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Nature-inspired small molecules such as catecholamines and polyphenols have gained a great deal of attention because of the exceptional surface-coating property that is applicable to many diverse substrates. Many researchers have conducted studies to expand molecular pools with surface-coating properties, but previous reports have still been limited to phenolic molecules as surface-coating agents. In this study, we describe for the first time the material-independent coating properties of nonphenolic molecules, namely, sulfonated pyrenes with ZrIV ions. Owing to the binding capability with several oxygen-containing ligands, ZrIV can be used for the molecular assembly of sulfonated pyrenes. We also report on the mixing of multiple sulfonated pyrenes and ZrIV results in cross-linked complexes that can coat diverse solid substrates. The resulting coating can serve as a platform for grafting functional polysaccharides.

Polyphenols containing catechol (1,2-dihydroxyphenyl)/pyrogallol (1,2,3-trihydroxyphenyl) groups have been employed as precursors to prepare substrate-independent (i.e., universal) coatings. However, quercetin, an interesting flavonol due to its unique biological properties, was previously found to be an inefficient compound for substrate coatings after screening polyphenolic compounds. We report that quercetin-based thin films could be formed on various substrates, including titanium dioxide, silicon wafers, gold, nylon, and glass, when diethylenetriamine (DETA) was used as an additive. DETA acted as a cross-linker to facilitate conjugate addition and imine formation with the catechol in quercetin. The film thickness was controllable by changing the quercetin concentration. Static water contact angles for all examined substrates converged to 25° regardless of the vastly different static water contact angles of the bare substrates, showing the universal coating capability of quercetin and DETA. Importantly, the films formed with quercetin and DETA were chemically modifiable; thus, specific functions on the surface could be introduced. α-Bromoisobutyryl bromide was immobilized on the films via esterification, and then a zwitterionic sulfobetaine polymer was subsequently grafted. Compared to the controls, the polymer-grafted surface effectively suppressed the adsorption of fibrinogen and platelets, demonstrating its non-biofouling effect. Considering its universal coating and postfunctionalization capabilities, this quercetin-based film provides a route for the preparation of functional organic coatings.

We report a facile approach for the fabrication of a marine antifouling coating using the red algae-derived polysaccharide, carrageenan (CAR). Because CAR is hydrophilic and negatively charged, we hypothesized that it would form strong hydration layers upon adsorption onto solid surfaces, thereby exhibiting marine antifouling properties. Although various types of CAR can be used for marine antifouling, a universally applicable coating method has not yet been developed; thus, a systematic study on the marine antifouling property of CAR coating is lacking. Here, we fabricated a versatile CAR coating via Zr

Enhancement of blood compatibility with the implant surface is critical for biomedical devices. Coating solid surfaces with an anticoagulant is a potentially promising strategy to improve blood compatibility with the implant surface. This study aimed to develop an approach to enhance blood compatibility with titanium/titanium dioxide (Ti/TiO2) surfaces using a green seaweed-derived polysaccharide ulvan. The approach comprises surface coating with tannic acid (TA) and grafting of ulvan onto the surface. Zirconium(IV)-based coordination linkage between ulvan and TA facilitated robust deposition of ulvan multilayers onto Ti/TiO2 surfaces. Adhesion assays revealed that more than 95% of fibrinogen adsorption and platelet adhesion was suppressed through an ulvan multilayer coating. The present results show that ulvan multilayers are robust against chemical and physical treatments and resistant to the adsorption of adherent proteins and human platelets.

A graphene aerogel (GA) with a three-dimensional (3D) structure, ultra-lightweight nature, and high hydrophobicity was simply fabricated by the one-step pyrolysis of glucose and ammonium chloride. The as-synthesized GA exhibited a 3D interconnected microporous architecture with a high surface area of ∼2860 m

Transcriptional regulator proteins are closely involved in essential survival strategies in bacteria. AcrR is a one-component allosteric repressor of the genes associated with lipid transport and antibiotic resistance. When fatty acid ligands bind to the C-terminal ligand-binding cavity of AcrR, a conformational change in the N-terminal operator-binding region of AcrR is triggered, which releases the repressed DNA and initiates transcription. This paper focuses on the structural transition mechanism of AcrR of Mycobacterium tuberculosis upon DNA and ligand binding. AcrR loses its structural integrity upon ligand-mediated structural alteration and bends toward the promoter DNA in a more compact form, initiating a rotational motion. Our functional characterization of AcrR and description of the ligand- and DNA-recognition mechanism may facilitate the discovery of new therapies for tuberculosis.

Dopamine surface chemistry has been of great interest because of its universal coating property and ability to transform nonadhesive molecules into adhesive molecules. Catechol oxidation and intramolecular cyclization underlie the unique property of dopamine (DA) surface chemistry and provide clues for developing new surface modification reagents such as norepinephrine, 5-pyrogallol-2-aminoethane, and perfluorinated DA derivatives. Based on these inspiring properties, a fast and universal surface chemistry technique using 4-(3-aminopropyl)-benzene-1,2-diol (3-catecholpropanamine, CPA) is reported herein. A single carbon insertion in the aliphatic chain of DA gives rise to the significantly accelerated intermolecular assembly and surface coating of CPA. The effect of CPA conjugation on an anticoagulant polysaccharide coating is also investigated. The use of CPA instead of DA to make polysaccharide coating materials improves the coating rate, while maintaining excellent antiplatelet performance on the coated surface.

In this work, a Prussian blue (PB)/graphene oxide (GO)/chitosan (CS) organic-inorganic composite was successfully synthesized and utilized as an adsorbent for the selective removal of cesium (Cs+) ions. Taking the advantage of synergistic effect GO, CS and PB nanoparticles, the PB/GO/CS composite exhibited maximum adsorption capacity of 48.35 mg g−1 for Cs+ ions. In the presence of competitive monovalent cations (K+ and Na+), PB/GO/CS showed excellent selectivity (86%) for Cs+ ions and had a 6-fold higher distribution coefficient (Kd) than GO/CS. This enhanced adsorption capacity with high selectivity of PB/GO/CS for Cs+ ions may have been attributed to (i) the presence of carboxylic, hydroxyl and amino functional groups on GO/CS matrix which strongly bind Cs+ ions through electrostatic attraction and chelation, and (ii) the trapping of Cs+ ions by the voids of the FCC-structured PB lattice whose size is equivalent to the hydration radius of Cs+ ions. Due to its low-cost, facile preparation, high adsorption capacity, and superior Cs+ ions selectivity, PB/GO/CS is a promising material for the selective removal of the Cs+ ions from the environment and for protecting ecosystems from the radiation hazards.

In this work, a unique one-pot green synthesis technique that utilizes high energy gamma-irradiation technology was successfully designed to fabricate a stable, highly-porous Prussian blue (PB)/polyvinylpyrrolidone (PVP)/reduced graphene oxide (rGO) aerogel (PB@PVP/rGO) with a 3D-network structure, low density, and high mechanical strength. In this synthesis process, PB nanoparticles were generated in situ and then homogenously distributed and entrapped within the PVP/rGO aerogel. The synthesized aerogel exhibited (i) a three-dimensional microporous architecture consisting of an interconnected network structure with an ultra-low density of 0.0273 g cm−3; (ii) remarkable swelling ability in the presence of water at low pH levels; and (iii) strong mechanical stability, leading to excellent deformability without cracks or the loss of structural integrity, due to the double-network structure of the PB@PVP/rGO aerogel and the crosslinking between the stiff GO sheets and the flexible PVP chains. The hydrophilic PB@PVP/rGO aerogel demonstrated the rapid adsorption of Cs+ ions and MB dye due to capillary action; based on the Langmuir model it demonstrated a maximum adsorption capacity of 143.88 and 44.73 mg g−1 for Cs+ and MB, respectively. The PB@PVP/rGO aerogel also exhibited outstanding oil absorption capacity, which we attribute to its highly interconnected porous structure and the presence of oleophilic rGO. The excellent adsorption properties coupling with the unique structural features of this PB@PVP/rGO aerogel make it a promising adsorbent for oil spills and for the removal of environmental pollutants such as Cs+ and MB in water.

N-doped graphene supported quaternary electrocatalyst (PtRuFeCo/NG) was synthesized and evaluated for potential oxygen reduction (ORR) and methanol oxidation reaction (MOR) in fuel cells. The catalyst exhibited excellent MOR (strong CO tolerance, lower onset potential), ORR (four electron transfer) activities and delivered maximum power densities of 778 and 122 mW cm−2 with direct methanol and proton exchange membrane fuel cells, respectively. The N-doping and synergistic effects of alloying low-cost Fe and Co with Pt and Ru makes PtRuFeCo/NG as excellent bifunctional catalyst that greatly reduces the processing cost of fuel cell which is the major problem facing the fuel cell industry.

Surface modification using alginic acid and its salt, alginate (Alg), has attracted much attention owing to its potential applications in various fields, including tissue engineering, drug delivery, antiplatelet surface preparation, and energy-storage technologies. In these applications, efficient immobilization of Alg on the solid surface is required because the delamination of the surface-bound Alg eventually leads to a significant decrease in its function. Therefore, much effort has been made to introduce Alg onto solid surfaces in a stable manner. Despite recent advances, existing methods for immobilizing Alg on surfaces have some limitations: (i) derivatization of Alg is typically also required and (ii) these methods only function under specific reaction conditions. Herein, we report a Zr(IV)-mediated strategy to immobilize Alg on solid surfaces. We demonstrate efficient Alg grafting onto carboxyl-, catechol-, polydopamine-, and tannic acid-functionalized surfaces via Zr(IV)-mediated cross-linking reactions. This strategy yields Alg multilayers that suppress fibroblast and platelet adhesion onto the solid surfaces. Furthermore, we show that the Alg multilayers can be selectively constructed on specific sites of solid surfaces. Given its ease of use and the wide selection of available carboxyl polymers, the current strategy is expected to be a useful tool for preparing functional polymer films for various applications.

Mussel-inspired surface chemistry, in which catechol derivatives play an important role, has garnered extensive research interest owing to material-independent surface coating capability and easy implementation to a wide range of applications. Generally, sequential reactions comprising catechol oxidation, intramolecular reaction of oxidized catechols with nucleophiles, and intermolecular assembly result in polymers that can adhere to many diverse surfaces. Although amines and thiols have similar reactivity toward oxidized catechols, most studies have been conducted with catechol and amine groups as essentials. Surface coating with catechol-thiol has not been investigated. In this study, we show that 4-(2-mercapto-ethyl)-benzene-1,2-diol (catechol-thiol) can serve as a surface coating agent in the presence of a strong oxidant. A wide range of materials are coated with catechol-thiol, and an additional grafting of the functional molecules onto the surface is also performed through well-established thiol chemistry, Michael addition, and thiol-ene reaction.

Consumption of sunset yellow (SY) above a certain concentration through food products may leads to adverse health issues. Therefore, it is imperative to develop technologies for rapid and selective detection of SY. Herein, a flower-like reduced graphene oxide (rGO)-graphitic carbon nitride (g-CN)/ZnO-Au nanoparticle (NPs) has been prepared and utilized for the specific detection of SY. The fabricated rGO-g-CN/ZnO-AuNPs composite was characterized and investigated by XRD, FTIR, SEM, TEM, XPS, EIS, and voltammetry techniques. Characterization techniques elucidated the deposition of ZnO-AuNPs on to the rGO-g-CN and successful fabrication of rGO-g-CN/ZnO-AuNPs composite. rGO-g-CN/ZnO-AuNPs composite possesses excellent catalytic activity for the oxidation of SY. Developed rGO-g-CN/ZnO-AuNPs sensor exhibits LOD of 1.34 nM for SY concentrations ranging from 5 to 85 nM. Noteworthily, the sensor has been successfully employed for the detection and recovery of SY in real-time samples. Fabricated composite opens up new avenues to develop electrochemical sensor for food safety.

We synthesized a zwitterionic dopamine derivative ( ZW-DOPA) containing both catechol and amine groups, and we demonstrated an excellent marine antifouling surface by controlling the oxidation of ZW-DOPA. The oxidation was mediated by the deprotonation of catechol or the addition of an oxidant (ammonium persulfate (AP) or sodium periodate (NaIO4)). The oxidation and subsequent molecular transformation of ZW-DOPA was investigated over time by UV-vis spectroscopy. Among the different oxidation conditions tested, NaIO4-induced ZW-DOPA coating was the most efficient and successfully formed on various substrates, such as titanium dioxide, stainless steel, and nylon. Compared with uncoated substrates, ZW-DOPA-coated substrates showed high resistance to marine diatom adhesion. Considering the ease of use and substrate independence of the ZW-DOPA coating, this method shows promise as a basis for inhibiting marine fouling on a variety of substrates used in the marine industry and aquatic environments.

In this work, multifunctional Fe-aminoclay (FeAC)/carboxymethyl cellulose (CMC)/ polyhedral oligomeric silsesquioxane (POSS) composite (FeAC/CMC/POSS) with layered structure was successfully synthesized and utilized as adsorbent for the removal of cesium ions (Cs+) and cationic dyes methylene blue (MB) and chrysoidine G (CG) from aqueous solutions. The FeAC/CMC/POSS exhibit excellent adsorption capacities for Cs+ ions, MB and CG of 152, 438, and 791 mg g–1, respectively. The adsorption capacities for Cs+ ions, MB and CG are substantially greater than those of many previously reported adsorbents due to (i) the layered morphology of the composite and abundance of amino (−NH2) groups on clay surface and (ii) existence of carboxylate (−COO–) and hydroxyl (−OH–) groups on the CMC backbone, which contribute to the adsorption of large number of Cs+ ions and dye molecules through electrostatic attraction and ion-exchange process. More importantly, the incorporation of POSS increases the interlayer spacing of Fe-a...

A customized droplet-based microfluidic reactor was fabricated for the synthesis of silver nanoparticles (Ag NPs) using silver nitrate (AgNO3) and branched polyethyleneimine (BPEI) as a precursor and a reducing agent, respectively. The effects of static mixing, temperature, and the volumetric flow rates of AgNO3 and BPEI on the particle size were investigated. The use of a static mixer and the optimization of the reaction temperature enhanced the monodispersity of the Ag NPs. In addition, the size of the Ag NPs was manipulated by changing the flow rate ratio of AgNO3 to BPEI at 60 °C for 60 min.

Here, we designed and synthesized a recoverable multifunctional adsorbent using a microfluidic reaction system and evaluated the removal performance of the smart adsorbent toward radioactive cesium as a model sample. Prussian blue-laden magnetic micro-adsorbents (PB-MNPs-MAs) with uniform morphology and monodispersity were generated via two-step sequential procedures using a glass capillary microfluidic system, followed by chemical co-precipitation with a high production rate. The cesium removal efficacy of the PB-MNPs-MAs was analyzed based on Langmuir and Freundlich isotherms by controlling adsorption parameters such as adsorbent size, initial cesium concentration, and contact time. The adsorption isotherm of the PB-MNPs-MAs was better fitted to the Langmuir model with a maximum cesium adsorption capacity of 58.73 mg g−1, which was 40% higher than that of macro-adsorbents in a dynamic magnetic field. This result can be attributed to their large specific area, which increased the kinetic rate of cesium adsorption and achieved saturation within 20 min. Additionally, the PB-MNPs-MAs were recovered from wastewater within 5 s under a static magnetic field, indicating their great potential for magnetic actuation. We believe that our PB-MNPs-MAs can encapsulate nano-functional adsorbents and prevent actuation, making them promising for environmental remediation and especially for removal of radionuclides.

In this work, we prepared two-dimensional (2D) stack-structured aminopropylIsobutyl polyhedral oligomeric silsesquioxane (POSS-NH2) intercalated titanium carbide (Ti3C2Tx) MXene material (Ti3C2Tx/POSS-NH2) using a post-intercalation strategy as a potential adsorbent for the removal of cesium (Cs+) and strontium (Sr2+) ions from aqueous solutions. Ti3C2Tx/POSS-NH2 exhibited unprecedented adsorption capacities of 148 and 172 mg g−1 for Cs+ and Sr2+ ions, respectively. Batch adsorption experimental data well fitted the Freundlich isotherm model, which revealed multilayer adsorption of Cs+ and Sr2+ ions onto heterogeneous –OH, –F, –O, and –NH2 adsorption sites of Ti3C2Tx/POSS-NH2 with different energies. Ti3C2Tx/POSS-NH2 exhibited rapid Cs+/Sr2+ ions adsorption kinetics and attained equilibrium within 30 min. Also, Ti3C2Tx/POSS-NH2 exhibited recyclable capability over three cycles and remarkable selectivities of 89% and 93% for Cs+ and Sr2+ ions, respectively, in the presence of co-existing mono- and divalent cations. We suggest the high adsorption capacity of Ti3C2Tx/POSS-NH2 might be due to the synergistic effects of (i) increased inter-lamellar distance between Ti3C2Tx galleries due to POSS-NH2 intercalation, enabling diffusion and encapsulation of large numbers of Cs+/Sr2+ ions, (ii) strong complexation of amine (–NH2) groups of POSS-NH2 with Cs+/Sr2+ ions, and (iii) the presence of large numbers of heterogeneous surface functional groups (e.g., –OH, –F, and –O), which resulted in the adsorptions of Cs+/Sr2+ ions through electrostatic, ion exchange, and surface complexation mechanisms. Given the extraordinary adsorption capacities observed, intercalation appears to be a promising strategy for the effective removal of radioactive Cs+ and Sr2+ ions from aqueous media.

In this study, we have synthesized N-doped graphene (NG) supported ternary PtRuFe nanocatalyst with size ranging from 2 to 3 nm using microwave-assisted polyol method and evaluated its electrochemical activity towards methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR) in direct methanol fuel cell (DMFC) and proton exchange membrane fuel cell (PEMFC), respectively. The as-prepared bifunctional PtRuFe/NG catalyst exhibited excellent electrocatalytic activity towards both MOR and ORR. During MOR, the PtRuFe/NG catalyst showed the stronger CO tolerance, lower onset potential, and higher methanol oxidation current than that of its un-doped counterpart (PtRuFe/rGO). In ORR, the catalyst exhibited higher oxygen reduction current with four electron transfer. The maximum power density delivered by PEMFC and DMFC using PtRuFe/NG were 870 and 112 mW cm−2, respectively, which are 25% higher than that of its un-doped counterpart. Also PtRuFe/NG showed 2- to 3-fold improvement in MOR, ORR, PEMFC and DMFC performances as compared with previously reported values of mono-, bi-, and tri-metallic catalysts supported on NG and other carbon substrates. The enhanced electrochemical activity may be attributed to the synergetic effect of nitrogen-doping along with the bi-functional and ligand effects of alloying low-cost Fe with Pt and Ru. The bifunctional ternary PtRuFe nanocatalysts supported on N-doped graphene has excellent potential to catalyze both MOR and ORR with remarkable reduction in the processing cost of fuel cells which is the primary problem facing the commercialization of fuel cells.

The authors describe an electrochemical sensor for nitrite that is based on the use of a screen printed carbon electrode modified with palladium nanoparticles and an amino-functionalized metal-organic framework. The morphology and properties of the resulting material were examined by X-ray photoelectron spectroscopy, X-ray diffraction, thermogravimetry, FTIR spectroscopy and transmission electron microscopy. Nitrite was chosen as a model analyte to evaluate the electron transfer performance of the modified SPCE. Its preparation conditions were optimized. The response to nitrite was studied via cyclic voltammetry, linear sweep voltammetry, and square wave voltammetry. Under the optimal conditions, the oxidation current (typically measured at −0.86 V vs Ag/AgCl) increases linearly in the 5 to 150 nM nitrite concentration range, and the detection limit is 1.3 nM. The sensor was applied to the detection of nitrite in (spiked) sausage and pickle samples. It is highly selective to nitrite in the presence of high concentrations of other electro-active compounds, stable, and well reproducible. In our perception, the sensor presented here reveals the large potential of MOF-based hybrid materials for use as an electrode material.

A facile approach to enhancing the blood compatibility of solid surfaces based on ZrIV -heparin complexation is reported. Solid surfaces are pretreated with tannic acid (TA)/ZrIV complexes. Heparin is then deposited on the surface through a spin-coating process and fixed by a ZrIV -mediated crosslinking reaction. Using this approach, TA/ZrIV /heparin complex multilayers that are highly resistant to human platelet adhesion are formed on various substrates including metal, metal oxides, ceramics, and synthetic polymers. This approach presents a sustainable way for the immobilization of heparin onto surfaces because it does not require any derivatization of heparin molecule as well as time-consuming processes.

The original version of this article unfortunately missed Prof. A.T. Ezhil Vilian’s project number in Acknowledgements. The missing project number is 2017R1D1A1B03034977.

In current work, Prussian blue (PB)- and hydroxyapatite (HAp)-embedded micro-adsorbents (PB-HAp-MAs) were rationally fabricated through an easy and flexible custom-made micronozzle system as a novel bifunctional adsorbent. The adsorption performance of the as–prepared samples was conducted based on the removal of cesium (Cs+) and strontium (Sr2+) ions. Adsorption behaviors of the PB-HAp-MAs were also evaluated as function extrusion dimensions and adsorbate concentration. The adsorption isotherm was well fitted by the Langmuir model with adsorption capacities of 24.688 mg g−1 and 29.254 mg g−1 for Cs+ and Sr2+, respectively. Specially, the enhanced adsorption activity can be synergistically attributed to the porous nature of the developed alginate backbone with a high surface area of encapsulated functional nanoparticles, thus leading to rapid saturation within 1 min. In addition, the as-synthesized PB-HAp-MAs were successfully separated from the aqueous solution within 10 s by applying a magnetic field. We expect that our findings will provide valuable guidelines towards developing highly efficient adsorbents for environmental remediation.

Dry cleaning process has been limited to particular field of removing native oxide because it has low etching selectivity for various oxide films. To increase etching selectivity, we added H2O steam feeding step before NF3 feeding step. From the experimental, we can change selectivity between oxide films from tens to hundreds.

In this research, we successfully synthesized a reduced graphene oxide/tin oxide (rGO/SnO2) composite for the electrochemical detection of fungal contaminant, patulin (PAT) that does not require a biological or chemical receptor or specific antibodies. The resulting rGO/SnO2 composite exhibited promising electrochemical properties and demonstrated outstanding performance in the direct measurement of PAT levels in contaminated apple juice samples. The differential pulse voltammetric response of the rGO/SnO2 composite electrode exhibited a linear relationship with PAT concentration in the 50–600 nM range and had a lower detection limit of 0.6635 nM. The sensor electrode exhibited high sensitivity, reliable reproducibility, and good selectivity. The designed electrochemical sensor was also tested against the time-consuming and conventional high-performance liquid chromatography (HPLC) approach for the detection of PAT in spiked apple juice samples. We found that the electrochemical sensor had ability to rapidly detect PAT in apple juice samples without the need of extraction or clean-up steps and achieved a higher recovery rate (74.33 ± 0.70 to 99.26 ± 0.70%) within a short-time analysis than did by the HPLC (61.97 ± 1.78 to 84.31 ± 1.96%), thus illustrating its feasibility for use in agricultural and food safety industries.

The primary objective of this review article is to summarize the development and structural diversity of 2D/3D molybdenum disulfide (MoS2) based modified electrodes for electrochemical sensors and biosensor applications. Hydrothermal, mechanical, and ultrasonic techniques and solution-based exfoliation have been used to synthesize graphene-like 2D MoS2 layers. The unique physicochemical properties of MoS2 and its nanocomposites, including high mechanical strength, high carrier transport, large surface area, excellent electrical conductivity, and rapid electron transport rate, render them useful as efficient transducers in various electrochemical applications. The present review summarizes 2D/3D MoS2-based nanomaterials as an electrochemical platform for the detection and analysis of various biomolecules (e.g., neurotransmitters, NADH, glucose, antibiotics, DNA, proteins, and bacteria) and hazardous chemicals (e.g., heavy metal ions, organic compounds, and pesticides). The substantial improvements that have been achieved in the performance of enzyme-based amperometry, chemiluminescence, and nucleic acid sensors incorporating MoS2-based chemically modified electrodes are also addressed. We also summarize key sensor parameters such as limits of detection (LODs), sensitivity, selectivity, response time, and durability, as well as real applications of the sensing systems in the environmental, pharmaceutical, chemical, industrial, and food analysis fields. Finally, the remaining challenges in designing MoS2 nanostructures suitable for electroanalytical applications are outlined. Graphical abstract • MoS2 based materials exhibit high conductivity and improved electrochemical performance with great potential as a sensing electrode. • The role of MoS2 nanocomposite films and their detection strategies were reviewed. • Biomarkers detection for disease identification and respective clinical treatments were discussed. • Future Challenges, as well as possible research development for "MoS2 nanocomposites", are suggested.

In this work, we elucidate polymer-layered hollow Prussian blue-coated magnetic nanocomposites as an adsorbent to remove radioactive cesium from environmentally contaminated water. To do this, Fe3O4 nanoparticles prepared using a coprecipitation method were thickly covered with a layer of cationic polymer to attach hollow Prussian blue through a self-assembly process. The as-synthesized adsorbent was confirmed through various analytical techniques. The adsorbent showed a high surface area (166.16 m2/g) with an excellent cesium adsorbent capacity and removal efficiency of 32.8 mg/g and 99.69%, respectively. Moreover, the superparamagnetism allows effective recovery of the adsorbent using an external magnetic field after the adsorption process. Therefore, the magnetic adsorbent with a high adsorption efficiency and convenient recovery is expected to be effectively used for rapid remediation of radioactive contamination.

The control of biofouling, which is the unwanted adsorption of biomolecules and organisms on solid surfaces, is a prerequisite for wider applicability of the functional materials that are currently being used in biomedical industries. One of the frequently used methods for controlling biofouling is the use of surface coatings with antifouling materials. Herein, fucoidan, which is a marine-derived polysaccharide, is reported as a new type of antifouling material that is safe and broadly applicable. Fucoidan is conjugated with catechols, which are known to act as adhesives for grafting functional molecules onto solid substrates. Fucoidan catechol (FD-C) is subsequently utilized for robust fucoidan coatings of solid substrates, and the FD-C-coated surfaces show excellent antifouling capability for fouling organisms, including platelets and bacteria. The FD-C coating is also confirmed to be nonirritating upon skin contact, demonstrating its potential use in public places for inhibiting contagions.

Despite scientific progress in the study of Alzheimer's disease (AD), it is still challenging to develop a robust and sensitive methodology for the early diagnosis of AD due to the lack of a decisive biomarker in blood. Recent reports on the oligomer amyloid β (Aβ) as a biomarker demonstrated its possibility for identifying early onset of AD in patients, but its low concentration in blood requires highly reliable detection techniques. To overcome the low reliability and labor-intensive procedures of conventional enzyme-linked immunosorbent assay (ELISA), we present a magnetic bead-droplet immunoassay platform for simple and highly sensitive detection of oligomer Aβ for the diagnosis of AD. This microchip consists of chambers that contain water-based reagents or oil for consecutive assay procedures, and there are arrays of micro-pillars fabricated between the two adjacent chambers to form robust water-oil interfaces. With the aid of these micro-pillars, magnetic beads can stably pass through each chamber by linearly actuating a magnet along the microchip. The robust water-oil interface and simple procedures of the assay make it possible to obtain reliable results from this microchip. The intensity of the fluorescence at the read-out chamber increased quantitatively and linearly, depending on the amount of serially-diluted standard Aβ solution. The results of the assay indicated that the limit of detection was about 10 pg/mL even though it was done with manual manipulation of the magnet. This platform simplified the complicated ELISA procedure and achieved high sensitivity that was no lower than that of the conventional magnetic bead immunoassay. The magnetic bead-droplet platform reduced the assay time to 45 min, and it also reduced the amount of antibody usage in a single diagnosis significantly (10-30 ng of antibody per single assay). Consequently, this microfluidic chip has strong potential as a feasible system for use in the diagnosis of AD with a fast and easy immunoassay process, since the suggested platform can be automated with ease for point-of-care testing as well as high-throughput diagnostic equipment.

The design and development of fluorescent chemosensors have recently been the focus of considerable attention for the sensitive and specific detection of environmentally and biologically relevant metal ions in aqueous solutions and in living cells. Herein, we report photophysical results for a 1 H -pyrrole-2-carboxaldehyde-substituted rhodamine 6G derivative (RCS) that possesses specific binding affinity toward Al 3+ and Cu 2+ at micromolar concentration levels. In an N , N -dimethylformamide (DMF) and water (v/v = 2/8) medium, the RCS chemosensor exhibits a substantially enhanced absorbance intensity at 532 nm and a color change from colorless to pink for Cu 2+ ; it also exhibits significant “off–on” fluorescence at 557 nm, accompanied by a color change from colorless to fluorescent-yellow upon binding to Al 3+ . The RCS sensor exhibits extremely high fluorescence enhancement upon complexation with Al 3+ , and it can be used as a “naked eye” sensor. Through fluorescence titration at 557 nm, we confirmed that RCS exhibits a fluorescence response with a remarkable enhancement in emission intensity resulting from the complexation between RCS and Al 3+ , whereas no emission appeared in the case of competitive metal ions (Cu 2+ , Al 3+ , Li + , Na + , K + , Cs + , Mg 2+ , Ca 2+ , Fe 2+ , Co 2+ , Ag + , Zn 2+ , Cd 2+ , Hg 2+ and Pb 2+ ) in a DMF and water (v/v = 2/8) solution. The reversible ring-opening mechanism of the rhodamine spirolactam induced by Al 3+ /Cu 2+ binding and the 1:1 stoichiometric structure between RCS and Al 3+ were adequately supported by Job-plot evaluation, optical titration and FT-IR analysis. The lowest detection limit for Al 3+ is 3.20 × 10 6 M −1 in a DMF and water (v/v = 2/8) solution. Al 3+ -induced chelation-enhanced fluorescence (CHEF) is associated with spirolactam ring opening of the rhodamine unit. Finally, RCS was successfully applied for the bio-imaging of Al 3+ in living HeLa cells and for fluorescence imaging of a microfluidic system.

We report a perfluoroaryl azide-based photoreaction for synthesizing functionalizable and nonbiofouling poly[oligo(ethylene glycol) methacrylate] (pOEGMA) films on a chemically inert COC substrate, and an estimation of a surface coverage of the antibody immobilized onto the surface with the immuno-gold nanoparticles. The processes were confirmed by water contact angle measurement, FT-IR spectroscopy, and FE-SEM. The strategy demonstrated in this work could be applied to functionalizations of other polymeric materials and determination of the binding capacity of analytes in biosensors and microfluidic devices.

In the present study, we successfully synthesized a porous three-dimensional Prussian blue-cellulose aerogel (PB-CA) composite and used it as a decorporation agent for the selective removal of ingested cesium ions (Cs+) from the gastrointestinal (GI) tract. The safety of the PB-CA composite was evaluated through an in vitro cytotoxicity study using macrophage-like THP-1 cells and Caco-2 intestinal epithelial cells. The results revealed that the PB-CA composite was not cytotoxic. An adsorption study to examine the efficiency of the decorporation agent was conducted using a simulated intestinal fluid (SIF). The adsorption isotherm was fitted to the Langmuir model with a maximum Cs+ adsorption capacity of 13.70 mg/g in SIF that followed pseudo-second-order kinetics. The PB-CA composite showed excellent stability in SIF with a maximum Cs+ removal efficiency of 99.43%. The promising safety toxicology profile, remarkable Cs+ adsorption efficacy, and excellent stability of the composite demonstrated its great potential for use as an orally administered drug for the decorporation of Cs+ from the GI tract.

We report an effective and versatile approach to control marine fouling on artificial surfaces based on specific chemical interactions found in marine mussels. The approach consists of mussel-inspired polydopamine coating, spin-coating-assisted deposition of poly(ethylene glycol) (PEG) catechols, and their cross-linking via catechol–Fe3+–catechol interactions. Using this approach, multilayered PEG films that were highly resistant to marine diatom adhesion were successfully constructed on various substrates, such as stainless steel, nylon, titanium oxide, and silicon oxide. We believe that our results will provide a basis for the construction of a marine antifouling agent that can be applied by a large variety of industries owing to its applicability to different types of substrates and stability under marine environments.

The surface coating of solid substrates using dextrans has gained a great deal of attention, because dextran-coated surfaces show excellent anti-fouling property as well as biocompatibility behavior. Much effort has been made to develop efficient methods for grafting dextrans on solid surfaces. This led to the development of catechol-conjugated dextrans (Dex-C) which can adhere to a number of solid surfaces, inspired by the underwater adhesion behavior of marine mussels. The present study is a systematic investigation of the characteristics of surface coatings developed with Dex-C. Various Dex-C with different catechol contents were synthesized and used as a surface coating material. The effect of catechol content on surface coating and antiplatelet performance was investigated.

Curry stains on clothes and dishes in daily life inspired us to investigate the potential use of turmeric powder, the major ingredient in curry, as a universal coating material. After condition optimization, the coating solution was made by boiling and filtering a turmeric slurry, and the coating was formed at pH 3, leading to the formation of ultrathin, transparent films. Various inorganic and polymeric substrates were successfully coated with turmeric-based materials, including gold, TiO2, SiO2, glass, stainless steel, indium tin oxide, nylon, polyethylene, polycarbonate, polypropylene, acryl, and poly(ethylene terephthalate). The turmeric-based coating was also applied to poly(tetrafluoroethylene) (PTFE, Teflon) and cyclic olefin copolymer (COC), and after double dip-coating, the water contact angle was changed from 118.2° to 49.1° for PTFE and from 91.2° to 44.7° for COC. The water contact angles for the other substrates converged to 35° after coating, confirming the substrate-independent universal co...

Herein we demonstrate a systematic investigation of chemically functionalizable, non-biofouling agarose films over large-area glass surfaces. Agarose films, prepared with various concentrations of aqueous agarose, were activated by using periodate oxidation to generate aldehyde groups at the termini of the agarose chains. The non-biofouling efficacy and binding capabilities of the activated films were evaluated by using protein and cellular patterning, performed by using a microarrayer, microcontact printing, and micromolding in capillaries. Characterization by using a fluorescence slide scanner and a scanning-probe microscope revealed that the pore sizes of the agarose films played an important role in achieving desirable film performance; the 0.2 wt % agarose film exhibited the optimum efficacy in this work.

This study presents a micromolding for the synthesis of Janus particles with reconfigurable shape by pH stimuli. First, we use acrylic acid (AA) as pH responsive monomer in the hydrophilic part and trimethylolpropane triacylate (TMPTA) in the hydrophobic part, respectively. The change of acidity in solvent induces the swelling of hydrophilic part in the Janus particles. The pH-responsive Janus particles show different swelling ratio of hydrophilic part in according to composition of acrylic acid in diverse range (0-70% v/v) and pH (3-11). As the concentration of acrylic acid in the hydrophilic part and environmental pH increase, the hydrophilic part in the Janus particles is proportionally swelled. Second, we fabricate novel type of Janus particles with two different hydrophilicities. As a proof of concept, we have applied acrylic acid (AA) and 2-(dimethylamino)ethyl methacrylate (DAEMA) into each part because the monomers provide reverse responsive activity. As expected, these Janus particles show different shape anisotropies with reconfigurable property in accordance with the polarity of each part at same acidity of environ- mental solvent. We envision that the stimuli responsive Janus particles have a wide application from fundamental science to diagnostic apparatus.

FolC plays important roles in the folate metabolism of cells by attaching l-Glu to dihydropteroate (DHP) and folate, which are known activities of dihydrofolate synthetase (DHFS) and folylpolyglutamate synthetase (FPGS), respectively. Here, we determined the crystal structure of Helicobacter pylori FolC (HpFolC) at 1.95 &Aring, resolution using the single-wavelength anomalous diffraction method. HpFolC has globular N- and C-terminal domains connected by a single loop, and a binding site for ATP is located between the two domains. Apo-HpFolC was crystallized in the presence of citrate in a crystallization solution, which was held in the ATP-binding site. Structural motifs such as the P-loop and &Omega, loop of HpFolC for binding of ATP and two magnesium ions are well conserved in spite of the low overall sequence similarity to other FolC/FPGSs. The &Omega, loop would also recognize a folate molecule, and the DHP-binding loop of HpFolC is expected to exhibit a unique recognition mode on DHP, compared with other FolCs. Because human FolC is known to only exhibit FPGS activity, the DHFS activity of bacterial FolC is an attractive target for the eradication of pathogenic bacteria. Consequently, our structural analyses of HpFolC provide a valuable foundation for a universal antibacterial strategy against H. pylori as well as other pathogenic bacteria.

We present a surfactant-free fabrication method for simultaneous generation of monodisperse microspheres with controllable size manner. Droplets that become microspheres by solidification processes are made in a two-step process: capillary rising-induced fluid division and wetting of immiscible fluid in a micromold. Design of the mold geometry and the monomer concentration primarily determines the microsphere size and the size distribution. Furthermore, the synergistic effect of two parameters is able to efficiently manipulate the microsphere sizes from submicrometers to a few hundred micrometers.

Cell nanoencapsulation, generating cell-in-shell structures ("artificial spores"), provides a chemical toolbox for controlling the cellular behaviors and functional characteristics of individual cells. Among the shell materials studied so far, naturally occurring polyphenolic compounds, including polydopamine and tannic acid, have intensively been employed in cell-surface engineering, because their material-independent coating property eliminates an extra priming step for inducing subsequent shell formation. Albeit successful in generating cell-in-shell structures, the coating of polyphenolic compounds generally requires alkaline conditions and/or high salt conditions, which are not compatible with certain cell types. In this work, we demonstrate that the nanocoating of individual cells with a plant-derived phenolic compound, pyrogallol (1,2,3-trihydroxybenzene), occurs at mildly alkaline pH of 7.8 in an isotonic buffer. Three different cell types (anucleate, microbial, and mammalian cells) are coated with pyrogallol without noticeable decrease in cell viability. The protocol developed in this work could be applied to other polyphenolic compounds, and, considering the many polyphenols identified as a coating material, provides an advanced chemical tool in cell-surface engineering.

A novel microporous three-dimensional pomegranate-like micro-scavenger cage (P-MSC) composite has been synthesized by immobilization of iron phyllosilicates clay onto a Prussian blue (PB)/alginate matrix and tested for the removal of radioactive cesium from aqueous solution. Experimental results show that the adsorption capacity increases with increasing the inactive cesium concentration from 1 ppm to 30 ppm, which may be attributed to greater number of adsorption sites and further increase in the inactive cesium concentration has no effect. The P-MSC composite exhibit maximum adsorption capacity of 108.06 mg of inactive cesium per gram of adsorbent. The adsorption isotherm is better fitted to the Freundlich model than the Langmuir model. In addition, kinetics studies show that the adsorption process is consistent with a pseudo second-order model. Furthermore, at equilibrium, the composite has an outstanding adsorption capacity of 99.24% for the radioactive cesium from aqueous solution. This may be ascribed to the fact that the AIP clay played a substantial role in protecting PB release from the P-MSC composite by cross-linking with alginate to improve the mechanical stability. Excellent adsorption capacity, easy separation, and good selectivity make the adsorbent suitable for the removal of radioactive cesium from seawater around nuclear plants and/or after nuclear accidents.

In this study, we developed an integrative bioinspired approach that improves the power and safety of Li-ion batteries (LIBs) by the surface modification of polyethylene (PE) separators. The approach involves the synthesis of a diatom-inspired silica layer on the surface of the PE separator, and the adhesion of the silica layer was inspired by mussels. The mussel- and diatom-inspired silica coating increased the electrolyte wettability of the separator, resulting in enhanced power and improved thermal shrinkage, resulting safer LIBs. Furthermore, the overall processes are environmentally friendly and cost-effective. The process described herein is the first example of the use of diatom-inspired silica in practically important energy storage applications. The improved wetting and thermal properties are critical, particularly for large-scale battery applications.

The direct synthesis of hydrogen peroxide (DSHP) from H2 and O2 is conceptually the most ideal and straightforward reaction for producing H2O2 in industry. However, precisely tailored catalysts are...

Heparin immobilization on surfaces has drawn a great deal of attention because of its potential application in enhancing blood compatibility of various biomedical devices such as catheters, grafts, and stents. Existing methods for the heparin immobilization are based on covalent linkage formation and electrostatic interaction between substrates and heparin molecules. However, complicated multistep procedures and uncontrolled desorption of heparin are limitations of these methods. In this work, we report a new heparin derivative that exhibits robust adhesion on surfaces. The derivative, called hepamine, was prepared via conjugation of dopamine, a mussel-inspired adhesive moiety, onto a heparin backbone. Immersion of poly(urethane) substrates into an aqueous solution of hepamine resulted in robust heparin coating of the poly(urethane), the most widely used polymeric material for blood-contacting medical devices. The hepamine-coated poly(urethane) substrate showed significant inhibition of blood coagulation and platelet adhesion. The use of hepamine for surface modification is advantageous for several reasons: for example, no chemical pretreatment of the substrates is necessary, and surface functionalization is a simple, one-step procedure. Thus, the heparin immobilization method described herein is an excellent alternative approach for the introduction of heparin molecules onto surfaces.