Kerrcunningham9545
Biofuels are considered sustainable and renewable alternatives to conventional fossil fuels. Biobutanol has recently emerged as an attractive option compared to bioethanol and biodiesel, but a significant challenge in its production lies in the separation stage. The current industrial process for the production of biobutanol includes the ABE (acetone-butanol-ethanol) fermentation process from biomass; the resulting fermentation broth has a butanol concentration of no more than 2 wt% (the rest is essentially water). Therefore, the development of a cost-effective process for separation of butanol from dilute aqueous solutions is highly desirable. The use of porous materials for the adsorptive separation of ABE mixtures is considered a highly promising route, as these materials can potentially have high affinities for alcohols and low affinities for water. To date, zeolites have been tested toward this separation, but their hydrophilic nature makes them highly incompetent for this application. The use of metal-organic frameworks (MOFs) is an apparent solution; however, their low hydrolytic stabilities hinder their implementation in this application. So far, a few nanoporous zeolitic imidazolate frameworks (ZIFs) have shown excellent potential for butanol separation due to their good hydrolytic and thermal stabilities. Herein, we present a novel, porous, and hydrophobic MOF based on copper ions and carborane-carboxylate ligands, mCB-MOF-1, for butanol recovery. mCB-MOF-1 exhibits excellent stability when immersed in organic solvents, water at 90 °C for at least two months, and acidic and basic aqueous solutions. We found that, like ZIF-8, mCB-MOF-1 is non-porous to water (type II isotherm), but it has higher affinity for ethanol, butanol, and acetone compared to ZIF-8, as suggested by the shape of the vapor isotherms at the crucial low-pressure region. This is reflected in the separation of a realistic ABE mixture in which mCB-MOF-1 recovers butanol more efficiently compared to ZIF-8 at 333 K.We detail the preparation of highly fluorescent quantum dots (QDs), surface-engineered with multifunctional polymer ligands that are compact and readily compatible with strain-promoted click conjugation, and the use of these nanocrystals in immunofluorescence and in vivo imaging. The ligand design combines the benefits of mixed coordination (i.e., thiol and imidazole) with zwitterion motifs, yielding sterically-stabilized QDs that present a controllable number of azide groups, for easy conjugation to biomolecules via the selective click chemistry. The polymer coating was characterized using NMR spectroscopy to extract estimates of the diffusion coefficient, hydrodynamic size, and ligand density. The azide-functionalized QDs were conjugated to anti-tropomyosin receptor kinase B antibody (α-TrkB) or to the brain-derived neurotrophic factor (BDNF). These conjugates were highly effective for labeling the tropomyosin receptor kinase B (TrkB) in pyramidal neurons within cortical tissue and for monitoring the BDNF induced activation of TrkB signaling in live neuronal cells. Finally, the polymer-coated QDs were applied for in vivo imaging of Drosophila melanogaster embryos, where the QDs remained highly fluorescent and colloidally stable, with no measurable cytotoxicity. These materials would be of great use in various imaging applications, where a small size, ease of conjugation, and great colloidal stability for in vivo studies are needed.A large number of organic reactions feature post-transition-state bifurcations. Selectivities in such reactions are difficult to analyze because they cannot be determined by comparing the energies of competing transition states. Molecular dynamics approaches can provide answers but are computationally very expensive. We present an algorithm that predicts the major products in bifurcating organic reactions with negligible computational cost. The method requires two transition states, two product geometries, and no additional information. The algorithm correctly predicts the major product for about 90% of the organic reactions investigated. For the remaining 10% of the reactions, the algorithm returns a warning indication that the conclusion may be uncertain. The method also reproduces the experimental and the molecular dynamics product ratios within 15% for more than 80% of the reactions. We have successfully applied the method to a trifurcating organic reaction, a carbocation rearrangement, and solvent-dependent Pummerer-like reactions, demonstrating the power of the algorithm to simplify and to help understand highly complex reactions.With the development of the internet of things (IoT) and 5th generation communication technology, construction of smart cities is making a great progress. However, the IoT system needs millions of sensing nodes; therefore, it is rather challenging to power various sensors. Here, we design an electrostatic force-based switch (EFS) that can work as either an optical or an electrical switch. The EFS provides a method to directly detect or control high-voltage electrical systems with delay characteristics. Advantages of the EFS include self-contained delay characteristics, ease of fabrication, low cost, and high stability, especially when used in combination with the triboelectric nanogenerator (TENG) to realize self-powered sensors. Based on the self-powered sensor, a mechanical motion-sensing system is built with high sensitivity and active response to the mechanical trigger. This study proposes a multifunctional self-powered switch, which realizes a high-voltage delay control system and can also combine with the TENG to expand the application of self-powered smart sensing systems.Redox-active sites present at large concentrations as part of a solid support or dissolved as molecules in fluid solutions undergo reversible self-exchange electron-transfer reactions. These processes can be monitored using a variety of techniques. Chronoamperometry and cyclic voltammetry are common techniques used to interrogate this behavior for molecules bound to mesoporous thin films of wide-bandgap semiconductors and insulators. In order to use these techniques to obtain accurate values for apparent diffusion coefficients, which are proxies for rate constants for self-exchange electron transfer, it is imperative to take into consideration nonidealities in redox titrations, parasitic currents, and ohmic resistances. Using spectroelectrochemical measurements taken concurrently with measurements of chronoamperometry data, we show that the spectroscopic data is not confounded from effects of parasitic currents or electroinactive dyes. However, we show that the thickness of the thin film over the region that is optically probed by the measurements must be known. When each of these considerations is included in data analyses, calculated apparent diffusion coefficients are, within error, independent of the method used to obtain the data. These considerations help reconcile variations in apparent diffusion coefficients measured using different techniques that have been reported over the past several decades and allow correct analyses to be performed in the future, independent of the method used to obtain the data.Random lasing is a lasing phenomenon realized in random media, and it has attracted a great deal of attention in recent years. An essential requirement for strong random lasing is to achieve strong and recurrent scattering among grain boundaries of a disordered structure. Herein, we report a random laser (RL) based on individual polycrystalline GaTe microflakes (MFs) with a lasing threshold of 4.15 kW cm-2, about 1-2 orders of magnitude lower than that of the reported single GaN microwire random laser. The strongly enhanced light scattering and trapping benefit from the reduced grain size in the polycrystalline GaTe MF, resulting in a ultralow threshold. We also investigate the dependence of spatially localized cavities' dimension on the pumping intensity profile and temperature. The findings provide a feasible route to realize RL with a low threshold and small size, opening up a new avenue in fulfilling many potential optoelectronic applications of RL.Numerous trap states and low conductivity of compact TiO2 layers are major obstacles for achieving high power conversion efficiency and high-stability perovskite solar cells. GSK126 order Here we report an effective Na2S-doped TiO2 layer, which can improve the conductivity of TiO2 layers, the contact of the TiO2/perovskite interface, and the crystallinity of perovskite layers. Comprehensive investigations demonstrate that Na cations increase the conductivity of TiO2 layers while S anions change the wettability of TiO2 layers, thus improving the crystallinity of perovskite layers and passivate defects at the TiO2/PVK interface. The synergetic effects of dopants lead to a champion efficiency as high as 21.25% in unencapsulated perovskite solar cells (PSCs), with much-improved stability. Our work provides new insights on anion dopants in TiO2 layers, which is usually neglected in previous reports, and also proposes a simple approach to produce low-cost and high-performance electron transport layers for high-performance PSCs.3D/4D printing is enabling transformative advances in device manufacturing and medicine but remains limited by the lack of printable resorbable materials with advanced properties and functions. Herein, we report the rapid and precise 4D printing of shape-memory scaffolds based on poly(propylene fumarate) (PPF) star polymers. Scaffolds with tunable and distinguishable properties can be produced with identical polymer formulation and stoichiometry. The resulting scaffold glass transition temperatures and Young's moduli increase with the postcuring time. Significantly, both the extent and rate of shape recovery following compression can be tuned by varying the strut design, the postcuring step duration, and/or the temperature applied for the recovery step. Finally, accelerated degradation studies confirmed the resorbability of the PPF star polymer gyroid scaffolds.Bacterial contamination accounts for more than half of food poisoning cases. Conventional methods such as colony-counting and general polymerase chain reaction are time-consuming, instrument-dependent, and sometimes not accurate. Herein, we developed a novel one-pot toolbox with precision and ultra sensitivity (OCTOPUS) platform for foodborne pathogen detection based on the mechanism in which Cas12a nontarget binding unleashes its collateral DNase activity. We demonstrated its application on two widespread foodborne bacteria, namely, E. coli O157H7 and Streptococcus aureus, using specific crRNA targeting rfbE and nuc gene, respectively. For better sensitivity, recombinase polymerase amplification (RPA) was integrated without product purification. This one-pot detection, that is, RPA reagent, crRNA, and ssDNA-FQ reporter are all in one tube with the subsequent addition of Cas12a enzyme, was able to detect genomic DNA at the attomolar level. It omits an extra cap-opening process to avoid practical inconvenience and possible cross-sample contamination. Moreover, we demonstrated this platform for a real food matrix. A simple water boiling method for genome extraction together with one-pot assay achieved a limit of detection value of 1 CFU/mL in less than 50 min. This OCTOPUS technique integrates bacterial genome extraction, preamplification based on RPA, and Cas12a/crRNA cleavage assay.