In stochastic blocking electrochemistry, microparticles generate individual current steps when they adsorb on a microelectrode and decrease the current and flux of a redox mediator reacting at the surface. The amplitude of the current step informs on particle size and landing locus, while step frequency correlates with particle transport. Here, we report a new method to estimate the average arrival velocities of single rod-shaped bacteria (bacilli). The method relies on simulating the nearby threshold distance from the surface where the bacillus no longer perturbs mediator flux and the current step approaches zero. We estimated the average velocities of bacillus arrival by dividing the threshold distance over the current step duration, a parameter that here we detect for the first time and increases with bacillus length. By comparing diffusional fluctuations to bacillus average velocity, we estimated diffusion and migration contributions as a function of bacterium size. Average arrival velocities increase with bacillus length at the same time as migration intensifies and diffusion weakens. Our analysis is universal and more effective in determining transport mode contributions than the present approach of comparing theoretical and experimental step frequencies. Uncertainty in landing locus is inconsequential because the step duration used to calculate the average arrival speed already contains such information and knowing bacillus electrophoretic mobility or ζ-potential is not needed. Additionally, by simulating and assigning edge landings to the most repeated values of current steps in a recording, we obtain bacilli lengths and widths similar to scanning electron microscopy, from which we infer landing orientation.
A novel series of 2-arylidenehydrazinyl-4-arylthiazole analogues (3a-p) was designed and synthesized in excellent yields using a rapid, simple, efficient methodology. Sixteen novel compounds were screened for in vitro antimicrobial activities against eleven bacteria, namely, Staphylococcus aureus, Listeria monocytogenes, Enterococcus faecalis, Bacillus subtilis, Klebsiella pneumonia, Citrobacter freundii, Cronobacter sakazakii, Salmonella enteritidis, Escherichia coli, Yersinia pestis, and Pseudomonas aeruginosa. All 16 compounds showed significant anti-bacterial activities against both Gram-positive and Gram-negative bacteria. In particular, compound 3g showed potent inhibition of E. coli and K. pneumonia, compound 3i inhibited E. faecalis, compound 3n S. tythi and E. faecalis, and compound 3c E. coli and C. sakazakii. In fact, our results indicate that most of the compounds synthesized exhibit strong antibacterial activity. The qualitative structureantibacterial activity relationships (QSAR) were studied using the physicochemical and quantum-chemical parameters of the ab initio Hartree-Fock model at the RHF/6-31G level of theory. A good qualitative correlation between predicted physicochemical parameters (log P and polar surface area (PSA)) and antibacterial activity has been found. The synthesized compounds were also evaluated for antioxidant activity. Compounds 3j, 3a and 3i exhibited the greatest antioxidant activity, with IC 50 values of 0.66, 0.81, and 1.08 µM, respectively, which were comparable to that of ascorbic acid (IC 50 0.87 µM). The promising antibacterial and antioxidant activities of some of these synthesized 2-arylidenehydrazinyl-4-arylthiazole derivatives, together with the results of quantum-chemical studies, could be helpful for the development of drugs to combat diseases caused by microorganisms and oxidative stress.
Current–time recordings of emulsified toluene microdroplets containing 20 mM Ferrocene (Fc), show electrochemical oxidation peaks from individual adsorption events on disk microelectrodes (5 μm diameter). The average droplet diameter (∼0.7 μm) determined from peak area integration was close to Dynamic Light Scattering measurements (∼1 μm). Random walk simulations were performed deriving equations for droplet electrolysis using the diffusion and thermal velocity expressions from Einstein. The simulations show that multiple droplet-electrode collisions, lasting ∼0.11 μs each, occur before a droplet wanders away. Updating the Fc-concentration at every collision shows that a droplet only oxidizes ∼0.58% of its content in one collisional journey. In fact, it would take ∼5.45 × 106 collisions and ∼1.26 h to electrolyze the Fc in one droplet with the collision frequency derived from the thermal velocity (∼0.52 cm/s) of a 1 μm-droplet. To simulate adsorption, the droplet was immobilized at first contact with the electrode while the electrolysis current was computed. This approach along with modeling of instrumental filtering, produced the best match of experimental peaks, which were attributed to electrolysis from single adsorption events instead of multiple consecutive collisions. These results point to a heightened sensitivity and speed when relying on adsorption instead of collisions. The electrochemical current for the former is limited by the probability of adsorption per collision, whereas for the latter, the current depends on the collision frequency and the probability of electron transfer per collision (J. Am. Chem. Soc. 2017, 139, 16923–16931).
The use of redox-active organic materials in rechargeable batteries has the potential to improve the field of energy storage by enabling lightweight and flexible green batteries. In addition, replacing lithium with sodium further mitigates the resource limitations and high cost of lithium for Li-ion batteries (LIBs). Herein, graphene oxide (GO) nanosheets were cross-linked by covalently bonded azo compounds to facilitate sodium-ion insertion and increase charge storage capacity. In the processes, diamine functional groups of p-phenylenediamine (PPD) were converted into diazonium salts (DSs), followed by an electrophilic aromatic substitution between the DSs and GO nanosheets to synthesize azobenzene partially reduced graphene oxide compounds (AB-PRGO) for sodium-ion storage. The as-synthesized AB-PRGO is characterized by various techniques, including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), nitrogen adsorption/desorption isotherm, Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The AB-PRGO was used as a new cathode material in half-cell Na-ion batteries (SIBs). The results revealed that within a given potential window (0.01−3.0 V), the AB-PRGO-based SIB exhibits good cyclic stability, a high specific capacity, and good rate capability while obtaining a specific capacity of 160 mAh g −1 at 50 mA g −1 and preserved the capacity for 50 cycles. This work provides an effective route for developing improved organic electrode materials for SIBs.
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