Multifunctional piezoelectric surfaces enhanced with layer-by-layer coating for improved osseointegration and antibacterial performance.

Implant failure is primarily caused by poor osseointegration and bacterial colonization, which demands readmissions and revision surgeries to correct it. A novel approach involves engineering multifunctional interfaces using piezoelectric polyvinylidene fluoride (PVDF) materials, which mimic bone tissue's electroactive properties to promote bone integration and provide antibacterial functionality when mechanically stimulated. In this study, PVDF films were coated with antibacterial essential oil nanoparticles and antibiofilm enzymes using a layer-by-layer (LBL) approach to ensure antibacterial properties even without mechanical stimulation. The experimental results confirmed the LBL build-up and demonstrated notable antibiofilm properties against Pseudomonas aeruginosa and Staphylococcus aureus while enhancing pre-osteoblast cell proliferation under mechanical dynamic conditions in a bioreactor that replicated the real-life environment of implants within the body. The findings highlight the potential of PVDF-coated surfaces to prevent biofilm formation and boost cell proliferation through the piezoelectric effect, paving the way for advanced implantable devices with improved osseointegration and antibacterial performance.

Fabrication of Fully Positively Charged Layer-by-Layer Polyelectrolyte Nanofilms with pH-Dependent Swelling Properties.

Nanofilms fabricated by layer-by-layer (LbL) assembly from polyelectrolytes (PEs) are important materials for various applications. However, PE films cannot retain the charges along the polymer chains during fabrication, resulting in a low charge density. In this study, the preparation of LbL nanofilms with preserved positive charges via a controllable and efficient approach was achieved. To fabricate fully positively charged (FPC) LbL nanofilms, a polycation, poly-l-lysine, was partially grafted with azide and alkyne groups. Through copper-catalyzed azide-alkyne cycloaddition and the LbL procedure, nanofilms were fabricated with all of the individual layers covalently bonded, improving the pH stability of the nanofilms. Because the resulting nanofilms had a high charge density with positive charges both inside and on the surface, they showed unique pH-dependent swelling properties and adsorption of negatively charged molecules compared with those of traditional polyelectrolyte LbL nanofilms. This kind of FPC nanofilm has great potential for use in sensors, diagnostics, and filter nanomaterials in the biomedical and environmental fields.

Enhanced filtration membranes with graphene oxide and tannic acid for textile industry wastewater dye removal.

A novel modification technique employing a layer-by-layer (LbL) self-assembly method, integrated with a pressure-assisted filtration system, was developed for enhancing a commercial polyethersulfone (PES) microfiltration (MF) membrane. This modification involved the incorporation of tannic acid (TA) in conjunction with graphene oxide (GO) nanosheets. The effectiveness of the LbL method was confirmed through comprehensive characterization analyses, including ATR-FTIR, SEM, water contact angle (WCA), and mean pore size measurements, comparing the modified membrane with the original commercial one. Sixteen variations of PES MF membranes were superficially modified using a three-factorial design, with the deposited amount of TA and GO as key factors. The influence of these factors on the morphology and performance of the membranes was systematically investigated, focusing on parameters such as pure water permeability (PWP), blue corazol (BC) dye removal efficiency, and flux recovery rate (FRR). The membranes produced with the maximum amount of GO (0.1 mg, 0.55 wt%) and TA as the inner and outer layers demonstrated remarkable FRR and significant BC removal, exceeding 80%. Notably, there was no significant difference observed when using either 0.2 (1.11 wt%) or 0.4 mg (2.22 wt%) in the first layer, as indicated by the Tukey mean test. Furthermore, the modified membrane designated as MF/TA0.4GO0.1TA0.4 was evaluated in the filtration of a simulated dye bath wastewater, exhibiting a BC removal efficiency of 49.20% and a salt removal efficiency of 27.74%. In conclusion, the novel PES MF membrane modification proposed in this study effectively enhances the key properties of pressure-driven separation processes.

Spray-assisted layer-by-layer deposition of quaternized chitosan/tannic acid for the construction of multifunctional bio-based nonwoven dressings.

Gauze wound dressings have received considerable attention due to their cost-effectiveness, excellent mechanical properties, and widespread applications. However, their inability to actively combat microorganisms and effectively scavenge free radicals results in suboptimal wound management. In this study, a novel nonwoven-based gauze dressing coated with quaternized chitosan/tannic acid (QCS/TA), based on electrostatic interaction and hydrogen bonding, was successfully prepared using a spray-assisted layer-by-layer assembly method. The bio-based nonwoven dressing, assembled with multiple interlacing bilayers, demonstrated outstanding antimicrobial properties, eliminating 99.99 % of Staphylococcus aureus (S. aureus) and 85 % of Escherichia coli (E. coli). Compared to the pristine nonwoven dressing, the QCS/TA-coated nonwoven dressing scavenged >85 % of the surrounding radicals within 2 h. Additionally, the nonwoven dressing exhibits excellent coagulation properties. Notably, the facile spraying procedure preserved most of the softness and breathability of the nonwoven substrate. After the deposition of seven bilayers, the bending stiffness and drape coefficient increased by only 37.63 % and 3.85 %, respectively, while the air permeability and moisture permeability reached 1712 mm/s and 3683.58 g/m2/d, respectively. This bio-based nonwoven dressing, derived from safe and non-toxic ingredients, holds promise as the next generation of multifunctional gauze dressings.

Over 18.2% efficiency of layer-by-layer all-polymer solar cells enabled by homoleptic iridium(III) carbene complex as solid additive.

The vertical phase distribution of active layers plays a vital role in balancing exciton dissociation and charge transport for achieving efficient polymer solar cells (PSCs). The layer-by-layer (LbL) PSCs are commonly prepared by using sequential spin-coating method from donor and acceptor solutions with distinct solvents and solvent additives. The enhanced exciton dissociation is expected in the LbL PSCs with efficient charge transport in the relatively neat donor or acceptor layers. In this work, a series of LbL all-polymer solar cells (APSCs) were fabricated with PM6 as donor and PY-DT as acceptor, and triplet material m-Ir(CPmPB)3 is deliberately incorporated into PY-DT layer to prolong exciton lifetimes of active layers. The power conversion efficiency (PCE) of LbL APSCs is improved to 18.24% from 17.32% by incorporating 0.3 wt% m-Ir(CPmPB)3 in PY-DT layer, benefiting from the simultaneously enhanced short-circuit current density (JSC) of 25.17 mA cm-2 and fill factor (FF) of 74.70%. The enhancement of PCE is attributed to the efficient energy transfer of m-Ir(CPmPB)3 to PM6 and PY-DT, resulting in the prolonged exciton lifetime in the active layer and the increased exciton diffusion distance. The efficient energy transfer from m-Ir(CPmPB)3 to PM6 and PY-DT layer can be confirmed by the increased photoluminescence (PL) intensity and the prolonged PL lifetime of PM6 and PY-DT in PM6 + m-Ir(CPmPB)3 and PY-DT + m-Ir(CPmPB)3 films. This study indicates that the triplet material as solid additive has great potential in fabricating efficient LbL APSCs by prolonging exciton lifetimes in active layers.

Trafficking through the blood-brain barrier is directed by core and outer surface components of layer-by-layer nanoparticles.

Drug-carrying nanoparticles are a promising strategy to deliver therapeutics into the brain, but their translation requires better characterization of interactions between nanomaterials and endothelial cells of the blood-brain barrier (BBB). Here, we use a library of 18 layer-by-layer electrostatically assembled nanoparticles (NPs) to independently assess the impact of NP core and surface materials on in vitro uptake, transport, and intracellular trafficking in brain endothelial cells. We demonstrate that NP core stiffness determines the magnitude of transport, while surface chemistry directs intracellular trafficking. Finally, we demonstrate that these factors similarly dictate in vivo BBB transport using intravital imaging through cranial windows in mice. We identify that hyaluronic acid surface chemistry increases transport across the BBB in vivo, and flow conditions are necessary to replicate this finding in vitro. Taken together, these findings highlight the importance of assay geometry, cell biology, and fluid flow in developing nanocarriers for delivery to the brain.

Sequential Self-Assembly of Polystyrene-block-Polydimethylsiloxane for 3D Nanopatterning via Solvent Annealing.

This study aims to develop a strategy for the fabrication of multilayer nanopatterns through sequential self-assembly of lamella-forming polystyrene-block-polydimethylsiloxane (PS-b-PDMS) block copolymer (BCP) from solvent annealing. By simply tuning the solvent selectivity, a variety of self-assembled BCP thin-film morphologies, including hexagonal perforated lamellae (HPL), parallel cylinders, and spheres, can be obtained from single-composition PS-b-PDMS. By taking advantage of reactive ion etching (RIE), topographic SiO2 monoliths with well-ordered arrays of hexagonally packed holes, parallel lines, and hexagonally packed dots can be formed. Subsequently, hole-on-dot and line-on-hole hierarchical textures can be created through a layer-by-layer process with RIE treatment as evidenced experimentally and confirmed theoretically. The results demonstrated the feasibility of creating three-dimensional (3D) nanopatterning from the sequential self-assembly of single-composition PS-b-PDMS via solvent annealing, providing an appealing process for nano-MEMS manufacturing based on BCP lithography.

A polyoxometalate/chitosan-Ti3C2Tx MXene nanocomposite constructed by electrostatically mediated strategy for electrochemical detecting L-tryptophan in milk.

L-tryptophan (L-Trp) is crucial for human metabolism, and its imbalance or deficiency can lead to certain diseases, such as insomnia, depression, and heart disease. Since the body cannot synthesize L-Trp and must obtain it from external sources, accurately monitoring L-Trp levels in food is essential. Herein, a nanocomposite film based on polyoxometalate (P2Mo17V), Ti3C2Tx MXene, and chitosan (Cs) was developed through a green electrostatically mediated layer-by-layer self-assembly strategy for electrochemical detection of L-Trp. The composite film exhibits fast electron transfer and remarkable electrocatalytic performance for L-Trp with a wide linear range (0.1-103 µM), low limit of detection (0.08 µM, S/N = 3), good selectivity, reproducibility, and repeatability. In milk sample, the recoveries of L-Trp were from 95.78% and 104.31%. The P2Mo17V/Cs-Ti3C2Tx electrochemical sensor not only provides exceptional recognition and detection capabilities for L-Trp but also shows significant potential for practical applications, particularly in food safety and quality control.

"Target-and-release" nanoparticles for effective immunotherapy of metastatic ovarian cancer.

Immunotherapies such as checkpoint inhibitors (CPI) are effective in treating several advanced cancers, but these treatments have had limited success in metastatic ovarian cancer (OC). Here, we engineered liposomal nanoparticles (NPs) carrying a layer-by-layer (LbL) polymer coating that promotes their binding to the surface of OC cells. Covalent anchoring of the potent immunostimulatory cytokine interleukin-12 (IL-12) to phospholipid headgroups of the liposome core enabled the LbL particles to concentrate IL-12 in disseminated OC tumors following intraperitoneal administration. Shedding of the LbL coating and serum protein-mediated extraction of IL-12-conjugated lipids from the liposomal core over time enabled IL-12 to disseminate in the tumor bed following rapid NP localization in tumor nodules. Optimized IL-12 LbL-NPs promoted robust T cell accumulation in ascites and tumors in mouse models, extending survival compared to free IL-12 and remarkedly sensitizing tumors to CPI, leading to curative treatments and immune memory.

Polypeptide-based multilayer nanoarchitectures: Controlled assembly on planar and colloidal substrates for biomedical applications.

Polypeptides have shown an excellent potential in nanomedicine thanks to their biocompatibility, biodegradability, high functionality, and responsiveness to several stimuli. Polypeptides exhibit high propensity to organize at the supramolecular level; hence, they have been extensively considered as building blocks in the layer-by-layer (LbL) assembly. The LbL technique is a highly versatile methodology, which involves the sequential assembly of building blocks, mainly driven by electrostatic interactions, onto planar or colloidal templates to fabricate sophisticated multilayer nanoarchitectures. The simplicity and the mild conditions required in the LbL approach have led to the inclusion of biopolymers and bioactive molecules for the fabrication of a wide spectrum of biodegradable, biocompatible, and precisely engineered multilayer films for biomedical applications. This review focuses on those examples in which polypeptides have been used as building blocks of multilayer nanoarchitectures for tissue engineering and drug delivery applications, highlighting the characteristics of the polypeptides and the strategies adopted to increase the stability of the multilayer film. Cross-linking is presented as a powerful strategy to enhance the stability and stiffness of the multilayer network, which is a fundamental requirement for biomedical applications. For example, in tissue engineering, a stiff multilayer coating, the presence of adhesion promoters, and/or bioactive molecules boost the adhesion, growth, and differentiation of cells. On the contrary, antimicrobial coatings should repel and inhibit the growth of bacteria. In drug delivery applications, mainly focused on particles and capsules at the micro- and nano-meter scale, the stability of the multilayer film is crucial in terms of retention and controlled release of the payload. Recent advances have shown the key role of the polypeptides in the adsorption of genetic material with high loading efficiency, and in addressing different pathways of the particles/capsules during the intracellular uptake, paving the way for applications in personalized medicine. Although there are a few studies, the responsiveness of the polypeptides to the pH changes, together with the inclusion of stimuli-responsive entities into the multilayer network, represents a further key factor for the development of smart drug delivery systems to promote a sustained release of therapeutics. The degradability of polypeptides may be an obstacle in certain scenarios for the controlled intracellular release of a drug once an external stimulus is applied. Nowadays, the highly engineered design of biodegradable LbL particles/capsules is oriented on the development of theranostics that, limited to use of polypeptides, are still in their infancy.

Layer-by-layer fabrication of alginate/polyethyleneimine multilayer on magnetic interface with enhanced efficiency in immuno-capturing circulating tumor cells.

BACKGROUND: The technology of capturing circulating tumor cells (CTCs) plays a crucial role in the diagnosis, evaluation of therapeutic efficacy, and prediction of prognosis in lung cancer. However, the presence of complex blood environment often results in severe nonspecific protein adsorption and interferences from blood cells, which negatively impacts the specificity of CTCs capture. There is a great need for development of novel nanomaterials for CTCs capture with prominent anti-nonspecific adsorptions from proteins or blood cells. RESULTS: We present a novel immune magnetic probe Fe3O4@(PEI/AA)4@Apt. The surface of Fe3O4 particles was modified with four layers of PEI/AA composite by layer-by-layer assembly. Furthermore, aptamers targeting epithelial marker EpCAM (SYL3C) and mesenchymal marker CSV (ZY5C) were simultaneously connected on Fe3O4@(PEI/AA)4 to improve the detection of different phenotypic CTCs and reduce false negatives. The results demonstrated that the (PEI/AA)4 coatings not only minimized non-specific protein adsorptions, but also significantly reduced the adsorption rate of red blood cells to a mere 1 %, as a result of which, the Fe3O4@(PEI/AA)4@Apt probe achieved a remarkably high capture efficiency toward CTCs (95.9 %). In the subsequent validation of clinical samples, the probe was also effective in capturing rare CTCs from lung cancer patients. SIGNIFICANCE AND NOVELTY: A (PEI/AA) polymerized composite with controllable layers was fabricated by layer-by-layer self-assembly technique, which displayed remarkable anti-nonspecific adsorption capabilities toward proteins and cells. Importantly, Fe3O4@(PEI/AA)4@Apt probe significantly improved CTCs capture purity in lung cancer patients to 89.36 %. For the first time, this study combined controllable (PEI/AA) layers with magnetic separation to innovatively build a resistant interface that significantly improves the specific capture performances of CTCs, broadening the application of this polymerized composite.

Layer-by-Layer-Processed All-Polymer Solar Cells with Enhanced Performance Enabled by Regulating the Microstructure of Upper Layer.

The layer-by-layer (LBL) fabrication method allows for controlled microstructure morphology and vertical component distribution, and also offers a reproducible and efficient technique for fabricating large-scale organic solar cells (OSCs). In this study, the polymers D18 and PYIT-OD are employed to fabricate all-polymer solar cells (all-PSCs) using the LBL method. Morphological studies reveal that the use of additives optimizes the microstructure of the active layer, enhancing the cells' crystallinity and charge transport capability. The optimized device with 2% CN additive significantly reduces bimolecular recombination and trap-assisted recombination. All-PSCs fabricated by the LBL method based on D18/PYIT-OD deliver a power conversion efficiency (PCE) of 15.07%. Our study demonstrates the great potential of additive engineering via the LBL fabrication method in regulating the microstructure of active layers, suppressing charge recombination, and enhancing the photovoltaic performance of devices.

Construction of sustainable and highly efficient fire-protective nanocoatings based on polydopamine and phosphorylated cellulose for flexible polyurethane foam.

Layer-by-layer (LBL) self-assembly is an effective strategy for constructing fire-resistant coatings on flexible polyurethane foam (FPUF), while the efficiency of fire-resistant coatings remains limited. Therefore, this study proposes an in situ flame retardancy modification combined with LBL self-assembly technology to enhance the efficiency of flame retardant coatings for FPUF. Initially, polydopamine (PDA) and polyethyleneimine (PEI) were employed to modify the FPUF skeleton, thereby augmenting the adhesion on the surface of the skeleton network. Then, the self-assembly of MXene and phosphorylated cellulose nanofibers (PCNFs) via the LBL technique on the foam skeleton network formed a novel, sustainable, and efficient flame retardant system. The final fire-protective coatings comprising PDA/PEI and MXenes/PCNF effectively prevented the collapse of the foam structure and suppressed the melt dripping of the FPUF during combustion. The peak heat release rate, the peak CO production rate and peak CO2 production rate were reduced by 68.6 %, 61.1 %, and 68.4 % only by applying a 10-bilayer coating. In addition, the smoke release rate and total smoke production were reduced by 83.3 % and 57.7 %, respectively. This work offers a surface modification approach for constructing highly efficient flame retardant coatings for flammable polymeric materials.

Structure engineering of nickel silicate/carbon composite with boosted electrochemical performances for hybrid supercapacitors.

In the wake of the carbon-neutral era, the exploration of innovative materials for energy storage and conversion has garnered increasing attention. While nickel silicates have been a focal point in energy storage research, their application in supercapacitors (SCs) has been relatively underreported due to poor conductivity. A newly designed architecture, designated as rGO@NiSiO@NiO/C (abbreviated for reduced graphene oxide (rGO), nickel silicate (NiSiO), nickel oxide/carbon (NiO/C)), has been developed to enhance the electrochemical performance of NiSiO. The incorporation of inner rGO provides structural support for NiSiO, enhancing conductivity, while the outer NiO/C layer not only boosts conductivity but also safeguards NiSiO from structural degradation and electrolyte dissolution. This architecture eliminates multi-phase mixtures, facilitating rapid electron/mass transfer kinetics and accelerating electrochemical reactions, resulting in exceptional electrochemical properties. The rGO@NiSiO@NiO/C architecture achieves a specific capacitance of 324F·g-1 at 0.5 A·g-1, with a superb cycle performance of âˆ¼ 91 % after 10,000 cycles, surpassing state-of-the-art nickel silicates. Furthermore, the hybrid supercapacitor (HSC) device incorporating the rGO@NiSiO@NiO/C electrode attains an areal capacitance of 159 mF·cm-2 at 2.5 mA·cm-2, a retention ratio of âˆ¼ 98 % after 10,000 cycles, and an energy density of 0.68 Wh·m-2 (26.7 Wh·kg-1) at 3.4 W·m-2 (343.8 W·kg-1). This study presents a layer-by-layer approach for constructing transition metal silicates/C architectures to enhance their electrochemical performance.

Wearable, Machine Washable, Breathable Polyethylenimine/Sodium Alginate Layer-by-Layer-Coated Cotton-Based Multifunctional Triboelectric Nanogenerators.

Cotton-based textiles are ubiquitous in daily life and are prime candidates for application in wearable triboelectric nanogenerators. However, pristine cotton is vulnerable to bacterial attack, lacks antioxidant and ultraviolet (UV)-protective abilities, and shows lower triboelectric charge generation against tribonegative materials because it is present in the neutral region of the triboelectric series. To overcome such drawbacks, herein, a facile layer-by-layer method is proposed, involving the deposition of alternate layers of polyethylenimine (PEI) and sodium alginate (SA) on cotton. Such modified fabric remains breathable and flexible, retains its comfort properties, and simultaneously shows multifunctionalities and improved triboelectric output, which are retained even after 50 home laundering cycles. Also, the modified fabric becomes more tribopositive than nylon, silk, and wool. A triboelectric nanogenerator consisting of modified cotton and polyester fabric is proposed that shows a maximum power density of 338 mW/m2. An open-circuit voltage of ∼97.3 V and a short-circuit current of ∼4.59 µA are obtained under 20 N force and 1 Hz tapping frequency. Further, the modified cotton exhibits excellent antibacterial, antioxidant, and UV-protective properties because of the incorporation of PEI, and its moisture management properties are retained due to the presence of sodium alginate in the layer. This study provides a simple yet effective approach to obtaining durable multifunctionalities and improved triboelectric performance in cotton substrates.

pH-response of protein-polysaccharide multilayers adsorbed on a flat gold surface: A surface plasmon resonance study.

Polysaccharide-protein multilayers (PPMLs) consisting of bovine serum albumin (BSA) and chondroitin sulfate (CS) are assembled in acidic solution (pH 4.2) via layer-by-layer deposition method. The formation of PPMLs on gold surface and their responsiveness to pH change from 4.2 to 7 is investigated by Surface Plasmon Resonance Spectroscopy. The buildup of the multilayer at pH 4.2 exhibits non-linear growth while the formation of the first layers is strongly affected by the physicochemical properties of the gold surface. Neutral solution (pH 7) affects the interactions between the biopolymers and results in a partially disassemble (disintegration) of the multilayer film. On one hand, the single pair of layers, BSA-CS and the double pair of layers, (BSA-CS)2, assemblies are stable in neutral pH, a result that will be of interest for biomedical applications. On the other hand, multilayer films consisting of more than four layers that is (BSA-CS)2

Low Fouling Polyelectrolyte Layer-by-Layer Self-Assembled Membrane for High Performance Dye/Salt Fractionation: Sequence Effect of Self-Assembly.

Layer-by-layer (LbL) self-assembly of oppositely charged polyelectrolytes (PEs) is usually performed on a conventional ultrafiltration base substrate (negative zeta potential) by depositing a cationic PE as a first layer. Herein, we report the facile and fast formation of high performance molecular selective membrane by the nonelectrostatic adsorption of anionic PE on the polyvinylidene fluoride (PVDF, zeta potential -17 mV) substrate followed by the electrostatic LbL assembly. Loose nanofiltration membranes have been prepared via both concentration-polarization (CP-LbL, under applied pressure) driven and conventional (C-LbL, dipping) LbL self-assembly. When the first layer is poly(styrene sodium) sulfonic acid, the LbL assembled membrane contains free -SO3- groups and exhibits higher rejection of Na2SO4 and lower rejection of MgCl2. The reversal of salt rejection occurs when the first layer is quaternized polyvinyl imidazole (PVIm-Me). The membrane (five layers) prepared by first depositing PStSO3Na shows higher rejection of several dyes (97.9 to >99.9%), higher NaCl to dye separation factor (52-1800), and higher dye antifouling performance as compared to the membrane prepared by first depositing PVIm-Me (97.5-99.5% dye rejection, separation factor ∼40-200). However, the C-LbL membrane requires a longer time of self-assembly or higher PE concentration to reach a performance close to the CP-LbL membranes. The membranes exhibit excellent pressure, pH (3-12), and salt (60 g L-1) stability. This work provides an insight for the construction of low fouling and high-performance membranes for the fractionation of dye and salt based on the LbL self-assembly sequence.

Chitosan/bovine serum albumin layer-by-layer assembled particles for non-invasive inhaled drug delivery to the lungs.

Layer-by-Layer (LbL) assembly of polyelectrolytes on a solid core particle is a well-established technique used to deliver drugs, proteins, regenerative medicines, combinatorial therapy, etc. It is a multifunctional delivery system which can be engineered using various core template particles and coating polymers. This study reports the development and in-vitro evaluation of LbL assembled particles for non-invasive inhaled delivery to the lungs. The LbL assembled particles were prepared by successively coating polyelectrolyte macromolecules, glycol chitosan and bovine serum albumin on 0.5- and 4.5-µm polystyrene particles. The LbL assembly of polyelectrolytes was confirmed by reversible change in zeta potential and sequential increase in the particle size after accumulation of the layer. The prepared LbL particles were further assessed for aerodynamic properties using two distinct nebulizers, and toxicity assessment in normal lung cells. The in-vitro aerosolization study performed using next generation impactor coupled with Pari LC Plus and Aeroeclipse nebulizer showed that both the LbL assembled 0.5 and 4.5-µm particles had MMAD <5 µm confirming suitable aerodynamic properties for non-invasive lung delivery. The in-vitro cytotoxicity, and TEER integrity following treatment with the LbL assembled particles in normal lung epithelial and fibroblasts showed no significant cytotoxicity rendering the LbL assembled particles safe. This study extends the efficiency of LbL assembled particles for novel applications towards delivery of small and large molecules into the lungs.

Layer-by-layer self-assembly of PLL/CPP-ACP multilayer on SLA titanium surface: Enhancing osseointegration and antibacterial activity in vitro and in vivo.

Dental Implants are expected to possess both excellent osteointegration and antibacterial activity because poor osseointegration and infection are two major causes of titanium implant failure. In this study, we constructed layer-by-layer self-assembly films consisting of anionic casein phosphopeptides-amorphous calcium phosphate (CPP-ACP) and cationic poly (L-lysine) (PLL) on sandblasted and acid etched (SLA) titanium surfaces and evaluated their osseointegration and antibacterial performance in vitro and in vivo. The surface properties were examined, including microstructure, elemental composition, wettability, and Ca2+ ion release. The impact the surfaces had on the adhesion, proliferation and differentiation abilities of MC3T3-E1 cells were investigated, as well as the material's antibacterial performance after exposure to the oral microorganisms such as Porphyromonas gingivalis (P. g) and Actinobacillus actinomycetemcomitans (A. a). For the in vivo studies, SLA and Ti (PLL/CA-3.0)10 implants were inserted into the extraction socket immediately after extracting the rabbit mandibular anterior teeth with or without exposure to mixed bacteria solution (P. g & A. a). Three rabbits in each group were sacrificed to collect samples at 2, 4, and 6 weeks of post-implantation, respectively. Radiographic and histomorphometry examinations were performed to evaluate the implant osseointegration. The modified titanium surfaces were successfully prepared and appeared as a compact nano-structure with high hydrophilicity. In particular, the Ti (PLL/CA-3.0)10 surface was able to continuously release Ca2+ ions. From the in vitro and in vivo studies, the modified titanium surfaces expressed enhanced osteogenic and antibacterial properties. Hence, the PLL/CPP-ACP multilayer coating on titanium surfaces was constructed via a layer-by-layer self-assembly technology, possibly improving the biofunctionalization of Ti-based dental implants.

Layer-by-layer Assembly of Nanosheets with Matching Size and Shape for More Stable Membrane Structure than Nanosheet-Polymer Assembly.

Layer-by-layer (LbL) assembly of oppositely charged materials has been widely used as an approach to make two-dimensional (2D) nanosheet-based membranes, which often involves 2D nanosheets being alternately deposited with polymer-based polyelectrolytes to obtain an electrostabilized nanosheet-polymer structure. In this study, we hypothesized that using 2D nanosheets with matching physical properties as both polyanions and polycations may result in a more ordered nanostructure with better stability than a nanosheet-polymer structure. To compare the differences between nanosheet-nanosheet vs nanosheet-polymer structures, we assembled negatively charged molybdenum disulfide nanosheets (MoS2) with either positively charged graphene oxide (PrGO) nanosheets or positively charged polymer (PDDA). Using combined measurements by ellipsometer and quartz crystal microbalance with dissipation, we discovered that the swelling of MoS2-PrGO in ionic solutions was 60% lower than that of MoS2-PDDA membranes. Meanwhile, the MoS2-PrGO membrane retained its permeability upon drying, whereas the permeability of MoS2-PDDA decreased by 40% due to the restacking of MoS2. Overall, the MoS2-PrGO membrane demonstrated a better filtration performance. Additionally, our X-ray photoelectron spectroscopy results and analysis on layer density revealed a clearer transition in material composition during the LbL synthesis of MoS2-PrGO membranes, and the X-ray diffraction pattern suggested its resemblance to an ordered, layer-stacked structure. In conclusion, the MoS2-PrGO membrane made with nanosheets with matching size, shape, and charge density exhibited a much more aligned stacking structure, resulting in reduced membrane swelling under high salinity solutions, controlled restacking, and improved separation performance.