Chemphyschem最新文献

The rapid rise of antibiotic resistance poses a severe global health crisis, necessitating new approaches to counter this growing threat. The problem is exacerbated in Gram-negative bacterial pathogens as many antibiotics are unable to enter these cells owing to their unique additional outer membrane barrier. In this review, we discuss the challenges of targeting Gram-negative bacteria, including the complexity of the outer membrane, as well as the presence of efflux pumps and β-lactamases that contribute to resistance. We also review solutions proposed to facilitate the entry and accumulation of antibiotics in Gram-negative bacteria. These involve using existing antibiotics in combination with other inhibitors to attack the bacterial cell synergistically. We also highlight approaches to target Gram-negative pathogens via novel modes of action, providing new strategies to tackle antibiotic resistance.

With the rapid development of science and technology and for a sustainable future, the main energy resources in the world are transitioning from fossil fuels to electricity which is conceived to play a predominant role in the future. Therefore, it is essential to develop high-performance energy-storage devices such as supercapacitors and rechargeable batteries; even though they are commercialized, intense research efforts are still devoted to further improve the device performances, e.g. energy density, safety, durability and the charging rate. In this respect, exploring new advanced materials for better devices is a promising approach. The recently emerged two-dimensional conductive metal-organic frameworks (2D c-MOFs) with their inherent electrical conductivities and porosity, rich redox active sites and tailor-made architectures and functions have attracted considerable attention among energy-storage community. The initial research results reveal 2D c-MOFs are superb and advantageous electrode materials for advanced energy storage.

Photovoltaic technologies have garnered significant attention towards generating renewable and clean energy from solar power. Quantum-dot-sensitized solar cells represent a promising third-generation photovoltaic technology that offers alternatives to conventional silicon-based solar cells due to their unique properties, their favourable optoelectronic properties for photovoltaic applications including simplified manufacturing, lower processing temperatures, enhanced flexibility, semi-transparent design, and a theoretical efficiency up to 44%. The unique characteristic of tailoring the size and composition of quantum dots makes them valuable absorber materials capable of efficiently harnessing a broader range of the solar spectrum. The potential of quantum dot-sensitized solar cells to revolutionize the field of photovoltaic technology is a cause for optimism. However, the major limitation of the overall power conversion efficiency lies in their inability to absorb ultraviolet and near-infrared. Therefore, a photovoltaic technology that can effectively harness the entire solar spectrum becomes imperative. This review discusses the synthesis and light conversion mechanisms of these solar cells. Additionally, this review offers an overview of the various advancements made in quantum dot-sensitized solar cells for enhancement in the efficiency of energy conversion. It focuses on the light-absorbing materials used, their efficiency, and the advantages and drawbacks of quantum dot solar cell technology.

Organofluorine compounds have revolutionized chemical and pharmaceutical industries, serving as essential components in numerous applications and aspects of modern life. However, their bioaccumulation and resistance to degradation have resulted in environmental pollution, posing significant risks to human and animal health. The exceptionally strong C-F bond in these compounds makes their degradation challenging, with current methods often requiring extreme experimental conditions. Therefore, the development of eco-friendly approaches that operate under milder conditions is crucial, with enzyme-mediated C-F bond cleavage strategies emerging as a particularly promising solution. In this review, we present an overview of how computational approaches, including molecular docking, molecular dynamics simulations, quantum mechanics/molecular mechanics calculations, and bioinformatics, have been utilized to investigate the mechanisms underlying enzymatic C-F bond degradation and functionalization. This review highlights how these computational approaches provide critical insights into the atomic-level interactions and energetics underlying enzymatic processes, offering a foundation for the rational design and engineering of enzymes capable of addressing the challenges posed by fluorinated compounds. This review covers several types of enzymes including: fluoroacetate dehalogenases, cysteine dioxygenase, L-2-haloacid dehalogenase, cytochrome P450, fluorinase and tyrosine hydroxylase.

The Front Cover illustrates the effects of various atmospheric gas species on an argyrodite-type sulfide solid electrolyte, Li₆PS₅Cl during moisture exposure, examined by using multiple analytical methods. The electrolyte powder was exposed to different gases: Ar, Ar+CO₂, O₂, and O₂+CO₂, all under a dew point of −20 °C. The generation of H₂S gas was unaffected by the atmospheric gases; however, the conductivity retention of the electrolyte significantly differed. CO₂ exposure promoted the formation of carbonates, whereas O₂ exposure facilitated the formation of phosphates and sulfonates. These reactions led to surface degradation and a consequent reduction in conductivity. More information can be found in the Research Article by Y. Morino, H. Sano and co-workers (DOI: 10.1002/cphc.202400872).

The Cover Feature explores a bioinspired approach to CO₂ capture by using dipeptides. A database of 960 dipeptides was analyzed by automated modeling workflows and quantum chemical methods. Statistical analysis identified amino acid subunits that enhance CO₂ binding through cooperative effects, thus offering insights into designing efficient carbon capture materials. More information can be found in the Research Article by K. D. Vogiatzis and co-workers (DOI: 10.1002/cphc.202400498).

The Cover Feature shows a micro X-ray fluorescence map and spectrum together with a pictorial view of phases characterized by different iron vacancy configurations. In addition to the vacancy-ordered and -disordered phases, an interface configuration appears in the fluorescence map. The microscopic morphology with direct implications on transport can be controlled by heat treatment. More information can be found in the Research Article by G. Campi, N. L. Saini and co-workers (DOI: 10.1002/cphc.202400363).

The term "wolfium bond" is employed to denote attractive interactions between group 6 elements and electron-rich moieties. A theoretical investigation of the wolfium bond involving the compounds WnF4O or WnF2O, where Wn represents Cr, Mo or W, and π systems such as C2H2, C2H4 and C6H6, was conducted using density functional theory (DFT) at the ωB97XD/aug-cc-pVTZ level of theory. Interaction energies range from -3.74 to -10.86 kcal/mol upon formation of the π-Wn bond. The electrostatic contributions to the interaction energy were found to be dominant. Notably, the WnF4O system exhibits greater stability than its WnF2O counterpart, with the exception of the CrFxO system. The charge transfer between the interacting molecules lies between 0.0114 and 0.0946e in magnitude. The predominant type of orbital interaction is πC-C→BD*Wn-O. Our theoretical investigation revealed the presence of weak, but significant, wolfium bonds between group 6 elements and electron-rich π systems.

The optimized structures in the configuration space of cyclo[18]carbon (C₁₈) dimers, most of which haven't been studied in detail or even discovered yet, were explored here, and their electronic structure, aromaticity and intermolecular interaction between monomers were thoroughly investigated based on quantum chemistry and various electronic wavefunction analyses. For the dimers bound by weak interaction, their dimerization interactions are contributed mainly by dispersion and less significantly by electrostatic attraction. For those bound by covalent bonds, the symmetry of their geometric structures and hence the degeneracy of out-of-plane and in-plane $\pi$ orbitals ( ${\pi }_{out}$ and ${\pi }_{in}$ ) are broken after dimerization. Also predicted are the interesting phenomena including their aromaticity or anti-aromaticity, as well as the spin polarization of their singlet ground states as a result of the distortion of their carbon rings.

Nanoalloys occupy a focal point of research across many fields as, for instance, catalysis, optics, magnetism, quantum technologies and biomedical materials. This special collection provides a panorama of the research ongoing about their synthesis, modelling and applications.