Layered Double Hydroxide Hybrid Research Articles

Interleaved Electroactive Molecules into LDH Working on Both Electrodes of an Aqueous Battery-Type Device.

By selecting two electroactive species immobilized in a layered double hydroxide backbone (LDH) host, one able to act as a positive electrode material and the other as a negative one, it was possible to match their capacity to design an innovative energy storage device. Each electrode material is based on electroactive species, riboflavin phosphate (RF) on one side and ferrocene carboxylate (FCm) on the other, both interleaved into a layered double hydroxide (LDH) host structure to avoid any possible molecule migration and instability. The intercalation of the electroactive guest molecules is demonstrated by X-ray diffraction with the observation of an interlayer LDH spacing of about 2 nm in each case. When successfully hosted into LDH interlayer space, the electrochemical behavior of each hybrid assembly was scrutinized separately in aqueous electrolyte to characterize the redox reaction occurring upon cycling and found to be a rapid faradic type. Both electrode materials were placed face to face to achieve a new aqueous battery (16C rate) that provides a first cycle-capacity of about 7 mAh per gram of working electrode material LDH/FCm at 10 mV/s over a voltage window of 2.2 V in 1M sodium acetate, thus validating the hybrid LDH host approach on both electrode materials even if the cyclability of the assembly has not yet been met.

Ultrathin graphene@NiCo2S4@Ni-Mo layered double hydroxide with a 3D hierarchical flowers structure as a high performance positive electrode for hybrid supercapacitor

This study presents three-dimensional flower-like spheres composed of NiCo2S4@Ni-Mo layered double hydroxide (LDH) nanocomposites, which are grown in situ on reduced graphene oxide (RGO). The RGO@NiCo2S4@NiMo-LDH nanocomposites exhibit remarkable electrochemical properties and have a specific capacitance of 1346 F g−1 at the current density of 1 A g−1. In addition, using RGO@NiCo2S4 @NiMo-LDH hybrid nanosheets and activated carbon (AC) as the positive and negative electrodes, the asymmetric supercapacitor device was successfully assembled, and it showed a significant energy density of 59.38 Wh kg−1 at a power density of 808.19 W kg−1, with good cycle stability. The initial capacity retention rate is 80 % after 10,000 cycles. These results demonstrate the great potential of the synthesized RGO@NiCo2S4@NiMo-LDH composite for the development of high-performance electrode materials for supercapacitors.

Showcasing advanced electrocatalytic behavior of layered double hydroxide wrapped on carbon nanotubes: Real-time monitoring of L-cysteine in biological matrices

L-cysteine is an imperative amino acid which exists in natural proteins and plays crucial roles in biological systems, thereby its sensitive and selective monitoring is extremely necessary. In this work, novel hybrid nanoarchitectures have been fabricated by wrapping positively charged NiAl layered double hydroxide (LDH) nanosheets on negatively charged carbon nanotubes (CNTs). The electrochemical behavior of CNTs@NiAl LDH hybrids having different concentrations of NiAl LDH precursor salts with fixed amount of CNTs have been explored in detection of L-cysteine using cyclic voltammetry and amperometry techniques. High conductivity of CNTs together with enhanced electrocatalytic properties of NiAl LDH and plentiful surface active sites are accountable to facilitate the direct detection of L-cysteine. Therefore, the fabricated electrode exhibits excellent sensing performance with 0.05 µM to 780 µM wide linear range, sensitivity of 351 μA mM−1 cm−2, low limit of detection upto 3 nM (S/N = 3), superb reproducibility and stability as well as brilliant selectivity against common interferents. Arising from remarkable efficiency, the CNTs@NiAl LDH based sensing system has been practically used in real-time detecting L-cysteine effluxes from different living cells upon stimulation as-well-as in-vitro monitoring of L-cysteine concentrations in human samples (urine and serum).

Preparation of well-structured hybrid material through ion exchange of chloride by 2,4,5-trichlorophenoxyacetic herbicide in a layered double hydroxide

The [Zn2–Al–Cl] layered double hydroxide (LDH) was used to successfully exchange chloride ions by 2,4,5-trichlorophenoxyacetic acid (2,4,5-T), as a model of the carboxylate herbicide family. The total exchange was obtained after 6 h of stirring with a 2,4,5-T/Cl molar ratio of 10 and a pH of 7. The characterization by various techniques (XRD, FTIR, TG-DTG and SEM) indicates that this exchange led to the production of a new stable hybrid LDH phase intercalated by the herbicide. The structural analysis of the material, based on the interlayer distance of 1.855 nm, indicates that the 2,4,5-T anion takes a vertical arrangement in a double layer. The cohesion of the structure is ensured by hydrogen bonds between the carboxylate group of the herbicide and the hydroxyl groups of the LDH sheets. The exchange causes a modification of the type of symmetry from a 3R stacking mode for [Zn2–Al–Cl] (space group R3‾m) to a 2H for [Zn2–Al-2,4,5-T] (space group P63/mmc). This result confirms the already proven use of LDH materials as efficient anion exchangers for the trapping and elimination of this type of pollutant from wastewater.

Photocatalytic Water Oxidation by Phosphotungstate and Mg-Al Layered Double Hydroxide Hybrid

Abstract Immobilization of phosphotungstate ([PW12O40]3−) in the interlayer space of a Mg-Al layered double hydroxide (LDH) resulted in an absorption edge at ∼350 nm, different from the pristine LDH or the POM (either in aqueous solution or in the solid state). The obtained hybrid showed enhanced photocatalytic activity for water oxidation in the presence of Ag+ as an electron acceptor.

Synthesis of Organic-Inorganic Hybrid Material with a Synergistic Interface as a Release Agent for Free Acid β-Hydroxy-β-Methyl Butyrate

We report the preparation and characterization of a new organic-inorganic hybrid system composed of type-I collagen and ZnAl layered double hydroxide (LDH) particles loaded with β-hydroxy-β-methyl butyrate (HMB) by coprecipitation reaction. X-ray diffraction (peaks well agree with those reported in the literature), infrared spectroscopy (stretching bonds for both organic-inorganic compounds), and X-ray photoelectron spectroscopy confirmed the hybrid system retained HMB in the carboxylate form, and a small fraction turned to the acid form. In both cases, the HMB molecules are assembled to the LDH surface. The hybrid compound results in improved thermal stability for HMB and collagen, as shown by thermal analysis. Scanning electron microscopy data reflects different arrangements from LDH sheets with interesting physicochemical properties since LDH and collagen protect free HMB and make it more bioavailable and functional. In vitro studies as part of high-throughput screening strategies indicated that LDH hybrids reduced cell viability around 75-90%, which is an acceptable viability value because of the L6 cell line susceptibility. However, all new nanomaterials must be carefully analyzed by different toxicity tests because a single test does not evaluate complete physiological compartments.

Effect of hybrid fillers of Mg–Al layered double hydroxide and nanoclay on the mechanical behavior and formability of glass laminate AA5052‐reinforced epoxy composites

AbstractThis research work investigates the influence of hybrid particulate fillers, Mg–Al layered double hydroxide (LDH), and nanoclay (NC), on the mechanical properties and formability of glass laminate AA5052 epoxy composites (GLARE). The composite laminates were prepared by varying the weight percentage (i.e., 3, 4, and 5 wt%) of the hybrid fillers in the epoxy resin. The conventional hand layup technique was utilized for the fabrication of the laminates. The tensile test samples were prepared in different orientations with respect to the rolling direction (i.e., 0°, 45°, and 90°) to address their anisotropic nature. The flexural, impact, lap shear, and formability tests were conducted as per ASTM and IS standards. The Erichsen cupping test was performed to study the formability of the composite laminates. For each test, the results were compared with that of the laminates containing individual LDH filler, NC filler, and no filler material. The results showed that the composite laminate with 5 wt% of LDH + NC hybrid filler exhibited enhanced tensile properties, impact energy, and lap shear strength while the laminate of 4 wt% LDH + NC filler possessed better flexural properties. The formability of the composite laminates with hybrid LDH + NC fillers was observed to be lower than that of the laminates with individual filler materials and laminate without any filler. The variation observed in the test results was justified by investigating the failure mechanism of the composite laminates using a scanning electron microscope.

Synthesis of CNTs/CoNiFe-LDH Nanocomposite with High Specific Surface Area for Asymmetric Supercapacitor.

Ternary layered double hydroxide (LDH) materials have shown promising application in hybrid supercapacitors. However, the low electrical conductivity of LDHs is still a restriction to their performance. Herein, carbon nanotubes/cobalt–nickel–iron LDH (CNTs/CoNiFe-LDH) hybrid material was prepared by a one-step hydrothermal approach for the first time. The presence of CNTs improved the conductivity and surface area of the electrode, leading to an enhanced electrochemical performance. The CNTs/CoNiFe-LDH hybrid electrode exhibited high specific capacity 170.6 mAh g−1 at a current density of 1 A g−1, with a capacity retention of 75% at 10 A g−1. CNTs/CoNiFe-LDH//AC asymmetric supercapacitor (ASC) was also assembled, which had high specific capacitance (96.1 F g−1 at the current density of 1 A g−1), good cycling stability (85.0% after 3000 cycles at 15 A g−1) and high energy density (29.9 W h kg−1 at the power density of 750.5 W kg−1). Therefore, the CNTs/CoNiFe-LDH material could be used for hybrid supercapacitor electrodes.

The nonvolatile resistive switching memristor with Co-Ni layered double hydroxide hybrid nanosheets and its application as a artificial synapse

Because of its excellent electrical properties and promising application prospects, two-dimensional materials have attracted extensive research interests of researchers. Among them, Co-Ni layered double hydroxide (LDH) has semiconductor properties and has been widely studied in super capacitor. However, there are few reports about 2D Co-Ni LDHs materials as memristors. In this work, a memristor based on Co-Ni LDHs hybrid nanosheets is reported. After electroforming, Al/Co-Ni LDHs/Al devices exhibit nonvolatile resistance switching behavior. More importantly, multiple progressive resistance switches could be achieved by adjusting the duration or amplitude of the applied pulse (less than the set threshold voltage to prevent a sudden setting process). Given its gradual resistive switching, Co-Ni LDHs-based memristors were used to simulate synaptic function in biology, including: “learning” and “forgetting” process, STP and LTP, PPF characteristics, and STDP. By studying the microstructure, it is proposed that the O vacancy is the physical mechanism of the resistance switch behavior. This work reveals that Co-Ni LDH nanosheets have excellent application potential in memristors, which may open the door to more functions and applications.

Surface enhanced Co-Mn double hydroxide coronal architectures for hybrid energy storage

Tailoring of surface-enhanced materials is vital towards achieving enhanced energy storage. In order to achieve this, hybrid material combinations often used in traditional vertically stacked morphologies. However, the inherent nature of poor conductivity and aggregation results in a bottleneck in exploiting such materials' full potential. In particular, the hybrid composites of layered double hydroxide (LDH) architectures suffer from restacking and results in poor charge transport. To mitigate these issues, the rational design of a graphene-based interlinked framework is vital. The interfacial phenomena associated with graphene's charge transport properties are also of considerable interest for manoeuvring graphene-based hybrid material architectures. Herein, we report the synthesis of Co-Mn LDH coronal hybrids with radially aligned LDH lamellae on graphene-based core shells. The synthesis process involves spherical graphene oxide core shells obtained from GO encapsulated SiO2 spheres to prepare hollow coronal LDH hybrids. Without any harsh reagents, self-sacrificial removal of the SiO2 core occurs. The process also helps formulate open porous graphene channels, which help in an efficient charge transfer process. The charge transfer efficiency of LDH becomes superior by incorporating the electrically conductive graphene-based nano core framework. The battery type hybrid material shows an enhanced energy storage capacity of ~770 Cg−1 at a current density of 1 Ag−1.

Reliability study under thermal and photonic stresses of sulforhodamine B (SRB) confined in layered double hydroxide (LDH)

When sulforhodamine B (SRB) is entrapped in a tightly packed hybrid material composed of dodecylsulfate anions interleaved in layered double hydroxide, the organic dye is considered as a possible red-emitting phosphor for white light-emitting diodes (WLEDs). To confirm such promising potential, a reliability study is here undertaken and the materials and their associated silicone films are subjected to different thermal and photonic stresses. Optical properties, photoluminescence quantum yields and emission spectra are recorded after photo-aging studies. Interestingly, the composite silicone film is found to be completely stable under blue LED excitation, while in the absence of the hybrid LDH the emission of SRB decays rapidly, thus underlining the protective role of the LDH hybrid cargo. At this stage, these results confirm the potential offered by a system consisting of such an emitter film and a blue LED. This system also opens up new possibilities for interesting organic dyes that are sensitive to photonic and/or thermal stresses.

Morphological and Thermal Properties of Poly(Vinyl Alcohol)/Layered Double Hydroxide Hybrid Nanocomposite Fibers

Nanolayered particulate of Zn-based layered double hydroxide (LDH) was prepared by a low temperature greener sol-gel method. X-ray diffraction (XRD) studies were performed on the particles annealed at different temperatures. Hexagonal crystal structure of the as-grown LDH particulates was observed. The crystal structure was modified to tetragonal structure of layered double oxide (LDO) on annealing at 250°C. Rietveld fittings showed a collapse of interlayer separation distance along the preferred orientation of the LDH particles as a result of heat treatment. Further, LDH particles were used as fillers of electrospun poly(vinyl alcohol) (PVA) fibers. Heat treatment of the polymer fibers was also performed at different temperatures, and thermal changes were studied by thermogravimetric analysis (TGA), Raman spectroscopy, and scanning electron microscopy (SEM) techniques. Improved interaction of fibers with LDH nanoparticles was observed and ascribed to LDH-related LDO phase transformation at higher temperature. Thermal mechanisms of the rapid weight loss in filled fibers were discussed in comparison to the pure PVA fiber losses. Experimental Raman frequencies of the composite fibers were compared with the calculated Raman modes of the enol and ZnO monomers. The molecular vibration frequencies were found to differ significantly due to heat treatment. Finally, the role filler in the faster and greener thermal decomposition of polymeric fibers was also discussed in the present work.

Internal electric field induced S–scheme heterojunction MoS2/CoAl LDH for enhanced photocatalytic hydrogen evolution

The requisite interfacial contact of heterojunction photocatalysts has a significant contribution in separation of interfacial charge carriers for photocatalytic hydrogen (H2) evolution in a more efficient manner. Herein, an internal electric field (IEF)-induced S–scheme system comprised of two-dimensional (2D) CoAl layered double hydroxide (LDH) and 2D molybdenum disulfide (MoS2) was constructed via a simple hydrothermal process. In the presence of visible-light irradiation, the 2D/2D MoS2/CoAl LDH hybrid demonstrates eightfold greater photocatalytic H2 generation rate as compared with that of CoAl LDH. The mechanism was investigated in the light of the results of the X-ray photoelectron spectroscopy (XPS) and work-function calculated by density functional theory (DFT) simulation, and the improved activity was ascribed to that the rapid detachment of the electron-hole (e−-h+) combinations and high redox ability, both are simultaneously realized in MoS2/CoAl LDH hybrid with a 2D/2D S–scheme charge transfer mechanism induced by the IEF across interface of the MoS2 and CoAl LDH. Furthermore, favorable 2D/2D structure and better H* adsorption behavior of MoS2/CoAl LDH also promoted the improvement of water reduction performance. This work is a valuable guideline in developing of IEF-induced S–scheme photocatalysts with 2D/2D architecture for improved photocatalytic performance.

Layered Double Hydroxide Nanoparticles to Overcome the Hydrophobicity of Ellagic Acid: An Antioxidant Hybrid Material.

Ellagic acid (EA), a polyphenolic antioxidant of poor water solubility, was intercalated into biocompatible layered double hydroxide (LDH) nanoparticles by the coprecipitation method. Structural investigation of the composite revealed that the lactone bonds split under the synthetic experimental conditions, and EA was transformed to 4,4′,5,5′,6,6′-hexahydroxydiphenic acid during intercalation. To improve the surface properties of the EA-LDH composite, the samples were treated with different organic solvents. The antioxidant activity of the LDH hybrids was assessed in test reactions. Most of the obtained hybrids showed antioxidant activity comparable to the one of the free EA indicating that the spontaneous structural transformation upon immobilization did not change the efficiency in radical scavenging. Treatments with organic solvents influenced the activities of the materials remarkably. The main advantage of the immobilization procedure is that the products can be applied in aqueous samples in high concentrations overcoming the problem related to the low solubility of EA in water. The developed composites of high antioxidant content can be applied as efficient reactive oxygen species scavenging materials during biomedical treatments or industrial manufacturing processes.

Multifunctional carboxymethyl chitosan derivatives-layered double hydroxide hybrid nanocomposites for efficient drug delivery to the posterior segment of the eye

Efficient ocular drug delivery to the posterior segment of the eye by topical administration is a great challenge to pharmacologists. To explore drug delivery system of organic-inorganic hybrid nanocomposites for the efficient delivery of dexamethasone disodium phosphate (DEXP), a targeted hybrid nanocomposite based on layered double hydroxide (LDH) and functional carboxymethyl chitosan (CMCS) derivatives was designed. A special substrate of peptide transporter-1 (PepT-1) and glutathione was modified on CMCS. CMCS-glutathione-glycylsarcosine (CMCG-GS) and CMCS-glutathione-valyl-valine (CMCG-VV)-LDH hybrid nanocomposites were prepared and structurally confirmed. The in vitro experiments on human conjunctival epithelial cells showed noncytotoxicity (LDH concentration ≤100.0 µg/mL) and enhanced permeability for hybrid nanocomposites. Additionally, cellular uptake of the CMCG-GS-DEXP-LDH (10:1) nanocomposite eye drops involved clathrin-mediated endocytosis and PepT-1 mediated actively targeting transport. Results of the in vivo precorneal retention study showed an 8.35-fold, 2.87-fold and 2.58-fold increase of AUC0–6 h, Cmax and MRT for CMCG-GS-DEXP-LDH (10:1) hybrid nanocomposite eye drops, respectively, compared to that of the commercial product. Fluorescence imaging of fluorescein isothiocyanate isome (FITC)-loaded LDH hybrid nanocomposites demonstrated that FITC could diffuse into the choroid-retina with the shelter of LDH and CMCG-GS. The presence of a strong fluorescence signal of FITC-conjugated LDH hybrid nanocomposites in the sclera revealed that integral LDH nanocarrier reached the sclera. In the tissue distribution evaluation of rabbit's eyes, DEXP of CMCG-GS-DEXP-LDH (10:1) nanocomposites group retained in the target of the choroid-retina for 3 h with final concentration at 120.04 ng/g. Furthermore, the results of fluorescence imaging and tissue distribution suggested that the intraocular transport pathway for the hybrid nanocomposites is the conjunctival-scleral route. Consequently, the developed hybrid nanocomposites offer a simple and efficient strategy for topically administered drug delivery to the posterior segment of the eye. Statement of SignificanceEfficient ocular drug delivery to the posterior segment of the eye by topical administration is a great challenge to pharmacologists. In this manuscript, hybrid nanocomposite based on layered double hydroxide (LDH) and functional carboxymethyl chitosan (CMCS) derivatives were designed. The multifunctional properties of these hybrid nanocomposites were attributed to active targeting, bioadhesive capacity and penetration enhancement. Visualization of transport routes of fluorescein isothiocyanate-conjugated LDH hybrid nanocomposites demonstrated that the integral LDH nanocarrier reached the sclera through the conjunctival-scleral pathway, and the loaded drug could further diffuse to the retina. The multifunctional CMCS derivatives-LDH hybrid nanocomposites could be applied for the efficient drug delivery to the posterior segment of the eye through noninvasive topical instillation.

Doxorubicin intercalated copper diethyldithiocarbamate functionalized layered double hydroxide hybrid nanoparticles for targeted therapy of hepatocellular carcinoma.

Hepatocellular carcinoma (HCC) is one of the deadliest cancers due to its long incubation period and low cure rate. Layered double hydroxide (LDH) nanoparticles have attracted considerable research interest in the field of nanomedicine owing to their surface effects and good biocompatibility. In this research, we synthesized a hexagonal nanoparticle by the co-precipitation method, referred to as Cu-Al LDH. As an alternative to traditional drug-loading methods, sodium diethyldithiocarbamate (DDC) was introduced and combined with Cu2+ in LDHs to form a diethyldithiocarbamate-copper complex (Cu(DDC)2), which was not only the composition of carrier materials but also an effective component for cancer therapy. Doxorubicin (DOX) was also encapsulated into LDHs due to the clinical relevance of DOX treatment for HCC. Formulations of the Cu(DDC)2 and DOX co-loaded nanoparticles were optimized to precisely control the Cu(DDC)2/DOX ratio. The nanoparticles were coated with polyethylene glycol-graft-polyglutamic acid (PEG-PLG) through electrostatic adsorption to improve the stability of the nanoparticles. The outer layer was decorated with hyaluronic acid (HA) to achieve specific targeting of tumors. Compared with non-HA coated nanoparticles, HA coated nanoparticles showed greater cellular uptake in Hep G2 cells, which could cause higher cytotoxicity. In addition, targeted nanoparticles effectively inhibited tumor growth in mouse models of ectopic hepatocellular carcinoma. It can be concluded that there is a great potential for synergistic cancer therapy using the novel DOX intercalated Cu(DDC)2 functionalized layered double hydroxide hybrid nanoparticles.

Synthesis of a novel dual layered double hydroxide hybrid nanomaterial and its application in epoxy nanocomposites

Ease of undesirable agglomeration and low efficiency are two problems that highly restrict the application of MgAl-layered double hydroxides (MgAl-LDH) as suitable flame retardants for epoxy resins. Herein, a new strategy that chose MOFs as the precursor to connect two different LDHs into a hybrid nanomaterial is reported. Nanosheets of NiCo-layered double hydroxides (NiCo-LDH) with multidimensional nanostructures were uniformly anchored on the surface of MgAl-LDH slabs. This led to a better dispersion and stronger interaction within the epoxy matrix, resulting in enhanced strength of the char layers, and also enabled synergistic flame retardant effect to the epoxy nanocomposite, when compared to the case of the unmodified epoxy. The sample passed V-0 rating in UL-94 test and its peak of heat release rate was reduced by 66.7% in cone calorimeter test with the addition of only 2.5 wt% of as-prepared flame retardant. Besides, due to the unique structure of the nanofiller, the mechanical properties of the nanocomposite were only slightly impacted. This is the first report on the synthesis of a dual LDH hybrid nanomaterial, which moreover, improved the flame retardancy of epoxy nanocomposite even when added in relatively low amounts.

Zingiber officinale Extract (ZOE) Incorporated with Layered Double Hydroxide Hybrid through Reconstruction to Preserve Antioxidant Activity of ZOE against Ultrasound and Microwave Irradiation.

We prepared Zingiber officinale extract (ZOE) incorporated in a layered double hydroxide (LDH) hybrid through a reconstruction method in order to preserve the antioxidant activity of ZOE from ultrasound and microwave irradiation. X-ray patterns, infrared spectroscopy, and scanning electron microscopy suggested that ZOE moieties were encapsulated in the interparticle space of reconstructed LDH, thus preserving its intact structure. Dynamic light scattering and zeta-potential measurement also supported the hypothesis that ZOE moieties were located in the interparticle pore of LDH rather than at the surface of LDH particles. Thermogravimetry analysis revealed that thermal stability of encapsulated ZOE could be enhanced by LDH encapsulation. Radical scavenging assay showed that antioxidant activity of ZOE–LDH hybrid was increased after ultrasound and microwave irradiation, while ZOE itself dramatically lost its antioxidant activity upon ultrasound and microwave treatment.

On Demand One-Pot Mild Preparation of Layered Double Hydroxides and Their Hybrid Forms: Advances through the Epoxide Route.

Epoxide ring opening driven alkalinization process was explored with the aim of preparing layered double hydroxide (LDH) phases on demand, at room temperature. Employing iodide as nucleophilic agent, the precipitation reaction can be driven under much lower halide concentrations. This scenario favors the selective intercalation of concomitant bulky oxo anions as nitrate or perchlorate in the LDH products, allowing for the one-pot synthesis of an LDH able to delaminate in formamide. Even large dicarboxylic acids, - O2 C-(CH2 )n -CO2 - , with n up to 8, can be quantitively intercalated within the growing LDH phase, providing a versatile one-pot route for hybrid LDHs as well. Under the mild conditions employed, governed by a continuous pH rise from a starting acid condition, a MII to M*III ratio of 2 prevails, independently from the overall cationic composition. However, after moderate hydrothermal aging LDH phases bearing a cationic ratio higher than 2 could result. The solubility of a given chloride-containing MII 2 M*III LDH can be approximated as a linear combination of the solubility of the pure hydroxylated phases of the constitutive cations, M(OH)2 and M* (OH)3 .

Amelioration of PEMFC performance at high temperature by incorporation of nanofiller (sepiolite/layered double hydroxide) in Nafion membrane

Nanoheterostructured material composed of sepiolite clay mineral in which is assembled a MgAl layered double hydroxide (LDH) was used in the preparation of Nafion composite electrolyte membranes and their behavior compared to those of membranes filled with the LDH alone. Both, the neat MgAl LDH and the MgAl LDH-sepiolite hybrid materials were obtained via the co-precipitation method. Sepiolite fibers provide a large external surface area for bonding MgAl LDH particles while maintaining high microporosity and water molecules. The nanocomposite membranes were prepared incorporating different amount of LDH or LDH-sepiolite hybrid. Composite membranes present better water retention, good thermal properties and high proton conductivities at high temperatures than the pure Nafion membrane. The proton conductivity at 100 °C and 100% RH reaches a value of 0.13 S/cm for the LDH-sepiolite Nafion membrane whereas is only 0.010 S/cm in the case of the Nafion membrane. Fuel cell tests using Nafion membranes containing LDH or LDH-sepiolite hybrid as composite electrolytes show a good result for the operation of the PEMFC at 80 °C, 100 °C and 110 °C, with a clear favoring effect of the LDH-sepiolite filler for operation at the highest temperatures.