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Antimicrobial Properties of 2D MnO 2 and MoS 2 Nanomaterials Vertically Aligned on Graphene Materials and Ti 3 C 2 MXene
Two-dimensional (2D) nanomaterials have attracted considerable attention in biomedical and environmental applications due to their antimicrobial activity. In the interest of investigating the primary antimicrobial mode-of-action of 2D nanomaterials, we studied the antimicrobial properties of MnO 2 and MoS 2 , toward Gram-positive and Gram-negative bacteria. Bacillus subtilis and Escherichia coli bacteria were treated individually with 100 μg/mL of randomly oriented and vertically aligned nanomaterials for ~3 h in the dark. The vertically aligned 2D MnO 2 and MoS 2 were grown on 2D sheets of graphene oxide, reduced graphene oxide, and Ti 3 C 2 MXene. Measurements to determine the viability of bacteria in the presence of the 2D nanomaterials performed by using two complementary techniques, flow cytometry, and fluorescence imaging showed that, while MnO 2 and MoS 2 nanosheets show different antibacterial activities, in both cases, Gram-positive bacteria show a higher loss in membrane integrity. Scanning electron microscopy images suggest that the 2D nanomaterials, which have a detrimental effect on bacteria viability, compromise the cell wall, leading to significant morphological changes. Here, we propose that the peptidoglycan mesh (PM) in the bacterial wall is likely the primary target of the 2D nanomaterials. Vertically aligned 2D MnO 2 nanosheets showed the highest antimicrobial activity, suggesting that the edges of the nanosheets were likely compromising the cell walls upon contact.
Cooperative Role of Mixed Solvent in the Evaporation-Induced Self-Assembly of Polypeptoid Nanocrystals
Peptoids, or polypeptoids, are biomimetic polymers that can self-assemble into nanocrystals for biomedical and biotechnological applications. Polypeptoid nanocrystals can be prepared by evaporation-induced self-assembly, but the roles of solvent components for this process have long been overlooked at the molecular level, leaving a tunable parameter for improving self-assembly protocols. This work utilized molecular dynamics simulations to study the effects of water and the commonly used tetrahydrofuran (THF) on the assembly of nanosheets from molecules of acetylated diblock polypeptoid, poly-(N-decylglycine)-b-poly-(N-2-(2-(2-methoxyethoxy)-ethoxy) ethylglycine), abbreviated as Ac-Ndc10-Nte10. To probe the stages of self-assembly, isolated molecules and preassembled nanofibers/nanosheets were simulated in pure THF, water, and their mixtures, respectively. The assembly energies show that the THF/water mixture has a greater tendency to form nanosheets than pure water. In a THF/water mixture, polypeptoids were found more uncoiled in isolated states, less compact in disordered agglomerates, and with reduced requirement for the Nte block to cover hydrophobic Ndc surfaces in the nanocrystals. Mixed solvent is vital to initiating self-assembly, as THF assists in the opening of coiled polypeptoid molecules, while water provides the thermodynamics to aggregate and ultimately form nanocrystals. To obtain wider nanosheets, it is recommended that some THF be maintained in the aqueous solvent before it becomes exhausted by evaporation. Near the nanosheet surface, the THF concentration is higher than that in bulk solution (3-4 times in 4 M THF/water). The strong adsorption of THF indicates the self-assembly in a de facto mixed solvent. These results are expected to guide the refinement of evaporation-induced self-assembly protocols for polypeptoid nanocrystals.
Source of Bright Near-Infrared Luminescence in Gold Nanoclusters
Gold nanoclusters with near-infrared (NIR) photoluminescence (PL) have great potential as sensing and imaging materials in biomedical and bioimaging applications. In this work, Au 21 (S-Adm) 15 and Au 38 S 2 (S-Adm) 20 are used to unravel the underlying mechanisms for the improved quantum yields (QY), large Stokes shifts and long PL lifetimes in gold nanoclusters. Both nanoclusters show decent PL QY. In particular, the Au 38 S 2 (S-Adm) 20 nanocluster shows a bright NIR PL at 900 nm with QY up to 15% in normal solvents (such as toluene) at ambient conditions. The relatively lower QY for Au 21 (S-Adm) 15 (4%) compared to Au 38 S 2 (S-Adm) 20 is attributed to the lowest-lying excited state being symmetry-disallowed, as evidenced by the pressure-dependent anti-spectral shift of the absorption spectra compared to PL. Yet, Au 21 (S-Adm) 15 maintains some emissive properties due to a nearby symmetry-allowed excited state. Furthermore, our results show that suppression of non-radiative decay due to the surface “lock rings” which encircle the Au kernel and the surface “lock atoms” which bridge the fundamental Au-kernel units (e.g., tetrahedra, icosahedra, etc.) is the key to obtain high QYs in gold nanoclusters. Here, the complicated excited-state processes and the small absorption coefficient of the band-edge transition lead to the large Stokes shifts and the long PL lifetimes that are widely observed in gold nanoclusters.
Reversible Emulsions from Polyoxometalate–Polymer: A Robust Strategy to Cyclic Emulsion Catalysis and High-Internal-Phase Emulsion Materials
Reversible Pickering emulsions, achieved by switchable, interfacially active colloidal particles, that enable on-demand emulsification/demulsification or phase inversion, hold substantial promise for biphasic catalysis, emulsion polymerization, cutting fluids, and crude oil pipeline transportation. However, particles with such a responsive behavior usually require complex chemical syntheses and surface modifications, limiting their extensive use. Herein, we report a simple route to generate emulsions that can be controlled and reversibly undergo phase inversion. The emulsions are prepared and stabilized by the interfacial assembly of polyoxometalate (POM)–polymer, where their electrostatic interaction at the interface is dynamic. The wettability of the POMs that dictates the emulsion type can be readily regulated by tuning the number of polymer chains bound to POMs, which, in turn, can be controlled by varying the concentrations of both components and the water/oil ratio. In addition, the number of polymer chains anchored to the POMs can be varied by controlling the number of negative charges on the POMs through an in situ redox reaction. As such, a reversible inversion of the emulsions can be triggered by switching between exposure to ultraviolet light and the introduction of oxygen. Combining the functions of POM itself, a cyclic interfacial catalysis system was realized. Inversion of the emulsion also affords a pathway to high-internal-phase emulsions. Finally, the diversity of the POMs, the polymers, and the responsive switching groups open numerous new, simple strategies for designing a wide range of responsive soft matter for cargo loading, controlled release, and delivery in biomedical and engineering applications without time-consuming particle syntheses.
A catalog of the diversity and ubiquity of bacterial microcompartments
Abstract Bacterial microcompartments (BMCs) are organelles that segregate segments of metabolic pathways which are incompatible with surrounding metabolism. BMCs consist of a selectively permeable shell, composed of three types of structurally conserved proteins, together with sequestered enzymes that vary among functionally distinct BMCs. Genes encoding shell proteins are typically clustered with those for the encapsulated enzymes. Here, we report that the number of identifiable BMC loci has increased twenty-fold since the last comprehensive census of 2014, and the number of distinct BMC types has doubled. The new BMC types expand the range of compartmentalized catalysis and suggest that there is more BMC biochemistry yet to be discovered. Our comprehensive catalog of BMCs provides a framework for their identification, correlation with bacterial niche adaptation, experimental characterization, and development of BMC-based nanoarchitectures for biomedical and bioengineering applications.
Imaging solvated oxygen atoms with a femtosecond laser
As a powerful oxidant, atomic oxygen (O) holds considerable promise for a variety of biomedical and industrial applications. However, the inability to quantify solvated oxygen atoms has prevented the determination of the fundamental parameters governing its behaviour in relevant aqueous environments. Here, we directly image ground-state oxygen atoms in water using femtosecond two-photon absorption laser-induced fluorescence. Measurements show that oxygen atoms persist for tens of microseconds in water, penetrating hundreds of micrometres into the liquid. This observed longevity has significant implications, suggesting a need to re-evaluate existing models of solvated atomic oxygen reactivity and transport. Beyond atomic oxygen, this technique is broadly applicable to other solvated atomic species of interest, including nitrogen (N) and hydrogen (H). This work establishes that radical atomic species can be quantified in liquid with ultrafast laser spectroscopy, providing the basis for the determination of key properties including reaction rates, chemical lifetimes, and Henry’s law constants.
A percolation theory for designing corrosion-resistant alloys
Iron-chromium and nickel-chromium binary alloys containing sufficient quantities of chromium serve as the prototypical corrosion-resistant metals owing to the presence of a nanometre-thick protective passive oxide film. Should this film be compromised by a scratch or abrasive wear, it reforms with little accompanying metal dissolution, a key criterion for good passive behaviour. This is a principal reason that stainless steels and other chromium-containing alloys are used in critical applications ranging from biomedical implants to nuclear reactor components. Unravelling the compositional dependence of this electrochemical behaviour is a long-standing unanswered question in corrosion science. Herein, we develop a percolation theory of alloy passivation based on two-dimensional to three-dimensional crossover effects that accounts for selective dissolution and the quantity of metal dissolved during the initial stage of passive film formation. We validate this theory both experimentally and by kinetic Monte Carlo simulation. Our results reveal a path forward for the design of corrosion-resistant metallic alloys.
Rapid prototyping of microchannels with surface patterns for fabrication of polymer fibers
Microfluidic technology has provided innovative solutions to numerous problems, but the cost of designing and fabricating microfluidic channels is impeding its expansion. In this study, Shrinky-Dink thermoplastic sheets are used to create multilayered complex templates for microfluidic channels. We also used inkjet and laserjet printers to raise a predetermined microchannel geometry by depositing several layers of ink for each feature consecutively. We achieved feature heights over 100 μm, which were measured and compared with surface profilometry. Templates closest to the target geometry were then used to create microfluidic devices from soft-lithography with the molds as a template. These microfluidic devices were, futhermore used to fabricate polymer microfibers using the microfluidic focusing approach to demonstrate the potential that this process has for microfluidic applications. Finally, an economic analysis was conducted to compare the price of common microfluidic template manufacturing methods. We showed that multilayer microchannels can be created significantly quicker and cheaper than current methods for design prototyping and point-of-care applications in the biomedical area.
Characterization of surface–solute interactions by diffusioosmosis
The accurate measurement of wall zeta potentials and solute–surface interaction length scales for electrolyte and non-electrolyte solutes, respectively, is critical to the design of many biomedical and microfluidic applications. We present a novel microfluidic approach using diffusioosmosis for measuring either the zeta potentials or the characteristic interaction length scales for surfaces exposed to, respectively, electrolyte or non-electrolyte solutes. When flows containing different solute concentrations merge in a junction, local solute concentration gradients can drive diffusioosmotic flow due to electrokinetic, steric, and other interactions between the solute molecules and solid surfaces. We demonstrate a microfluidic system consisting of a long, narrow pore connecting two large side channels in which solute concentration gradients drive diffusioosmosis within the pore, resulting in predictable fluid velocity/pressure and solute profiles. Furthermore, we present analytical results and a methodology to determine the zeta potential or interaction length scale for the pore surfaces based on the solute concentrations in the main side channels, the flow rate in the pore, and the pressure drop across the pore. We apply this method to the experimental data of Lee et al. to predict the zeta potentials of their system, and we use 3D numerical simulations to validate the theory and show that end effects caused by the junctions are negligible for a wide range of parameters. Because the dynamics in the proposed system are driven by diffusioosmosis, this technique does not suffer from certain disadvantages associated with the use of sensitive electronics in traditional zeta potential measurement approaches such as streaming potential, streaming current, or electroosmosis. As a result, to the best of our knowledge this is the first flow-based approach to characterize surface/solute interactions with non-electrolyte solutes.
Bi-continuous pattern formation in thin films via solid-state interfacial dealloying studied by multimodal characterization
Solid-state interfacial dealloying creates bi-continuous nanostructured thin films with 3D interconnected morphology, revealed by multimodal characterization, offering potential applications in catalysis, biomedical sensing and energy storage.
Iron carbide nanoplatelets: colloidal synthesis and characterization
Iron carbide nanoplatelets with an orthorhombic Fe 3 C structure were synthesized following a simple liquid chemical approach. The formation of the carbide phases was shown to depend on the presence of a long chain diol and the reaction temperature. Confirmation of the iron carbide phases and structural characterization was made by X-ray diffraction (XRD) and Mössbauer spectroscopy. Particle morphology was characterized by transmission electron microscopy (TEM) and HR-TEM and the magnetic properties were measured with magnetometry (VSM). The sample with the Fe 3 C phase shows a ferromagnetic behavior with a magnetization of 139 emu g -1 under a 30 kOe applied field. The simple methodology presented here for producing iron carbide nanoplatelets has promising application in the biomedical and catalyst industries.
Graphene-extracted membrane lipids facilitate the activation of integrin α v β 8
Despite the remarkable electrochemical properties of graphene, strong van der Waals attraction between graphene and biomolecules often causes cytotoxicity, which hinders its applications in the biomedical field. Unfortunately, surface passivation of graphene might stimulate undesired immune response as the nanomaterial triggers cytokine production through membrane receptor activation. In this work, we use all-atom Molecular Dynamics (MD) simulations to unravel the underlying mechanism of graphene-induced inside-out activation of integrin αvβ8, a prominent membrane receptor expressed in immune cells. We model the transmembrane (TM) domains of integrin αvβ8 in a 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC) lipid bilayer and observe the structural changes in the integrin–membrane complex when interacting with a graphene nanosheet across the membrane. We find that the β8 TM domain interacts with the graphene nanosheet directly or indirectly through extracted lipids, facilitating the pulling of a β8 subunit away from an αv subunit and thus leading to the disruption of the TM domain association by breaking the hydrophobic cluster in the cytoplasmic domains of the αv and β8 subunits. Alanine substitution of two conserved phenylalanine residues on the αv subunit at this hydrophobic cluster further reveals the importance of a stable T-shaped structure in retaining integrin in its inactive state. Our results agree with previous studies on the interactions between other integrin subtypes and their endogenous activators, suggesting an intriguing role that the graphene nanosheet may play in the integrin-related signal transduction during its interaction with the membrane.
New approach for absolute fluence distribution calculations in Monte Carlo simulations of light propagation in turbid media
A novel way to attain three dimensional fluence rate maps from Monte-Carlo simulations of photon propagation is presented in this work. The propagation of light in a turbid medium is described by the radiative transfer equation and formulated in terms of radiance. For many applications, particularly in biomedical optics, the fluence rate is a more useful quantity and directly derived from the radiance by integrating over all directions. Contrary to the usual way which calculates the fluence rate from absorbed photon power, the fluence rate in this work is directly calculated from the photon packet trajectory. The voxel based algorithm works in arbitrary geometries and material distributions. It is shown that the new algorithm is more efficient and also works in materials with a low or even zero absorption coefficient. The capabilities of the new algorithm are demonstrated on a curved layered structure, where a non-scattering, non-absorbing layer is sandwiched between two highly scattering layers.
An atomic charge model for graphene oxide for exploring its bioadhesive properties in explicit water
Graphene Oxide (GO) has been shown to exhibit properties that are useful in applications such as biomedical imaging, biological sensors, and drug delivery. The binding properties of biomolecules at the surface of GO can provide insight into the potential biocompatibility of GO. Here we assess the intrinsic affinity of amino acids to GO by simulating their adsorption onto a GO surface. The simulation is done using Amber03 force-field molecular dynamics in explicit water. The emphasis is placed on developing an atomic charge model for GO. The adsorption energies are computed using atomic charges obtained from an ab initio electrostatic potential based method. The charges reported here are suitable for simulating peptide adsorption to GO.
Deep-red semiconductor monolithic mode-locked lasers
A deep-red semiconductor monolithic mode-locked laser is demonstrated. Multi-section laser diodes based on an AlGaAs multi-quantum-well structure were passively mode-locked, enabling the generation of picosecond optical pulses at 752 nm, at pulse repetition rates of 19.37 GHz. An investigation of the dependence of the pulse duration as a function of reverse bias revealed a predominantly exponential decay trend of the pulse duration, varying from 10.5 ps down to 3.5 ps, which can be associated with the concomitant reduction of absorption recovery time with increasing applied field. A 30-MHz-tunability of the pulse repetition rate with bias conditions is also reported. The demonstration of such a compact, efficient and versatile ultrafast laser in this spectral region paves the way for its deployment in a wide range of applications such as biomedical microscopy, pulsed terahertz generation as well as microwave and millimeter-wave generation, with further impact on sensing, imaging and optical communications.
Superparamagnetic properties of carbon nanotubes filled with NiFe{sub 2}O{sub 4} nanoparticles
Multi walled carbon nanotubes (MWCNTs) were successfully synthesized using custom-made 80 nm pore-size alumina templates, and were uniformly filled with nickel ferrite (NFO) nanoparticles of 7.4 ± 1.7 nm diameter using a novel magnetically assisted capillary action method. X-ray diffraction confirmed the inverse spinel phase for the synthesized NFO. Transmission electron microscopy confirms spherical NFO nanoparticles with an average diameter of 7.4 nm inside MWCNTs. Magnetometry indicates that both NFO and NFO-filled MWCNTs present a blocking temperature around 52 K, with similar superparamagnetic-like behavior, and weak dipolar interactions, giving rise to a super-spin-glass-like behavior at low temperatures. These properties along with the uniformity of sub-100 nm structures and the possibility of tunable magnetic response in variable diameter carbon nanotubes make them ideal for advanced biomedical and microwave applications.