Strategic engineering of alkyl spacer length for a pH-tolerant lysosome marker and dual organelle localization

Long-term visualization of lysosomal properties is extremely crucial to evaluate diseases related to their dysfunction. However, many of the reported lysotrackers are less conducive to imaging lysosomes precisely because they suffer from fluorescence quenching and other inherent drawbacks such as pH-sensitivity, polarity insensitivity, water insolubility, slow diffusibility, and poor photostability. To overcome these limitations, we have utilized an alkyl chain length engineering strategy and synthesized a series of lysosome targeting fluorescent derivatives namely NIMCs by attaching a morpholine moiety at the peri position of the 1,8-naphthalimide (NI) ring through varying alkyl spacers between morpholine and 1,8-naphthalimide. The structural and optical properties of the synthesized NIMCs were explored by ¹H-NMR, single-crystal X-ray diffraction, UV-Vis, and fluorescence spectroscopy. Afterward, optical spectroscopic measurements were carefully performed to identify a pH-tolerant, polarity sensitive, and highly photostable fluoroprobes for further live-cell imaging applications. NIMC6 displayed excellent pH-tolerant and polarity-sensitive properties. Consequently, all NIMCs were employed in kidney fibroblast cells (BHK-21) to investigate their applicability for lysosome targeting and probing lysosomal micropolarity. Interestingly, a switching of localization from lysosomes to the endoplasmic reticulum (ER) was also achieved by controlling the linker length and this phenomenon was subsequently applied in determining ER micropolarity. Additionally, the selected probe NIMC6 was also employed in BHK-21 cells for 3-D spheroid imaging and in Caenorhabditis elegans (C. elegans) for in vivo imaging, to evaluate its efficacy for imaging animal models.

A series naphthalimide-based fluorophores were designed by alkyl spacer length engineering to discover a pH-tolerant lysosomal marker. This approach also allows to probe lysosome-related organelles in C. elegans and communication between organelles.     

Coupling Effects of Electrostatic Interactions and Salt Concentration Gradient in Polymer Translocation through a Nanopore: A Coarse-Grained Molecular Dynamics Simulations Study

We study the influence of polymer pore interactions and focus on the role played by the concentration gradient of salt in the translocation of polyelectrolytes (PE) through nanopores explicitly using coarse-grained Langevin dynamics simulations. The mean translocation time is calculated by varying the applied voltage, the pH, and the salt concentration gradient. Changing the pH can alter the electrostatic interaction between the protein pore and the polyelectrolyte chain. The polymer pore interaction is weakened by the increase in the strength of the externally applied electric field that drives translocation. Additionally, the screening effect of the salt can reduce the strong charge-charge repulsion between the PE beads which can make translocation faster. The simulation results show there can be antagonistic or synergistic coupling between the salt concentration-induced screening effect and the drift force originating from the salt concentration gradient thereby affecting the translocation time. Our simulation results are explained qualitatively with free energy calculations.     

Predicting particle deposition for flow over a circular cylinder in combustion environments

Particle deposition on heat exchanger tubes is a serious concern in solid fuel combustion and gasification systems, such as power plants and syngas coolers. To predict deposition rates, several detailed computational fluid dynamic (CFD) models have been developed. However, these models are computationally expensive and cannot be used for quick determination of deposition rates and/or slagging tendencies. Particle impaction efficiency correlations, while not as accurate as detailed CFD models, are easier to use and are able to estimate the impaction rate of particles on the heat exchanger tubes. Nonetheless, since deposition and slagging are not just functions of particle impaction rates, but also sticking propensity, which is related to the particle temperature at impact, the impaction efficiency correlations fail to provide sufficient information. To address this shortcoming, similar correlations for particle temperature at impact have been developed in this work, based on a non-dimensional parameter that captures the flow and boundary conditions, as well as particle properties. When used alongside the impaction efficiency correlations, the new correlations developed can provide a reasonable estimate of the deposition and slagging tendencies, at negligible computational expense.     

Strong Law of Large Numbers for Betti Numbers in the Thermodynamic Regime

Journal of Statistical Physics - We establish the strong law of large numbers for Betti numbers of random ?ech complexes built on $${\mathbb {R}}^N$$ -valued binomial point processes and...     

Toward quantifying the electrostatic transduction mechanism in carbon nanotube molecular sensors

Despite the great promise of carbon nanotube field-effect transistors (CNT FETs) for applications in chemical and biochemical detection, a quantitative understanding of sensor responses is lacking. To explore the role of electrostatics in sensor transduction, experiments were conducted with a set of highly similar compounds designed to adsorb onto the CNT FET via a pyrene linker group and take on a set of known charge states under ambient conditions. Acidic and basic species were observed to induce threshold voltage shifts of opposite sign, consistent with gating of the CNT FET by local charges due to protonation or deprotonation of the pyrene compounds by interfacial water. The magnitude of the gate voltage shift was controlled by the distance between the charged group and the CNT. Additionally, functionalization with an uncharged pyrene compound showed a threshold shift ascribed to its molecular dipole moment. This work illustrates a method for producing CNT FETs with controlled values of the turnoff gate voltage, and more generally, these results will inform the development of quantitative models for the response of CNT FET chemical and biochemical sensors.     

Advances in Electrochemical and Catalytic Performance of Nanostructured FeCo2O4 and Its Composites

It is well established that the excessive and uncontrolled use of fossil fuels and organic chemicals have put a risk to the earth‘s environment and the life that sustains within it. Carbon-free, sustainable, alternative energy technologies have therefore become the prime focus of current research. Smart inorganic materials have emerged as the potential solution to suffice energy needs and remediate the organic pollutants discharged to the environment. One such promising, versatile material is FeCo₂O₄ which has gained immense research interest in the present decade due to its high efficiency and performance in energy and environmental applications. Innovative material design strategies involving the interplay of nanostructured morphology, chemical composition, redox surface states, and defect engineering have significantly enhanced both electrochemical and catalytic properties of FeCo₂O₄. Therefore, this review article aims to provide the first-ever comprehensive account of the latest research and developments in design-synthesis strategies, characterization techniques, and applications of nanostructured FeCo₂O₄ and its composites in various electrochemical as well as catalytic applications. A detailed account of the nanostructured FeCo₂O₄ and its composites in various energy storage and conversion devices such as supercapacitors (SCs), batteries, and fuel cells has been presented. Furthermore, a special section has been devoted to highlight the role of FeCo₂O₄ in enhancing the sluggish reaction kinetics of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in water splitting application. This review also highlights the role of nanostructured FeCo₂O₄ in photocatalytic waste water treatment, gas sensing, and dual-phase membrane technologies wherein FeCo₂O₄ has demonstrated promising performance.     

Cobalt-Catalyzed C8-Dienylation of Quinoline-N-Oxides

An efficient Cp*Co^III-catalyzed C8-dienylation of quinoline-N-oxides was achieved by employing allenes bearing leaving groups at the α-position as the dienylating agents. The reaction proceeds by Co^III-catalyzed C−H activation of quinoline-N-oxides and regioselective migratory insertion of the allene followed by a β-oxy elimination, leading to overall dienylation. Site-selective C−H activation was achieved with excellent selectivity under mild reaction conditions, and 30 mol % of a NaF additive was found to be crucial for the efficient dienylation. The methodology features high stereoselectivity, mild reaction conditions, and good functional-group tolerance. C8-alkenylation of quinoline-N-oxides was achieved in the case of allenes devoid of leaving groups as coupling partners. Furthermore, gram-scale preparation and preliminary mechanistic experiments were carried out to gain insights into the reaction mechanism.     

A Note on Asymptotic Expansions to Approximate Eigenvalues of Integral Operators with Green's Kernels using the Iterated Galerkin Method

In this article, we consider approximation of eigenvalues of integral operators with Green's function-type kernels using the iterated Galerkin method. We obtain asymptotic expansions for approximate eigenvalues. The Richardson extrapolation is used to obtain eigenvalue approximations of higher order. A numerical example is considered in order to illustrate our theoretical results.