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  • Monrad Calhoun posted an update 5 hours, 23 minutes ago

    Despite considerable disparities in polymer chemical structures, the protein-polymer interactions promoting thermal stabilization show a notable degree of conservation. Our study revealed a clear relationship between polymer chain length and the thermal stability of protein-polymer bonds, which was observed across chemically disparate polymers. Extensive analysis of our data indicates that numerous polymers are likely candidates for engineering conjugate properties, offering useful guidelines for conjugate design strategies.

    The ability of materials to display both persistent porosity and high-temperature magnetic order could have profound implications for fundamental physics and emerging technologies. The desolvation of the archetypal molecule-based magnet and magnonic material V(TCNE)2 (TCNE = tetracyanoethylene) is demonstrated to yield a room-temperature microporous magnet. V(CO)6’s solution-phase reaction with TCNE results in the formation of V(TCNE)2095CH2Cl2, an entity whose characteristic temperature, T*, is estimated at 646 K through a Bloch fit analysis of variable-temperature magnetization data. Under reduced pressure conditions, the removal of the solvent results in the activated compound V(TCNE)2, which exhibits a T* value of 590 K and inherent microporosity (with a Langmuir surface area of 850 m²/g). Small gas molecules, specifically H2, N2, O2, CO2, ethane, and ethylene, are able to gain access to the porous structure found in V(TCNE)2. V(TCNE)2’s electron transfer with O2 is thermally activated, whereas the other gases under study experience physisorption. A relatively minor modification to the T* value of V(TCNE)2 occurs with the adsorption of H2 (T* = 583 K) or CO2 (T* = 596 K), in contrast to the substantially reduced T* value observed after ethylene insertion (T* = 459 K). smad signaling These results show an initial manifestation of microporosity within a room-temperature magnet, signifying the prospect of incorporating small-molecule guests, potentially even molecular qubits, into future applications.

    Directly modifying inert C-H bonds to construct molecules in organic chemistry is a strategy that presents both appeal and substantial difficulty. Unveiled herein is an unparalleled, earth-abundant Cu/Cr catalytic system which effects the transformation of unreactive alkyl C-H bonds into nucleophilic alkyl-Cr(III) species at room temperature, thus enabling carbonyl addition reactions with strong alkyl C-H bonds. Even on a gram scale, diverse aryl alkyl alcohols can be created utilizing mild reaction conditions. This novel radical-to-polar crossover strategy is additionally employed for the 11-difunctionalization of aldehydes using alkanes and a range of nucleophiles. Investigations into the mechanism show the aldehyde participating as both a reactant and a photosensitizer, facilitating the regeneration of the copper and chromium catalysts.

    Depending on their composition, suspensions of polymeric nano- and microparticles, which are fascinating stress-responsive material systems, display diverse flow properties including, but not limited to, drastic thinning, thickening, and reversible solidification, a phenomenon driven by shear. While prior investigations have overwhelmingly addressed non-responsive particles, this approach does not accommodate in-situ flow property adjustments. The chemical structure of polymeric materials dictates their phase transitions, allowing the design of versatile adaptive materials that respond dynamically to specific environmental stimuli. Micrometer-sized, readily prepared, polymeric particles with accessible glass transition temperatures (Tg) are suspended and reported in this work, with their non-Newtonian rheology controlled thermally. The underlying mechanical stiffness and interparticle friction exhibit dramatic variations in the area surrounding the glass transition temperature, Tg. The suspensions’ transit through the particles’ T_g is shown to induce a dramatic and non-monotonic change in shear thickening, distinct from the behavior in conventional systems, leveraging these properties. The straightforward strategy of modulating temperature relative to Tg allows for the in situ activation or deactivation of shear jamming within the system, establishing a foundation for further development of stimuli-responsive jamming systems with polymer chemistry at their core.

    High resistance to mass transport within the catalyst layer is a primary limitation in the performance and platinum loading parameters of proton exchange membrane fuel cells (PEMFCs). The catalyst binder, a novel partially ordered phosphonated ionomer (PIM-P), was conceived to resolve the issue by improving electrode mass transport, featuring both an intrinsic microporous structure and proton-conductive functionality. The inflexible and twisted structure of PIM-P hinders the unrestricted motion of its conformation and the optimal packing of polymer chains, consequently leading to the creation of a strong gas transport pathway. Phosphonated groups contribute to a stable framework for proton conduction, ensuring predictable and reliable movement. Efficient mass transport pathways are facilitated by the construction of an orderly molecular chain stacking, a result of strategically incorporating fluorinated and phosphonated groups into the local side chains based on group assembly. Under the exacting conditions of 160°C and a hydrogen-oxygen environment, the peak power density of membrane electrode assemblies containing PIM-P ionomer demonstrates a 18-379% improvement compared to assemblies featuring commercial or porous catalyst binders. This study highlights the essential part of an ordered framework in polymers with inherent micro-pores for rapid charge conduction, offering a unique approach for better mass transportation at electrodes focusing on structural optimization in place of complex processing.

    This correspondence summarizes a recent ACS Central Science study evaluating elemental analysis laboratory performance. The analysis prompts a broader conclusion encompassing the advantages of metrology and international quality standards.

    Applications in X-ray detection and imaging have been significantly enhanced by lead-free organic metal halide scintillators, which have low-dimensional electronic structures and excellent optoelectronic properties. (18-crown-6)2Na2(H2O)3Cu4I6 (CNCI), a zero-dimensional organic copper halide, exhibiting negligible self-absorption and near-unity green-light emission, was successfully incorporated into X-ray imaging scintillators, demonstrating remarkable X-ray sensitivity and imaging resolution. A novel CNCI/polymer composite scintillator was produced, showing an extraordinarily high light output of 109,000 photons per MeV, a top-tier result in the field of scintillator materials. Simultaneously, the extreme sensitivity, achieving a detection limit of 594 nGy/s, was significantly enhanced, being about 92 times less than the dose in a typical medical test. In addition, the spatial imaging resolution of the CNCI scintillator was refined through the utilization of a silicon template, owing to the light’s wave-guiding behavior within the CNCI-filled pores. The pixelated CNCI-silicon array scintillation screen displays a spatial resolution of 248 line pairs per millimeter (lp/mm), a remarkable feat compared to the 163 lp/mm resolution of CNCI-polymer film screens. This represents the highest resolution achieved so far in organometallic-based X-ray imaging systems. For medical radiography and security screening applications, the utilization of organic metal halides in the design of high-performance X-ray imaging scintillators presents a novel approach.

    With the persistent emergence of new SARS-CoV-2 variants, the world faces unprecedented obstacles during the ongoing COVID-19 pandemic. The occurrence of infectious disease outbreaks is an unavoidable reality, but the cumulative knowledge gathered from successful and unsuccessful encounters will pave the way for the establishment of a formidable and adaptable health system designed to manage such pandemics. Years were often required in the past to develop diagnostics, therapeutics, or vaccines, but recent advancements in high-throughput technologies coupled with unparalleled international scientific collaboration have enabled faster development and a broader range of insights. The new technology of computational protein design (CPD) has created alternative therapeutic strategies to address pandemic challenges. Besides the development of peptide-based inhibitors, miniprotein binders, decoys, biosensors, nanobodies, and monoclonal antibodies, CPD has also allowed for the redesign of native SARS-CoV-2 proteins and human ACE2 receptors. We explore the application of novel CPD strategies in the rational design and development of robust COVID-19 treatment approaches.

    SARS-CoV-2’s main protease (Mpro), with its critical role in coronavirus replication, makes it a particularly promising drug target. With the appearance of new viral variants, there is apprehension that mutations in Mpro may modify the protease’s structural and functional properties, ultimately impacting the potency of existing and potential antiviral drugs. A study of the effects of 31 mutations, encompassing 5 variants of concern (VOCs), on catalytic characteristics and substrate specificity revealed changes in peptide binding and cleavage rates. Eleven Mpro mutants’ crystal structures illuminated the structural basis for their altered functional attributes. Finally, we present evidence that Mpro mutations affect the proteolysis of the immunomodulatory protein Galectin-8 (Gal-8), resulting in a considerable decrease in cytokine production, providing further insight into the alteration of host antiviral mechanisms’ evasion. Correspondingly, the Gamma VOC and the highly virulent Delta VOC mutations produced a notable increase in the rate of Gal-8 cleavage. Importantly, the IC50 values for nirmatrelvir (Pfizer) and our irreversible inhibitor AVI-8053 were consistent across all the examined mutants, suggesting that Mpro will stay a top antiviral target as SARS-CoV-2 continues to adapt.

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