Transparent, Ultrahigh-Gas-Barrier Films with a Brick-Mortar-Sand Structure.

Transparent and flexible gas-barrier materials have shown broad applications in electronics, food, and pharmaceutical preservation. Herein, we report ultrahigh-gas-barrier films with a brick-mortar-sand structure fabricated by layer-by-layer (LBL) assembly of XAl-layered double hydroxide (LDH, X=Mg, Ni, Zn, Co) nanoplatelets and polyacrylic acid (PAA) followed by CO2 infilling, denoted as (XAl-LDH/PAA)n-CO2. The near-perfectly parallel orientation of the LDH "brick" creates a long diffusion length to hinder the transmission of gas molecules in the PAA "mortar". Most significantly, both the experimental studies and theoretical simulations reveal that the chemically adsorbed CO2 acts like "sand" to fill the free volume at the organic-inorganic interface, which further depresses the diffusion of permeating gas. The strategy presented here provides a new insight into the perception of barrier mechanism, and the (XAl-LDH/PAA)n-CO2 film is among the best gas barrier films ever reported.

Flexible CoAl LDH@PEDOT core/shell nanoplatelet array for high-performance energy storage.

A CoAl-layered double hydroxide (LDH)@poly(3,4-ethylenedioxythiophene) (PEDOT) core/shell nanoplatelet array (NPA) is grown on a flexible Ni foil substrate as a high-performance pseudocapacitor. The LDH@PEDOT core/shell NPA shows a maximum specific capacitance of 649 F/g (based on the total mass) by cyclic voltammetry (scan rate: 2 mV/s) and 672 F/g by galvanostatic discharge (current density: 1 A/g). Furthermore, the hybrid NPA electrode also exhibits excellent rate capability with a specific energy of 39.4 Wh/kg at a current density of 40 A/g, as well as good long-term cycling stability (92.5% of its original capacitance is retained after 5000 cycles). These performances are superior to those of conventional supercapacitors and LDH NPA without the PEDOT coating. The largely enhanced pseudocapacitor behavior of the LDH@PEDOT NPA electrode is related to the synergistic effect of its individual components: the LDH nanoplatelet core provides abundant energy-storage capacity, while the highly conductive PEDOT shell and porous architecture facilitate the electron/mass transport in the redox reaction.

Resettable fluorescence logic gate based on calcein/layered double hydroxide ultrathin films.

A fluorescent logic gate was fabricated based on calcein/layered double hydroxide ultrathin films (UTFs) via alternate assembly technique, which exhibits high stability, reversibility, and resettability. The logic gate was manipulated by utilizing pH value, Hg(2+) and Cl(-) ion as inputs, and the fluorescence emission of the (calcein/LDH)(16) UTF as output, serving as a three-input logic gate that combines the YES and INHIBIT operation.

Temperature-controlled electrochemical switch based on layered double hydroxide/poly(N-isopropylacrylamide) ultrathin films fabricated via layer-by-layer assembly.

In this paper we report the fabrication of layered double hydroxide (LDH) nanoparticles/poly(N-isopropylacrylamide) (pNIPAM) ultrathin films (UTFs) via the layer-by-layer assembly technique, and their switchable electrocatalytic performance in response to temperature stimuli was demonstrated. X-ray diffraction and UV-vis absorption spectroscopy indicate a periodic layered structure with uniform and regular growth of the (LDH/pNIPAM)(n) UTFs; an interaction based on hydrogen bonding between LDH nanoparticles and pNIPAM was confirmed by X-ray-photoelectron spectroscopy and Fourier transform infrared spectroscopy. Temperature-triggered cyclic voltammetry and electrochemical impedance spectroscopy switch for the UTFs was obtained between 20 and 40 °C, accompanied by reversible changes in surface topography and film thickness revealed by atomic force microscopy and ellipsometry, respectively. The electrochemical on-off property of the temperature-controlled (LDH/pNIPAM)(n) UTFs originates from the contraction-expansion configuration of pNIPAM with low-high electrochemical impedance. In addition, a switchable electrocatalytic behavior of the (LDH/pNIPAM)(n) UTFs toward the oxidation of glucose was observed, resulting from the temperature-controlled charge transfer rate. Therefore, this work provides a facile approach for the design and fabrication of a well-ordered command interface with a temperature-sensitive property, which can be potentially applied in electrochemical sensors and switching.

Magnetic-field-assisted assembly of layered double hydroxide/metal porphyrin ultrathin films and their application for glucose sensors.

The ordered ultrathin films (UTFs) based on CoFe-LDH (layered double hydroxide) nanoplatelets and manganese porphyrin (Mn-TPPS) have been fabricated on ITO substrates via a magnetic-field-assisted (MFA) layer-by-layer (LBL) method and were demonstrated as an electrochemical sensor for glucose. The XRD pattern for the film indicates a long-range stacking order in the normal direction of the substrate. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) images of the MFA LDH/Mn-TPPS UTFs reveal a continuous and uniform surface morphology. Cyclic voltammetry, impedance spectroscopy, and chronoamperometry were used to evaluate the electrochemical performance of the film, and the results show that the MFA-0.5 (0.5 T magnetic field) CoFe-LDH/Mn-TPPS-modified electrode displays the strongest redox current peaks and fastest electron transfer process compared with those of MFA-0 (without magnetic-field) and MFA-0.15 (0.15 T magnetic field). Furthermore, the MFA-0.5 CoFe-LDH/Mn-TPPS exhibits remarkable electrocatalytic activity toward the oxidation of glucose with a linear response range (0.1-15 mM; R(2) = 0.999), low detection limit (0.79 µM) and high sensitivity (66.3 µA mM(-1) cm(-2)). In addition, the glucose sensor prepared by the MFA LBL method also shows good selectivity and reproducibility as well as resistance to poisoning in a chloride ion solution. Therefore, the novel strategy in this work creates new opportunities for the fabrication of nonenzyme sensors with prospective applications in practical detection.

SARS-CoV-2: characterisation and mitigation of risks associated with aerosol generating procedures in dental practices.

Introduction The objectives were to characterise the particle size distribution of aerosols generated by standard dental aerosol generating procedures (AGPs) and to assess the impact of aerosol-management interventions on 'fallow time'. Interventions included combinations of high-volume intraoral suction (HVS[IO]), high-volume extraoral suction (HVS[EO]) and an air cleaning system (ACS).Method A sequence of six AGPs were performed on a phantom head. Real-time aerosol measurements (particle size range 0.0062-9.6 µm) were acquired from six locations within a typical dental treatment room (35 m3).Results The majority (>99%) of AGP particles were <0.3 µm diameter and remained at elevated levels around the dental team during the AGPs. With no active aerosol-management interventions, AGP particles were estimated to remain above the baseline range for up to 30 minutes from the end of the sequence of procedures.Conclusions The results emphasise the importance of personal protection equipment, particularly respiratory protection. Use of HVS(IO), either alone or in combination with the ACS, reduced particle concentrations to baseline levels on completion of AGPs. These data indicate potential to eliminate fallow time. The study was performed using a phantom head so confirmatory studies with patients are required.

Anionic poly(p-phenylenevinylene)/layered double hydroxide ordered ultrathin films with multiple quantum well structure: a combined experimental and theoretical study.

The sulfonated phenylenevinylene polyanion derivate (APPV) and exfoliated Mg-Al-layered double hydroxide (LDH) monolayers were alternatively assembled into ordered ultrathin films (UTFs) employing a layer-by-layer method, which shows uniform yellow luminescence. UV-vis absorption and fluorescence spectroscopy present a stepwise and regular growth of the UTFs upon increasing deposited cycles. X-ray diffraction, atomic force microscopy, and scanning electron microscopy demonstrate that the UTFs are orderly periodical layered structure with a thickness of 3.3-3.5 nm per bilayer. The APPV/LDH UTFs exhibit well-defined polarized photoemission characteristic with the maximum luminescence anisotropy of approximately 0.3. Moreover, the UTF exhibit longer fluorescence lifetime (3-3.85-fold) and higher photostability than the drop-casting APPV film under UV irradiation, suggesting that the existence of a LDH monolayer enhances the optical performance of the APPV polyanion. A combination study of electrochemistry and periodic density functional theory was used to investigate the electronic structure of the APPV/LDH system, illustrating that the APPV/LDH UTF is a kind of organic-inorganic hybrid multiple quantum well (MQW) structure with a low band energy of 1.7-1.8 eV, where the valence electrons of APPV can be confined into the energy wells formed by the LDH monolayers effectively. Therefore, this work not only gives a feasible method for fabricating a luminescence ultrathin film but also provides a detailed understanding of the geometric and electronic structures of photoactive polyanions confined between the LDH monolayers.

Ordered poly(p-phenylene)/layered double hydroxide ultrathin films with blue luminescence by layer-by-layer assembly.

Lavender layers: A poly(p-phenylene) anionic derivate and exfoliated Mg-Al layered double hydroxide monolayers were assembled into ultrathin films with well-defined blue fluorescence (see picture; the numbers indicate the number of bilayers), long-range order, and high photostability. These films work as multiple quantum-well structures for valence electrons.

Preparation of layered double hydroxides and their applications as additives in polymers, as precursors to magnetic materials and in biology and medicine.

In recent years layered double hydroxides (LDHs), also known as hydrotalcite-like materials, have attracted considerable interest from both industry and academia. In this article, we discuss methods of preparing LDHs with an emphasis on the way in which particle size and morphology can be controlled with regard to specific target applications; scale-up of one such preparation procedure is also described. In addition, we review selected applications of LDHs developed by our own and other laboratories.

Surface-confined fluorescence enhancement of Au nanoclusters anchoring to a two-dimensional ultrathin nanosheet toward bioimaging.

Gold nanoclusters (Au NCs) as ultrasmall fluorescent nanomaterials possess discrete electronic energy and unique physicochemical properties, but suffer from relatively low quantum yield (QY) which severely affects their application in displays and imaging. To solve this conundrum and obtain highly-efficient fluorescent emission, 2D exfoliated layered double hydroxide (ELDH) nanosheets were employed to localize Au NCs with a density as high as 5.44 × 10(13) cm(-2), by virtue of the surface confinement effect of ELDH. Both experimental studies and computational simulations testify that the excited electrons of Au NCs are strongly confined by MgAl-ELDH nanosheets, which results in a largely promoted QY as well as prolonged fluorescence lifetime (both ∼7 times enhancement). In addition, the as-fabricated Au NC/ELDH hybrid material exhibits excellent imaging properties with good stability and biocompatibility in the intracellular environment. Therefore, this work provides a facile strategy to achieve highly luminescent Au NCs via surface-confined emission enhancement imposed by ultrathin inorganic nanosheets, which can be potentially used in bio-imaging and cell labelling.

A monomeric photosensitizer for targeted cancer therapy.

A targeted photosensitizer used in photodynamic therapy (PDT) was fabricated by incorporation of zinc phthalocyanine (ZnPc) and folic acid (FA) into polyvinylpyrrolidone (PVP) micelles, which exhibits excellent anticancer performance revealed by both in vitro studies and in vivo tests.

Nanosheet-based titania microspheres with hollow core-shell structure encapsulating horseradish peroxidase for a mediator-free biosensor.

Nanosheet-based titania (TiO(2)) microspheres with a hollow core-shell structure have been synthesized and employed to immobilize horseradish peroxidase (HRP) in order to fabricate a mediator-free biosensor. The morphology and structure of the TiO(2) microspheres were characterized by X-ray diffraction, scanning electron microscopy and transmission electronic microscopy. A possible growth mechanism has been proposed. Spectroscopic and electrochemical measurements revealed that the TiO(2) microspheres are an immobilization support with biocompatibility for enzymes, affording good enzyme stability and bioactivity. Due to the nanosheet-based hollow core-shell structure of the TiO(2) microspheres, the direct electron transfer of HRP is facilitated and the resulting biosensor displayed good performance for the detection of H(2)O(2), with both a low detection limit of 0.05 µM and a wide linear range of 0.4-140 µM, as well as a fast response and excellent long-term stability. The nanosheet-based TiO(2) microspheres with hollow core-shell structure, can be used for the efficient entrapment of other redox-active proteins and have wide potential applications in biosensors, biocatalysis, biomedical devices and bioelectronics.

Biomimetic design and assembly of organic-inorganic composite films with simultaneously enhanced strength and toughness.

Inorganic nanoplatelet reinforced polymer films were fabricated via alternate layer-by-layer assembly of layered double hydroxide (LDH) nanoplatelets with poly(vinyl alcohol) (PVA), which showed largely enhanced strength and good ductility simultaneously.

Layer-by-layer ultrathin films of azobenzene-containing polymer/layered double hydroxides with reversible photoresponsive behavior.

We report the preparation of a reversible photoresponsive ultrathin film containing a photoactive azobenzene polymer poly{1-4[4-(3-carboxy-4-hydroxyphenylazo)benzenesulfonamido]-1,2-ethanediyl sodium salt} (PAZO) and exfoliated layered double hydroxide (LDH) nanosheets using a layer-by-layer (LBL) self-assembly technique. Alternate irradiation with UV and visible light (lambda > 450 nm) results in a reversible switching between the trans isomer and the cis-rich photostationary state of the azobenzene group with concomitant significant changes in film color. Fluorescence polarization measurements indicated that the orientation of the azobenzene chromophores in the LDH matrix undergoes a reversible realignment during the photoisomerization processes. Photoisomerization induced by alternate UV and visible light irradiation was accompanied by reversible morphological changes of the LBL film, observable by atomic force microscopy (AFM). Molecular dynamics (MD) studies demonstrated that the LDH monolayers allow sufficient free space for the PAZO to undergo isomerization of its azobenzene chromophores. The reversible photoalignment of PAZO was also followed by MD simulations, and the results are in reasonable agreement with the experimental findings, further validating the configurational and orientational changes proposed for PAZO during the reversible photoprocess. It has been demonstrated that the host (LDH nanosheet)-guest (PAZO) interactions are key factors in determining the reversible photoresponsive performances of the film, since the comparative pristine PAZO film shows no such properties. Therefore, the incorporation of a photoactive moiety within the inorganic nanosheets of LDH by the LBL technique provides an attractive and feasible methodology for creating novel light-sensitive materials and devices with potential read-write capabilities.