We report the preparation of free-standing flexible conductive reduced graphene oxide/Nafion (RGON) hybrid films by a solution chemistry that utilizes self-assembly and directional convective-assembly. The hydrophobic backbone of Nafion provided well-defined integrated structures, on micro- and macroscales, for the construction of hybrid materials through self-assembly, while the hydrophilic sulfonate groups enabled highly stable dispersibility ( approximately 0.5 mg/mL) and long-term stability (2 months) for graphene. The geometrically interlocked morphology of RGON produced a high degree of mechanical integrity in the hybrid films, while the interpenetrating network constructed favorable conduction pathways for charge transport. Importantly, the synergistic electrochemical characteristics of RGON were attributed to high conductivity (1176 S/m), facilitated electron transfer (ET), and low interfacial resistance. Consequently, RGON films obtained the excellent figure of merit as electrochemical biosensing platforms for organophosphate (OP) detection, that is, a sensitivity of 10.7 nA/microM, detection limit of 1.37 x 10(-7) M, and response time of <3 s. In addition, the reliability of RGON biosensors was confirmed by a fatigue test of 100 bending cycles. The strategy described here provides insight into the fabrication of graphene and hybrid nanomaterials from a material perspective, as well as the design of biosensor platforms for practical device applications.
2D nanomaterials have been found to show surface‐dominant phenomena and understanding this behavior is crucial for establishing a relationship between a material's structure and its properties. Here, the transition of molybdenum disulfide (MoS2) from a diffusion‐controlled intercalation to an emergent surface redox capacitive behavior is demonstrated. The ultrafast pseudocapacitive behavior of MoS2 becomes more prominent when the layered MoS2 is downscaled into nanometric sheets and hybridized with reduced graphene oxide (RGO). This extrinsic behavior of the 2D hybrid is promoted by the fast Faradaic charge‐transfer kinetics at the interface. The heterostructure of the 2D hybrid, as observed via high‐angle annular dark field–scanning transmission electron microscopy and Raman mapping, with a 1T MoS2 phase at the interface and a 2H phase in the bulk is associated with the synergizing capacitive performance. This 1T phase is stabilized by the interactions with the RGO. These results provide fundamental insights into the surface effects of 2D hetero‐nanosheets on emergent electrochemical properties.
Nanometer-scale metal particles are finding many applications in the fields of biology and nanotechnology owing to their unique optical and magnetic properties. Phytochelatin (PC) and other metal-binding proteins have an ability to bind heavy metals and have been used for heavy-metal removal. Thus, we reasoned that they might be employed for the synthesis of metal nanoparticles (NPs). Herein, we report the in vivo biosynthesis of diverse NPs by recombinant Escherichia coli expressing phytochelatin synthase (PCS) and/or metallothionein (MT). NPs of various metal elements, including semiconducting, alkali-earth, magnetic, and noble metals and rare-earth fluorides, could be synthesized in E. coli. The size of NPs could be tuned on the nanoscale by changing the concentration of metal ions in the medium. Thus, the controlled synthesis of NPs with desirable characteristics for in vitro assays and cellular imaging was possible. Paramagnetic NPs could also be synthesized by using the same system. The strategy of employing recombinant E. coli as an NP factory is generally applicable for the combinatorial synthesis of diverse NPs with a wide range of characteristics.Metal NPs exhibit unique optical, electronic, and magnetic properties, which depend on their composition, size, and structure, and have therefore been explored extensively for various applications in bio-and nanotechnology.
Metal nanoparticles are garnering considerable attention owing to their high potential for use in various applications in the material, electronics, and energy industries. Recent research efforts have focused on the biosynthesis of metal nanomaterials using microorganisms rather than traditional chemical synthesis methods. Microorganisms have evolved to possess molecular machineries for detoxifying heavy metals, mainly by employing metal-binding proteins and peptides. Biosynthesis of diverse metal nanoparticles has recently been demonstrated using such heavy metal detoxification systems in microorganisms, which provides several advantages over the traditional chemical synthesis methods. First, metal nanoparticles can be synthesized at mild temperatures, such as at room temperature, with less energy input. Second, no toxic chemicals or reagents are needed, and thus the process is environmentally friendly. Third, diverse metal nanoparticles, including those that have never been chemically synthesized, can be biosynthesized. Here, we review the strategies for the biosynthesis of metal nanoparticles using microorganisms, and provide future prospects.
A silicon nanowire field effect transistor (FET) straddled by the double-gate was demonstrated for biosensor application. The separated double-gates, G1 (primary) and G2 (secondary), allow independent voltage control to modulate channel potential. Therefore, the detection sensitivity was enhanced by the use of G2. By applying weakly positive bias to G2, the sensing window was significantly broadened compared to the case of employing G1 only, which is nominally used in conventional nanowire FET-based biosensors. The charge effect arising from biomolecules was also analyzed. Double-gate nanowire FET can pave the way for an electrically working biosensor without a labeling process.
Surface wrinkles are commonly observed in large-scale of graphene films. As a new feature, the wrinkled surface of graphene films may directly affect bacterial viability by means of various interactions of bacterial cells with graphene sheets. In the present study, we introduce a wrinkled surface geometry of graphene oxide (GO) thin films for antibacterial application. Highly wrinkled GO films were formed by vacuum filtration of a GO suspension through a prestrained filter. Several types of wrinkled GO surfaces were obtained with different roughness grades determined by root-mean-square values. Antibacterial activity of the fabricated GO films toward three different bacterial species, Escherichia coli, Mycobacterium smegmatis, and Staphylococcus aureus, was evaluated in relation to surface roughness. Because of their nanoscopically corrugated nature, the wrinkled GO films exhibited excellent antibacterial properties. On the basis of our detailed observations, we propose a novel concept of the surrounded contact-based mechanism for antimicrobial activity of wrinkled GO films. It postulates formation of a mechanically robust GO surface "trap" that prompts interaction of bacteria with the diameter-matched GO sink, which results in substantial damages to the bacterial cell membrane. We believe that our approach uncovered a novel use of a promising two-dimensional material for highly effective antibacterial treatment.
An efficient strategy for immobilizing proteins on a gold surface was developed by employing the gold binding polypeptide (GBP) as a fusion partner. Using the enhanced green fluorescent protein (EGFP), severe acute respiratory syndrome coronavirus (SARS-CoV) envelope protein (SCVme), and core streptavidin (cSA) of Streptomyces avidinii as model proteins, specific immobilization of the GBP-fusion proteins onto the gold nanoparticles and generation of protein nanopatterns on the bare gold surface were demonstrated. The GBP-fused SCVme bound to gold nanoparticles successfully interacted with its antibody and showed changes in absorbance and color, allowing efficient diagnosis of SARS-CoV. The fusion proteins could be successfully immobilized on the gold surface by nanopatterning and microcontact printing as examined by atomic force microscopy and surface plasmon resonance analysis. The poly(dimethylsiloxane) microfluidic channels were created on the gold surface and were used for antigen-antibody and DNA-DNA interaction studies. Specific immobilization of GBP-EGFP fusion protein and its interaction with the antibody in the microchannels could be demonstrated. By immobilizing the DNA probe through the use of GBP-fused cSA, specific hybridization of the target DNA prepared from Salmonella could also be achieved. The GBP-fusion method allows immobilization of proteins onto the gold surface without surface modification and in bioactive forms suitable for studying protein-protein, DNA-DNA, and other biomolecular interaction studies. Furthermore, these studies can be carried out in a microfluidic system, which allows high-throughput analysis of biomolecular interactions.
Nanomaterials (NMs) are mostly synthesized by chemical and physical methods, but biological synthesis is also receiving great attention. However, the mechanisms for biological producibility of NMs, crystalline versus amorphous, are not yet understood. Here we report biosynthesis of 60 different NMs by employing a recombinant strain coexpressing metallothionein, a metal-binding protein, and phytochelatin synthase that synthesizes a metal-binding peptide phytochelatin. Both an in vivo method employing live cells and an in vitro method employing the cell extract are used to synthesize NMs. The periodic table is scanned to select 35 suitable elements, followed by biosynthesis of their NMs. Nine crystalline single-elements of MnO, FeO, CuO, Mo, Ag, In(OH), SnO, Te, and Au are synthesized, while the other 16 elements result in biosynthesis of amorphous NMs or no NM synthesis. Producibility and crystallinity of the NMs are analyzed using a Pourbaix diagram that predicts the stable chemical species of each element for NM biosynthesis by varying reduction potential and pH. Based on the analyses, the initial pH of reactions is changed from 6.5 to 7.5, resulting in biosynthesis of various crystalline NMs of those previously amorphous or not-synthesized ones. This strategy is extended to biosynthesize multi-element NMs including CoFeO, NiFeO, ZnMnO, ZnFeO, AgS, AgTeO, AgWO, HgTeO, PbMoO PbWO, and Pb(VO)OH NMs. The strategy described here allows biosynthesis of NMs with various properties, providing a platform for manufacturing various NMs in an environmentally friendly manner.
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