Mathewsfoldager7208
It is evident that the exhaustive use of fossil fuels for decades has significantly contributed to global warming and environmental pollution. To mitigate the harm on the environment, lithium-oxygen batteries (LOBs) with a high theoretical energy density (3458 Wh kg-1Li2O2) compared to that of Li-ion batteries (LIBs) have been considered as an attractive alternative to fossil fuels. For this purpose, porous carbon materials have been utilized as promising air cathodes owing to their low cost, lightness, easy fabrication process, and high performance. However, the challenge thus far lies in the uncontrollable formation of Li2CO3 at the interface between carbon and Li2O2, which is detrimental to the stable electrochemical performance of carbon-based cathodes in LOBs. In this work, we successfully protected the surface of the free-standing carbon nanofibers (CNFs) by coating it with a layer of iridium metal through direct sputtering (CNFs@Ir), which significantly improved the lifespan of LOBs. Moreover, the Ir would play a secondary role as an electrochemical catalyst. This all-in-one cathode was evaluated for the formation and decomposition of Li2O2 during (dis)charging processes. Compared with bare CNFs, the CNFs@Ir cathode showed two times longer lifespan with 0.2 VLi lower overpotentials for the oxygen evolution reaction. We quantitatively calculated the contents of CO32- in Li2CO3 formed on the different surfaces of the bare CNFs (63% reduced) and the protected CNFs@Ir (78% reduced) cathodes after charging. The protective effects and the reaction mechanism were elucidated by ex situ analyses, including scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy.Protein-protein interactions (PPIs) are an essential part of correct cellular functionality, making them increasingly interesting drug targets. While Förster resonance energy transfer-based methods have traditionally been widely used for PPI studies, label-free techniques have recently drawn significant attention. These methods are ideal for studying PPIs, most importantly as there is no need for labeling of either interaction partner, reducing potential interferences and overall costs. Already, several different label-free methods are available, such as differential scanning calorimetry and surface plasmon resonance, but these biophysical methods suffer from low to medium throughput, which reduces suitability for high-throughput screening (HTS) of PPI inhibitors. Differential scanning fluorimetry, utilizing external fluorescent probes, is an HTS compatible technique, but high protein concentration is needed for experiments. To improve the current concepts, we have developed a method based on time-resolved luminescence, enabling PPI monitoring even at low nanomolar protein concentrations. This method, called the protein probe technique, is based on a peptide conjugated with Eu3+ chelate, and it has already been applied to monitor protein structural changes and small molecule interactions at elevated temperatures. Here, the applicability of the protein probe technique was demonstrated by monitoring single-protein pairing and multiprotein complexes at room and elevated temperatures. The concept functionality was proven by using both artificial and multiple natural protein pairs, such as KRAS and eIF4A together with their binding partners, and C-reactive protein in a complex with its antibody.Continuous emission of carbon dioxide gas (CO2) poses a significant effect on ambient environment, crop production, and human health, necessitating further improvement of CO2 monitoring especially at low concentrations. To overcome the obstacles of elevated operation temperatures and faint response encountered by traditional CO2-sensitive materials such as metal oxides and perovskites, a nitrogen-doped MXene Ti3C2T x (N-MXene)/polyethyleneimine (PEI) composite film decorated with reduced graphene oxide (rGO) nanosheets was initiatively leveraged in this work to detect 8-3000 ppm CO2 gas. Through subtle optimization in the aspects of componential constitutions, operation temperatures, PEI loading amounts, and relative humidity (RH), the ternary sensors with a PEI concentration of 0.01 mg/mL exhibited a reversible and superior performance over other counterparts under 62% RH at room temperature (20 °C). Apart from the inspiring detection limit of 8 ppm, favorable selectivity, repeatability, and long-term stability were demonstrated as well. During the humid CO2 sensing of the composites, few rGO nanosheets acted as an excellent conduction platform to transfer and collect charge carriers. Layered N-MXene offered more active sites for coadsorption of both CO2 and water, thereby facilitating the water-involving reactions. Rich amino groups of the PEI polymer were beneficial to bind CO2 molecules and thus induce appreciable density variation of charge carriers via proton-conduction behavior. This work initiatively offers an alternative ion-conduction strategy to detect ppm-level CO2 gas by harnessing rGO/N-MXene/PEI composites under a humid atmosphere at room temperature, simultaneously broadening the discrimination range of MXene-related gas sensing.Long-term stability of perovskite solar cells (PSCs) is one of the main issues to be solved for forthcoming commercialization of this technology. In this work, thermosetting polyurethane (PU)-based resins are proposed as effective encapsulants for perovskite solar cells to prevent degradation caused by both moisture and oxygen. Application consists of drop-casting the precursor mixture directly over the devices followed by in situ polymerization, avoiding the use of other adhesives. PUs are cost-effective, lightweight, thermal, and light-stable materials whose mechanical, chemical, and physical properties can be easily tuned by thoughtful choice of their precursor. Encapsulated PSCs show extremely good stability when stored under ambient light (maximum, 1000 lux), controlled humidity (28-65%), and temperature (18-30 °C) by retaining 94% of the initial power conversion efficiency after 2500 h (4 months), whereas control devices lose 90% of their performance after 500 h (T80 = 37 h); once stored according to ISOS-D-1, PU-protected devices showed T80 > 1200 h. Encapsulated devices are stable even when immersed in pure water. The demonstration of PUs as promising solution-processed encapsulant materials for PSCs can pave the way for these to become a cost-effective encapsulation route alternative for future industrialization of this technology.Integrating carbon nitride with graphene into a lateral heterojunction would avoid energy loss within the interlaminar space region on conventional composites. To date, its synthesis process is limited to the bottom-up method which lacks the targeting and homogeneity. Herein, we proposed a hydrogen-initiated chemical epitaxial growth strategy at a relatively low temperature for the fabrication of graphene/carbon nitride in-plane heterostructure. Theoretical and experimental analysis proved that methane via in situ generation from the hydrogenated decomposition of carbon nitride triggered the graphene growth along the active sites at the edges of confined spaces. With the enhanced electrical field from the deposited graphene (0.5%), the performances on selective photo-oxidation and photocatalytic water splitting were promoted by 5.5 and 3.7 times, respectively. Meanwhile, a 7720 μmol/h/g(graphene) hydrogen evolution rate was acquired without any cocatalysts. This study provides an top-down strategy to synthesize in-plane catalyst for the utilization of solar energy.Evolving antimicrobial resistance has motivated the search for novel targets and alternative therapies. see more Caseinolytic protease (ClpP) has emerged as an enticing new target since its function is conserved and essential for bacterial fitness, and because its inhibition or dysregulation leads to bacterial cell death. ClpP protease function controls global protein homeostasis and is, therefore, crucial for the maintenance of the bacterial proteome during growth and infection. Previously, acyldepsipeptides (ADEPs) were discovered to dysregulate ClpP, leading to bactericidal activity against both actively growing and dormant Gram-positive pathogens. Unfortunately, these compounds had very low efficacy against Gram-negative bacteria. Hence, we sought to develop non-ADEP ClpP-targeting compounds with activity against Gram-negative species and called these activators of self-compartmentalizing proteases (ACPs). These ACPs bind and dysregulate ClpP in a manner similar to ADEPs, effectively digesting bacteria from the inside out. Here, we performed further ACP derivatization and testing to improve the efficacy and breadth of coverage of selected ACPs against Gram-negative bacteria. We observed that a diverse collection of Neisseria meningitidis and Neisseria gonorrhoeae clinical isolates were exquisitely sensitive to these ACP analogues. Furthermore, based on the ACP-ClpP cocrystal structure solved here, we demonstrate that ACPs could be designed to be species specific. This validates the feasibility of drug-based targeting of ClpP in Gram-negative bacteria.It is challenging to fabricate plasmonic nanosensors on high-curvature surfaces with high sensitivity and reproducibility at low cost. Here, we report a facile and straightforward strategy, based on an in situ growth technique, for fabricating glass nanofibers covered by asymmetric gold nanoparticles (AuNPs) with tunable morphologies and adjustable spacings, leading to much improved surface-enhanced Raman scattering (SERS) sensitivity because of hotspots generated by the AuNP surface irregularities and adjacent AuNP coupling. First, nanosensors covered with uniform and well-dispersed citrate-capped spherical AuNPs were constructed using a polystyrene-b-poly(4-vinylpyridine) (PS-P4VP, with 33 mol % P4VP content and 61 kg/mol total molecular weight) block copolymer brush-layer templating method, and then, the deposited AuNPs were grown to asymmetric AuNPs. AuNP morphologies and hence the optical characteristics of AuNP-covered glass nanofibers were easily controlled by the choice of experimental parameters, such as the growth time and growth solution composition. In particular, tunable AuNP average diameters between about 40 and 80 nm with AuNP spacings between about 50 and 1 nm were achieved within 15 min of growth. The SERS sensitivity of branched AuNP-covered nanofibers (3 min growth time) was demonstrated to be more than threefold more intense than that of the original spherical AuNP-covered nanofibers using a 633 nm laser. Finite-difference time-domain simulations were performed, showing that the electric field enhancement is highest for intermediate AuNP diameters. Furthermore, SERS applications of these nanosensors for H2O2 detection and pH sensing were demonstrated, offering appealing and promising candidates for real-time monitoring of extra/intracellular species in vitro and in vivo.Hexagonal boron nitride (h-BN) can be used as a p-doped material in wide-bandgap optoelectronic heterostructures or as a release layer to allow lift-off of grown three-dimensional (3D) GaN-based devices. To date, there have been no studies of factors that lead to or prevent lift-off and/or spontaneous delamination of layers. Here, we report a unique approach of controlling the adhesion of this layered material, which can result in both desired lift-off layered h-BN and mechanically inseparable robust h-BN layers. This is accomplished by controlling the diffusion of Al atoms into h-BN from AlN buffers grown on h-BN/sapphire. We present evidence of Al diffusion into h-BN for AlN buffers grown at high temperatures compared to conventional-temperature AlN buffers. Further evidence that the Al content in BN controls lift-off is provided by comparison of two alloys, Al0.03B0.97N/sapphire and Al0.17B0.83N/sapphire. Moreover, we tested that management of Al diffusion controls the mechanical adhesion of high-electron-mobility transistor (HEMT) devices grown on AlN/h-BN/sapphire.