: poly(vinyl alcohol); PVA/NC: poly(vinyl alcohol)/nanoclay; RH: relative humidity; WVTR: water vapor transmission rates. Source: Reproduced with permission from MDPI.

Figure 4. (A) FE-SEM images of (a) the base paper, (b) PVA/AKD-S coated paper, (c) PVA/AKD/5% nanoclay-S coated paper, (d) PVA/AKD-D coated paper, and (e) PVA/AKD/5% nanoclay-D coated paper. (B) WVTR of papers; (C) WCA of the base paper and coated papers; and (D) elongations at break and tensile strengths of the base paper and coated papers [90]. BP: base paper; D: double coating; FE-SEM: field emission electron microscopy; PVA/AKD: poly(vinyl alcohol)/alkyl ketene dimer; S: single coating; WCA: water contact angle; WVTR: water vapor transmission rates. Source: Reproduced with permission from MDPI.

Figure 5. (A) Schematic of transparent NFC monolayer/nanoclay nanoplatelet based hybrid films with self-extinguishing behavior (90% transparency at 600 nm). One-dimensional nanofibrillated cellulose was extracted from wood pulp through mechanical and chemical treatments and mixed with disperse nanoclay nanoplatelets uniformly in water. The nanofibrillated cellulose dispersed monolayer nanoclay nanoplatelets suspension was blended with 0.5 wt.% nanoclay nanoplatelet suspension using mechanical stirring and ultra-sonication methods [97]. (Source: Reproduced with permission from ACS.) (B) Mechanism of MMT stacking and arrangement of stacks in nanocellulose network: (a) MMT stack formation at high loading level which decrease the tortuous paths and (b) MMT stacks broken down using high pressure homogenization of nanocellulose/MMT suspension which increase the tortuous path [112]. (Source: Reproduced with permission from Elsevier.) (C) WVP of nanocellulose/MMT nanocomposites. The pristine nanocomposite sheets; nanocomposite sheets with high pressure homogenization step, and sonication step [112]. (Source: Reproduced with permission from Elsevier.) (D) WVTR of PLA and its nanocomposites regarding the nanoclay contents and normalized to 25 µm [113]. (Source: Reproduced with permission from MDPI.) (E) The adsorption efficiency of C20A, C20AM, and PLAC20AM 5% (methylene blue dye concentration = 200 mg/L, nanocomposite content = 20 mg/20 mL, T = 25 °C and 60 min) [123]. (F) The removal efficiency of MB for 48 h in the presence of electrospun CA and of CA/NC1, CA/NC2, and CA/NC3 nanocomposites [124]. C20 A: Cloisite 20 A; C20AM: Cloisite 20 A with 1,4-diaminobutane dihydrochloride; CA: cellulose acetate; CA/NC: cellulose acetate/nanoclay; MB: methylene blue; MMT: montmorillonite; NFC: nanofibrillated cellulose; PLA: poly(lactic acid); PLAC20AM: poly(lactic acid)/Cloisite 20 A/methylene blue; WVP: water vapor permeability; WVTR: water vapor transportation. Source: Reproduced with permission from MDPI.

Figure 6. (A) Geometries of the lowest energy conformers of CV and TB optimized at the DFT/B3LYP/6-31G(d) level of theory; (B) (a) Front view and (b) side view of Na-MNC supercell lattice. ; (C) Equilibrium configurations of adsorption of TB onto MNC from NVT molecular dynamics for: (a) 33%; (b) 66%; and (c) 100% of surface loading rate. Polyhedron style was used to represent the Na-MNC for the top view [102]. CV: crystal violet; MNC: montmorillonite nanoclay; NVT: canonical ensemble; TB: toluidine blue. Source: Reproduced with permission from Elsevier.

Figure 7. (A) Schematic node normal and tangential stresses and displacements in CZM-based FEM modeling of debonding process of clay nanoparticles in PNCs. (B) Schematic σ_n–δ_n and σ_t–δ_t relations of a bilinear CZM. (C) RVE of a PNC reinforced with aligned, identical clay nanoparticles in a stack distribution configuration: (a) idealized identical stacking clay platelets; (b) a typical RVE; and (c) a quarter RVE for efficient simulation; and (D) von Mises stress and displacement fields of RVE of a PNC reinforced with a rectangle-shaped clay nanoparticle: (a) crack initiates; (b) crack propagates; and (c) crack propagates at final failure [103]. CZM: cohesive zone model; FEM: finite element analysis; PNCs: polymer nanoclay composites; RVE: representative volume element. Source: Reproduced with permission from MDPI.

Figure 8. (A) 0 wt.% MMT; (B) 10 wt.% MMT morphology of crosslinked PVA electrospun nanocomposite mats with different contents of nanoclay; (C) BSA delivery from PVA electrospun mats for different contents of nanoclay: 0 wt.% (circle), 2 wt.% (square), 10 wt.% (triangle), and 40 wt.% MMT (diamond) [128]; (D) Dissolution profiles of 500 mg theophylline granules 30–35 mesh, 20 wt.% theophylline) in 900 mL phosphate buffer pH 6.8 using USP apparatus II at 75 RPM (n = 3), Cloisite Na nanocomposites of different nanoclay loadings [130]. BSA: bovine serum albumin; MMT: montmorillonite; PVA: poly(vinyl alcohol). Source: Reproduced with permission from MDPI.

Figure 9. (A) Schematic representation of film structures with various clay concentrations; (B) SEM microphotograph of chitosan PEG nanoclay; and (C) TGA curves of CS/PEG films with various amounts of Lap [132]. CS/PEG: chitosan/poly(ethylene glycol); PEG: poly(ethylene glycol); SEM: scanning electron microscopy; TGA: thermogravimetric analysis; C1, C3, C5 = 0%, 1%, and 1.5% nanoclay. Source: Reproduced with permission from MDPI.

Table 1. Green nanoclay filled nanocomposite based systems for technical applications.

Polymer	Nanofiller	Processing	Property/application	Ref
Natural rubber	Organically modified Cloisite nanoclay	Melt blending technique	Strength and modulus increase	[65]
Natural rubber	Octadecylamine modified sodium montmorillonite	Solution	Dispersion, exfoliation, interaction	[67]
Natural rubber; polyisoprene	Montmorillonite modified polyisoprene	Vulcanization	Homogeneous dispersion; ion exchange mechanism	[68]
Poly(lactic acid)	Cloisite	Solution/intercalation technique	Antibacterial properties for gram-negative/gram-positive bacteria	[72]
Poly(lactic acid)	Montmorillonite	Melt extrusion method	Dielectric properties 26–40 GHz	[73]
Poly(lactic acid); starch	Montmorillonite	3D printing; injection molding	Interfacial adhesion; tensile strength 10–20 MPa	[74]
Poly(lactic acid)	Cloisite® 20 A	Solution	Finite element analysis; stress–strain	[75]
Poly(lactic acid)	Thymol; montmorillonite	Melt method	Multiple endothermic peaks due to enthalpic relaxation	[76]
Poly(lactic acid)	Montmorillonite	Melt method	Water contact angle 97°; hydrophobicity	[77]
Poly(lactic acid)	Montmorillonite	Laser sintering technique	Flexural modulus 41% increase	[78]
Poly(lactic acid)	Ammonium salt of L-isoleucine amino acid modified cloisite Na^+	Solution intercalation	Dispersion	[59]
Poly(lactic acid)	Sodium modified montmorillonite	Intercalation	Photochemical properties	[85]
Poly(lactic acid)	Montmorillonite	Solution casting	Heat stability 200 h on UV irradiation	[86]
Poly(vinyl alcohol)/corn starch	Montmorillonite	Melt	Strength, barrier, heat transport	[87]
Poly(lactic acid)	Montmorillonite-Na^+	Solution route	Pervaporation/separation efficiency; water/ethanol mixture	[88]
Poly(lactic acid); Cellulose	Montmorillonite	Sonication; coating	Water vapor transmission at 23 °C and 38 °C for 50% and 90% RH, respectively; water vapor transmission rate 512–1861 g/m^2.day; contact angle 108°; hydrophobicity > 90°	[89]
Poly(vinyl alcohol); alkyl ketene dimer	Cloisite Na	Buckypaper method	Water vapor transmission rate 533 g/m^2.day	[90]
Nanofibrillated cellulose	Montmorillonite	Mechanical stirring; ultra-sonication techniques	Non-flammability effects; self-extinguishing	[97]
Cellulose; triethyl citrate plasticizer	Gelatin functionalized montmorillonite	Solution	Non-flammability	[98]
Poly(lactic acid); triacetin plasticizer	Cloisite nanoclay	Solution	Water vapor permeability 1.06 × 10^–10 g/m.s Pa. In	[108]
Nanocellulose	Montmorillonite 16.7–23.1 wt.%	Solution method	Low water vapor permeability 6.3–13.3 g.μm/m^2.day.kPa; Packaging	[112]
Nanocellulose nanofiber	Vermiculite nanoclay	Solution method	Oxygen permeability 0.07 cm^3μm/m^2.day.kPa at 50% relative humidity; packaging	[109]
Cellulose	Montmorillonite	Solution method	Low water vapor transmission rate 43 g/m^2.day; packaging	[110]
Poly(ethylene glycol)	Montmorillonite; hexadecyltrimethylammonium bromide surfactant	Solution method	Methylene blue and trypan blue with adsorption capacities 237.22 and 190.81 mg/g, respectively; antimicrobial effects E. coli/M. luteus bacteria	[122]
Poly(lactic acid)	1,4-diaminobutane dihydrochloride modified Cloisite 20 A	Solution	Methylene blue dye; dye absorption efficiency 91%–97 % (1 h)	[123]
Cellulose acetate	Cloisite 20 A	Electrospinning	Methylene blue dye removal efficiency 34%	[124]
Poly-(DL-lactic acid)	Laponite	Solution method	Drug delivery; Type-2 diabetes curation	[129]
Poly(vinyl alcohol)	Montmorillonite	Electrospinning	20%–40 % nanoclay; normalized delivery time 7 days	[128]
Eudragit® RS	Cloisite 20	Melt extrusion	Drug delivery theophylline	[130]
Chitosan, poly(ethylene glycol)	Laponite® nanoclay	Solution	Water diffusion mechanism; support materials for drug release	[132]
Poly(lactic acid)	Halloysite nanoclay	Gentamicin; solution	Bone regeneration	[142]
Poly(ɛ-caprolactone)	Montmorillonite	Electrospinning	Tissue engineering; better cell adhesion and bioactivity	[143]
Poly(vinyl alcohol)	Montmorillonite	Solution method	Wound healing; penicillin drug to wounds	[146]
Poly(vinyl alcohol)	Montmorillonite	Solution method	Wound healing; high microbiological stability	[147]
Wood	Montmorillonite	Solution/melt method	Sustainable construction materials	[174]
Cellulose, starch, poly(lactic acid)	Montmorillonite	Solution/melt method	Packaging	[105,106,175]
Chitosan	Montmorillonite	Solution method	Rhodamin-6 dye adsorption capacity 446.43 mg/g	[176]
Poly(epicholorohydrin-dimethylamine)	Bentonite nanoclay	Solution	Dye adsorption capacity 13–31 mg/g	[177]

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