Intercalation of Sulfanilic Acid‐Phenol‐Formaldehyde Polycondensate into Hydrocalumite Type Layered Double ­Hydroxide

Polycondensates containing sulfonate groups, referred to as concrete superplasticizers, are widely used in the construction industry. A sulfanilic acid–phenol–formaldehyde polycondensate (SPF) with M_w ≈ 100.000 g · mol^–1 was synthesized from sulfanilic acid, phenol and formaldehyde by polycondensation reaction, and its intercalation into hydrocalumite type Layered Double Hydroxide (LDH) was investigated. Preparation was done by rehydration of tricalcium aluminate, a cement constituent, in the presence of the polymer. According to the XRD pattern, SPF was successfully intercalated. A d value of approx. 2.6 nm was found. Elemental composition of the new organo‐mineral phase reveals charge balancing of the cationic LDH main layers by the polycondensate. Thermogravimetry indicates that thermal degradation of intercalated SPF occurs at higher temperature, compared to non‐intercalated SPF. According to SEM imaging, the novel Ca‐Al‐LDH phase exhibits the morphology of intergrown platelets. Ultra‐thin nanosheets (foils) with approx. 50 nm thickness were obtained. The layered structure and d value obtained from diffraction analysis were confirmed by TEM imaging. The new hydride can be used as cement and concrete additive.     

Facile Fabrication of Highly‐Dispersed Nickel Nanoparticles with Largely Enhanced Electrocatalytic Activity

Supported nickel nanoparticles with high dispersion have been prepared by partial reduction of NiAl‐layered double hydroxide (NiAl‐LDH) precursors, which exhibit significant electrocatalytic behavior towards glucose. XRD and XPS results confirm that the nickel nanoparticles are successfully synthesized. TEM images reveal that the nickel nanoparticles are highly dispersed in the NiAl‐LDH matrix with a size of 6±0.3 nm. The resulting nanocomposite modified electrode displays significant electrocatalytic performance to glucose with a broad linear response range (8.0×10^?5–2.0×10^?3 M), low detection limit (3.6 µM), high sensitivity (339.2 µA/mM), selectivity and excellent reproducibility as well as repeatability.     

Reverse Micelle Synthesis of Colloidal Nickel–Manganese Layered Double Hydroxide Nanosheets and Their Pseudocapacitive Properties

Colloidal nanosheets of nickel–manganese layered double hydroxides (LDHs) have been synthesized in high yields through a facile reverse micelle method with xylene as an oil phase and oleylamine as a surfactant. Electron microscopy studies of the product revealed the formation of colloidal nanoplatelets with sizes of 50–150 nm, and X‐ray diffraction, energy dispersive X‐ray spectroscopy, and X‐ray photoelectron spectroscopy studies showed that the Ni–Mn LDH nanosheets had a hydrotalcite‐like structure with a formula of [Ni₃Mn(OH)₈](Cl^?) ? n H₂O. We found that the presence of both Ni and Mn precursors was required for the growth of Ni‐Mn LDH nanosheets. As pseudocapacitors, the Ni–Mn LDH nanosheets exhibited much higher specific capacitance than unitary nickel hydroxides and manganese oxides.     

Few‐Layer Nanosheets of n‐Type SnSe2

Layered p‐block metal chalcogenides are renowned for thermoelectric energy conversion due to their low thermal conductivity caused by bonding asymmetry and anharmonicity. Recently, single crystalline layered SnSe has created sensation in thermoelectrics due to its ultralow thermal conductivity and high thermoelectric figure of merit. Tin diselenide (SnSe₂), an additional layered compound belonging to the Sn‐Se phase diagram, possesses a CdI₂‐type structure. However, synthesis of pure‐phase bulk SnSe₂ by a conventional solid‐state route is still remains challenging. A simple solution‐based low‐temperature synthesis is presented of ultrathin (3–5 nm) few layers (4–6 layers) nanosheets of Cl‐doped SnSe₂, which possess n‐type carrier concentration of 2×10¹⁸ cm^?3 with carrier mobility of about 30 cm² V^?1 s^?1 at room temperature. SnSe₂ has a band gap of about 1.6 eV and semiconducting electronic transport in the 300–630 K range. An ultralow thermal conductivity of about 0.67 Wm^?1 K^?1 was achieved at room temperature in a hot‐pressed dense pellet of Cl‐doped SnSe₂ nanosheets due to the anisotropic layered structure, which gives rise to effective phonon scattering.     

Synthesis and Characterization of PE-g-MA／MgAI-LDH Exfoliation Nanocomposite via Solution Intercalation

An organo‐modified MgAl‐layered double hydroxide (OMgAl‐LDH) was successfully exfoliated in the xylene solution of polyethylene‐grafted‐maleic anhydride (PE‐g‐MA) under re‐fluxing condition. A PE‐g‐MA/MgAl‐LDH exfoliation nanocomposite was formed after the precipitation of PE‐g‐MA from the dispersion system. The structure and thermal property of the PE‐g‐MA/MgAl‐LDH exfoliation nanocomposite were characterized by X‐ray diffraction (XRD), transmission electron microscopy (TEM), and thermogravimetry analysis (TGA). The disappearance of d₀₀₁ XRD peak of OMgAl‐LDH at 20 = 3.2° suggests that the MgAl hydroxide sheets are exfoliated in the nanocomposite. The TEM image shows that the MgAl hydroxide sheets of less than 70 nm in length or width are exfoliated and dispersed disorderly in PE‐g‐MA matrix. TGA profiles indicate that the PE‐g‐MA/MgAl‐LDH nanocomposite with 5 wt% OMgAl‐LDH loading shows a faster charring process in temperature range from 210 to 390 °C and a greater thermal stability beyond 390 °C than PE‐g‐MA does. The decomposition temperature of the nanocomposite is 25 °C higher than that of PE‐g‐MA as measured at 50% weight loss. The PE‐g‐MA/MgAl‐LDH nanocomposite is promising for application of flame‐retardant polymeric materials.     

UV excited green luminescence of SrAl<Subscript>2</Subscript>O<Subscript>4</Subscript>:Eu<Superscript>2+</Superscript>, Dy<Superscript>3+</Superscript> nanophosphor

Eu, Dy co-doped strontium aluminate nanophosphors were prepared by the combustion synthesis method. Their structure and morphology were investigated by X-ray diffraction (XRD), scanning electron microscopy, transmission electron microscopy (TEM), and Fourier transform infrared spectroscopy. According to the XRD and the TEM analysis, the average crystallite size was found to be in the nanometer range. The phase structure of the prepared nanophosphor is consistent with a standard monoclinic phase with a space group P2₁. The prepared SrAl₂O₄:Eu²⁺, Dy³⁺ nanophosphor emitted green light with a peak at 510 nm showing blue shift, which is due to the reduction in the particle size. Two distinct peaks were observed in the ML intensity versus time curve. The two peaks in ML indicate the presence of charge transfer in an ML process.     

Thermomechanical properties and crystallization behavior of layered double hydroxide/poly(ethylene terephthalate) nanocomposites prepared by in‐situ polymerization

Thermomechanical properties and crystallization behavior of poly(ethylene terephthalate) (PET) nanocomposites containing layered double hydroxide (LDH) were investigated. To enhance the compatibility between PET matrix and LDH, dimethyl 5‐sulfoisophthalate (DMSI) anion intercalated LDH (LDH‐DMSI) was synthesized by coprecipitation method, and its structure was confirmed by Fourier transform infrared (FTIR) spectrometer and X‐ray diffraction (XRD) measurements. Then, PET nanocomposites with LDH‐DMSI content of 0, 0.5, 1.0, and 2.0 wt% were prepared by in‐situ polymerization. The dispersion morphologies were observed by transmission electron microscopy (TEM) and XRD, showing that LDH‐DMSI was exfoliated in PET matrix. Thermal and mechanical properties, such as thermal stability, tensile modulus, and tensile yield strength of nanocomposites, were enhanced by exfoliated LDH‐DMSI nanolayers. However, elongation at break was drastically decreased with LDH loading owing to the increased stiffness and microvoids. The effect of exfoliated nanolayers, which acted as a nucleating agent confirmed by differential scanning calorimeter (DSC), on the microstructural parameters during isothermal crystallization, was analyzed by synchrotron small‐angle X‐ray scattering (SAXS). It is believed that nanocomposites could be crystallized more easily owing to the increased nucleation sites, which lead to the decrease of average amorphous region size and the long period with the increase of LDH‐DMSI content. © 2006 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 45: 28–40, 2007     

Synthesis of Layered Hydroxide Zinc m‐Aminobenzoate Compounds and Their Exfoliation Reactions

Two types of layered hydroxide zinc m‐aminobenzoate compounds with structures of layered basic metal salt (LBMS) were prepared by the reaction of zinc hydroxide with m‐aminobenzoic acid solution in the temperature range of 40–120°C. The formation reactions, structures, chemical compositions, and exfoliation reactions of the layered compounds in alcohol solvents were investigated by XRD, TG‐DTA, SEM, and TEM. One layered phase with a basal spacing of 1.08 nm has a α‐Ni(OH)₂‐like structure, and its chemical formula can be written as Zn(OH)_0.67(m‐NH₂C₆H₄COO)_1.33. This phase has strip‐like particle morphology and cannot be exfoliated into its nanosheets in alcohol solvents. The other layered phase with a basal spacing of 2.66 nm has a zinc hydroxide‐nitrate‐like structure, and can be exfoliated in alcohol solvents.     

DFT‐Based Simulation and Experimental Validation of the Topotactic Transformation of MgAl Layered Double Hydroxides

The thermal topotactic transformation mechanism of MgAl layered double hydroxides (LDHs) is investigated by a combined theoretical and experimental study. Thermogravimetric differential thermal analysis (TG‐DTA) results reveal that the LDH phase undergoes four key endothermic events at 230, 330, 450, and 800 °C. DFT calculations show that the LDH decomposes into CO₂ and residual O atoms via a monodentate intermediate at 330 °C. At 450 °C, the metal cations almost maintain their original distribution within the LDH(001) facet during the thermal dehydration process, but migrate substantially along the c‐axis direction perpendicular to the (001) facet; this indicates that the metal arrangement/dispersion in the LDH matrix is maintained two‐dimensionally. A complete collapse of the layered structure occurs at 800 °C, which results in a totally disordered cation distribution and many holes in the final product. The structures of the simulated intermediates are highly consistent with the observed in situ powder XRD data for the MgAl LDH sample calcined at the corresponding temperatures. Understanding the structural topotactic transformation process of LDHs would provide helpful information for the design and preparation of metal/metal oxides functional materials derived from LDH precursors.     

Amine‐Assisted Syntheses of Carbonate‐Free and Highly Crystalline Nitrate‐Containing Zn‐Al Layered Double Hydroxides

Zn‐Al layered double hydroxides (LDHs), with nitrate as the charge balancing anion in the interlayer space, were synthesized by precipitation from homogeneous solution containing different amines [e.g., hexamethylenetetraamine (HMTA), diethylenediamine (DEDA), trimethylamine (TMA) and dimethylamine (DMA)]. The applied method does not require nitrogen atmosphere. The solution pH and concentration of different amines were varied in order to identify the controlling parameters and whether nitrate or carbonate are the interlayer anion. Particularly, the addition of amines turns out to be an effective tool for the synthesis of nitrate containing Zn‐Al LDHs independent from the nitrogen atmosphere. The structure, textural, composition, and morphological properties were investigated using the powder X‐ray diffraction (PXRD), thermogravimetric analysis (TGA), FT‐IR spectroscopy, and scanning electron microscopy (SEM). The analyses showed that the samples had high crystallinity and purity. The NO₃‐ZnAl LDHs samples show that LDH sheets are predominantly smooth textured and the thickness of LDH sheets are found to be around 23 nm. The results also indicate that this method successfully produces a NO₃^– form Zn‐Al LDH that is almost identical to the one synthesized by conventional methods.     

An Effective Asphalt UV Blocking Material Based on Host‐Guest Schiff Base/Layered Double Hydroxides

The development of asphalt‐based UV blocking materials is important to extend the alphalt lifespan in road construction. In this work, we put forward that the fabrication of host‐guest system can be an effective way to obtain UV blocking materials. Firstly, a new anionic Schiff base, N ,N' ‐bis(salicylidine)‐4,4'‐diaminostilbene‐2,2'‐disulfonic acid (SDSD ), has been synthesized, which was intercalated into Zn‐Al‐LDH by anion‐exchange method. FT‐IR and XRD illustrate the layered organic–inorganic composite, Zn‐Al‐SDSD‐LDH , has been successfully synthesized with high crystallinity. Laser particle size analyzer, SEM and TEM show that particle size distributions of Zn‐Al‐SDSD‐LDH is in the range 100–500 nm. UV –vis absorption spectra show that Zn‐Al‐SDSD‐LDH has better UV absorption than the pristine Zn‐Al‐LDH and SDSD . Furthermore, the mixture of asphalt and 3 wt% Zn‐Al‐SDSD‐LDH presents enhanced UV blocking property relative to the pristine asphalt after irradiating by UV spray accelerated weathering test. Therefore, this work not only develops a new type of host‐guest Zn‐Al‐SDSD‐ LDH , but also confirms it can be an effective asphalt UV blocking material for practical application.     

Layered double hydroxide – montmorillonite – a new nano‐dimensional material

A new nano‐dimensional material, layered double hydroxide – montmorillonite (LDH‐MMT), has been synthesized by the formation of an LDH in the presence of MMT. The structure is studied using X‐ray diffraction, Fourier transform infrared, scanning electron microscopy, and energy‐dispersive X‐ray spectroscopy analysis. The LDH‐MMT shows a novel layered structure containing negatively charged MMT layers and positively charged LDH layers with some sodium ions required to balance the charge. LDH‐MMT can be ion‐exchanged to obtain organically modified LDH‐MMT, and this material can be well‐dispersed in polystyrene. Copyright © 2012 John Wiley & Sons, Ltd.     

Morphological mapping and analysis of poly[styrene‐b‐(ethylene‐co‐butylene)‐b‐styrene] and its clay nanocomposites by atomic force microscopy

Atomic force microscopy was successfully applied for comprehensive nanoscale surface and bulk morphological characterization of thermoplastic elastomeric triblock copolymers: poly[styrene‐b‐(ethylene‐co‐butylene)‐b‐styrene] (SEBS) having different block lengths and their clay based nanocomposites. Commercially available Cloisite®20A and octadecyl (C₁₈) ammonium ion modified montmorillonite clay (OC) prepared in our laboratory by cation exchange reaction were used. The phase detected images in the tapping mode atomic force microscopy exhibited a well‐ordered phase separated morphology consisting of bright nanophasic domains corresponding to hard component and darker domains corresponding to softer rubbery ethylene‐co‐butylene (PEB) lamella for all the neat triblock copolymers. This lamellar morphology gave a domain width of 19–23 nm for styrenic nanophase and 12–15 nm for ethylene‐co‐butylene phase of SEBS having end to mid block length ratio of 30:70 and block molecular weights of 8800–41,200–8800. On increasing the ratio of block lengths of the polymer matrix and the selectivity of the solvent toward the blocks used for casting, the morphological features of the resultant films altered along with change in domain thickness. The phase images showed position and distribution of the brightest clay stacks in the dark‐bright contrast of the base matrix of the nanocomposite. Exfoliated and intercalated‐exfoliated morphology obtained in the case of Cloisite®20A and OC‐based SEBS nanocomposites, respectively, is further supported by X‐ ray diffraction and transmission electron microscopy studies. The lamellar thickness of the soft phases widened to 50–75 nm, where the layered clay silicates (40–54 nm in length and 4–17 nm in width) were embedded in the soft rubbery phases in the block copolymeric matrix of the nanocomposite. The marginally thicker width of the hard styrenic phases and slightly shrinked width of the soft rubbery lamella can be observed from the regions where no nanofiller is present. Distinct differences in bulk morphologies of the nanocomposites prepared in the melt and the solution processes were obtained with nanocomposites. The presence of clay particles was evident from the almost zero pull‐off and snap‐in force in the force‐distance analysis of SEBS based nanocomposite. This analysis also revealed stronger tip interaction resulting in highest contact and adhesive forces with the softer PEB region relative to the harder PS region. © 2006 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 45: 52–66, 2007     

Development of air‐assisted dispersive micro‐solid‐phase extraction‐based supramolecular solvent‐mediated Fe3O4@Cu–Fe–LDH for the determination of tramadol in biological samples

A simple method, air‐assisted dispersive micro‐solid‐phase extraction‐based supramolecular solvent was developed for the preconcentration of tramadol in biological samples prior to gas chromatography–flame ionization detection. A new type of carrier liquid, supramolecular solvent based on a mixture of 1‐dodecanol and tetrahydrofuran was combined with layered double hydroxide coated on a magnetic nanoparticle (Fe₃O₄@SiO₂@Cu–Fe–LDH). The supramolecular solvent was injected into the solution containing Fe₃O₄@SiO₂@Cu–Fe–LDH in order to provide high stability and dispersion of the sorbent without any stabilizer agent. Air assisted was applied to enhance the dispersion of the sorbent and solvent. A number of analytical techniques such as Fourier transform‐infrared spectrometry, field emission scanning electron microscope, energy‐dispersive X‐ray spectroscopy and X‐ray diffraction measurements were applied to assess the surface chemical characteristics of Fe₃O₄@SiO₂@Cu–Fe–LDH nanoparticles. The effects of important parameters on the extraction recovery were also investigated. Under optimized conditions, the limits of detection and quantification were obtained in the range of 0.9–2.4 and 2.7–7.5 μg L^?1 with preconcentration factors in the range of 450–472 in biological samples. This method was used for the determination of tramadol in biological samples (plasma, urine and saliva samples) with good recoveries.     

Adsorption of Metanil Yellow Azoic Dye from Aqueous Solution onto Mg‐Fe‐NO3 Layered Double Hydroxide

We report the preparation and characterization of a layered double hydroxide (LDH) adsorbent for azoic dye, metanil yellow (yellow GX; YGX) removal. The nanoparticles of Mg‐Fe‐LDH‐NO₃ adsorbent were prepared with Mg/Fe molar ratio of 3:1 by a hydrothermal process and coprecipitation method at pH 9.5 and were characterized by X‐ray powder diffraction (XRPD), thermal gravimetric analysis (TGA), elemental analysis, and Fourier transform infrared spectroscopy (FT‐IR). The size and morphology of nanoparticles were examined by scanning electron microscopy (SEM). The XRD patterns indicate that the intercalation of YGX between the LDH layers has not occurred and surface adsorption has happened. In the adsorption experiments, the Gibbs free energy ΔG⁰ values, the enthalpy ΔH⁰, and entropy ΔS⁰ was determined. The isotherms showed that the adsorption of YGX by Mg‐Fe‐LDH‐NO₃ was both consistent with Langmuir and Freundlich equations.     

ZnCr Layered Double Hydroxide (LDH) Nanosheets Assisted Formation of Hierarchical Flower‐Like CdZnS@LDH Microstructures with Improved Visible‐Light‐Driven H2 Production

The development of new semiconductor photocatalysts toward splitting water has supplied a promising way to obtain sustainable and clean hydrogen energy. Herein, CdZnS@layered double hydroxide (LDH) composites with a hierarchical flower‐like microstructure have been fabricated with the aid of ZnCr–LDH nanosheets as templates. XRD, SEM and HRTEM show that the ZnCr–LDH nanosheets are uniformly dispersed within the composites. The surface of the hierarchical structures is rough and composed of numerous nanocrystals of CdZnS. The HRTEM images indicate that the surface of CdZnS nanocrystals is mainly composed of the (111) plane. Moreover, the visible‐light‐driven H₂ production performance of the CdZnS in the presence and absence of ZnCr–LDH nanosheets has been measured. The results show that ZnCr–LDH nanosheets play an important role in the hierarchical morphology and photocatalytic activity of the as‐prepared samples. In the water‐splitting process, the visible‐light‐driven H₂‐production rate of hierarchical flower‐like CdZnS@LDH is 4.03 times and nearly 10 times higher than that of pristine CdZnS microsphere and pure commercial CdS, respectively. Therefore, this work not only achieves enhanced catalytic performance of the CdZnS by the introduction of ZnCr–LDH nanosheets, but also supplies an insight into the relationship between the hierarchical morphology and the semiconductor photocatalytic activity.     

Effect of Electrolytes and Polymers on the Thixotropy of Mg‐Al‐Layered Double Hydroxides/Kaolinite Dispersions

The effect of electrolytes (NaCl and CaCl₂) and polymers (CPAM and HPAM) on the thixotropy of Mg‐Al‐layered double hydroxide (LDHs)/kaolinite dispersions has been investigated. It was observed that the type of thixotropy in LDH/kaolinite dispersions may be affected by NaCl, but not by CaCl₂ in range of concentration of interest. The type of thixotropy in LDH/kaolinite dispersion with R=0 transformed from positive thixotropy to complex thixotropy and at last positive thixotropy again with the concentration of NaCl in range of 0.00–0.10 mol·L⁻¹; the type of thixotropy in LDHs/kaolinite dispersions with R=0.25 transformed from complex thixotropy to positive thixotropy and then complex thixotropy again with the concentration of NaCl in range of 0.00–0.10 mol·L⁻¹. The type of thixotropy in LDH/kaolinite dispersion with R=0 may be not affected by cationic polyacrylamide (CPAM) and hydrolyzed polyacrylamide (HPAM); but the LDHs/kaolinite dispersions with R=0.25 transformed from complex thixotropy to positive thixotropy with the both polymers concentration in range of interest, which indicated that the microstructure of the dispersion changed from weak folc sediments structure to steric network structure.     

Adsorption of 4‐Chloro‐2‐methylphenoxy Acetic Acid (MCPA) from Aqueous Solution onto Cu‐Fe‐NO3 Layered Double Hydroxide Nanoparticles

The nanoparticles of Cu‐Fe‐NO₃ layered double hydroxide (LDH) were prepared with Cu/Fe molar ratio of 2:1 by a thermal process and co‐precipitation method at pH 9 and were characterized by X‐ray powder diffraction (XRPD), thermal gravimetric analysis (TGA), atomic adsorption spectroscopy (AAS) and fourier infrared spectroscopy (FT‐IR). The size and morphology of nanoparticles were examined by transmission electron microscopy (TEM). Cu‐Fe‐NO₃‐LDH was studied as a potential adsorbent of the acid herbicide MCPA [(4‐chloro‐2‐methylphenoxy) acetic acid] as function of pH, contact time and temperature. The results showed high and rapid adsorption of MCPA on the LDH. The characterization of the adsorption products by XRD indicates that the intercalation of MCPA between the LDH layers has not occurred and surface adsorption has happened. The adsorption kinetic was tested for pseudo‐first‐order, pseudo‐second‐order, elovich and intra‐particle diffusion kinetic models and rate constants were calculated. Freundlich and Langmuir isotherm models were applied to experimental equilibrium data obtained from the measurements of pesticide adsorption. Langmuir isotherm slightly better fitted to the experimental data than that of Freundlich. In the adsorption experiments, the Gibbs free energy ΔG⁰ values, the enthalpy ΔH⁰, and entropy ΔS⁰ were determined.     

Preparation and Properties of Transparent Ultrathin Lanthanide‐Complex Films

Highly transparent ultrathin films (UTFs) based on alternative layer‐by‐layer assembly of Eu‐ and Tb‐based lanthanide complexes (LCs) and Mg–Al‐layered double hydroxide (LDH) nanosheets are reported herein. UV–visible absorption and fluorescence spectroscopy showed an orderly growth of the two types of ultrathin films upon increasing the number of deposition cycles. AFM and SEM measurements indicate that the films feature periodic layered structures as well as uniform surface morphology. Luminescent investigations reveal that (LCs/LDH)_n UTFs can detect Fe³⁺ with relative selectivity and high sensitivity (Stern–Volmer constant K_SV=8.43×10³ L mol^?1); this suggests that (LCs/LDH)_n UTFs could be a promising luminescent probe for selectively sensing Fe³⁺ ion.     

Improving Thermal and Flame Retardant Properties of Epoxy Resin with Organic NiFe‐Layered Double Hydroxide‐Carbon Nanotubes Hybrids

To improve the dispersion of carbon nanotubes (CNTs) and flame retardancy of layered double hydroxide (LDH) in epoxy resin (EP), organic nickel‐iron layered double hydroxide (ONiFe‐LDH‐CNTs) hybrids were assembled through co‐precipitation. These hybrids were further used as reinforcing filler in EP. EP/ONiFe‐LDH‐CNTs nanocomposites containing 4 wt% of ONiFe‐LDH‐CNTs with different ratios of ONiFe‐LDH and CNTs were prepared by ultrasonic dispersion and program temperature curing. The structure and morphology of the obtained hybrids were characterized by different techniques. The dispersion of nanofillers in the EP matrix was observed by transmission electron microscopy (TEM). The results revealed a coexistence of exfoliated and intercalated ONiFe‐LDH‐ CNTs in polymer matrix. Strong combination of the above nanofillers with the EP matrix provided an efficient thermal and flame retardant improvement for the nanocomposites. It showed that EP/ONiFe‐LDH‐CNTs nanocomposites exhibited superior flame retardant and thermal properties compared with EP. Such improved thermal properties could be attributed to the better homogeneous dispersion, stronger interfacial interaction, excellent charring performance of ONiFe‐LDH and synergistic effect between ONiFe‐LDH and CNTs.