electronic proximity

The construction of defective sites is one of the effective strategies to create high-activity Metal-Organic frameworks (MOFs) catalysts. However, traditional synthesis methods usually suffer from cumbersome synthesis steps and disordered defect structures. Herein, a cluster-cluster co-nucleation (CCCN) strategy is presented that involves the in situ introduction of size-matched functional polyoxometalates (H6 P2 W18 O62 , {P2 W18 }) to intervene the nucleation process of cluster-based MOFs (UiO-66), achieving one-step inducement of exposed defective sites without redundant post-processing...

Light-chain proximal tubulopathy (LCPT) is typically characterized by the intracytoplasmic deposition of light chains within the proximal tubular epithelial cells, which is usually classified into crystalline and noncrystalline subgroups. Membranous nephropathy (MN) is a common glomerular disease characterized by diffused subepithelial electron-dense deposits along the capillary loop accompanied by the effacement and microvillus transformation of the foot process. Here, we report a biopsy-confirmed case of a concurrence of LCPT with crystals (κ light chains restricted) and antigen-undetermined MN in a male patient...

BACKGROUND: Exposure to repetitive pain during the neonatal period has been shown to have important short and long-term effects on the neurodevelopment of the premature neonate and can contribute to experienced prolonged pain. A uniform taxonomy of neonatal prolonged pain is still lacking to this day which contributes to suboptimal prolonged pain management in neonatal intensive care units. Accordingly, a scoping review exploring the state of knowledge about prolonged pain in preterm neonates hospitalised in the neonatal intensive care unit will contribute to the developing field of neonatal prolonged pain and provide recommendations for clinical prolonged pain management...

A sterically encumbered trans -A2 B-corrole possessing a perylenediimide (PDI) scaffold in close proximity to the macrocycle has been synthesized via a straightforward route. Electronic communication as probed via steady-state absorption or cyclic voltammetry is weak in the ground state, in spite of the corrole ring and PDI being bridged by an o -phenylene unit. The TDDFT excited-state geometry optimization suggests after excitation the interchromophoric distance is markedly reduced, thus enhancing the through-space electronic coupling between the corrole and the PDI...

The sluggish kinetics for anodic oxygen evolution reaction (OER) and insufficient catalytic performance over the corresponding Ir-based catalysts are still enormous challenges in proton exchange membrane water electrolyzer (PEMWE). Herein, we report that KIr4 O8 nanowires anode catalyst with more exposed active sites and rich hydroxyl achieves a current density of 1.0 A/cm2 at 1.68 V and possesses excellent catalytic stability with 1230 h in PEMWE. Combining in situ Raman spectroscopy and differential electrochemical mass spectroscopy results, we propose the modified adsorbate evolution mechanism that rich hydroxyl in the inherent structure of KIr4 O8 nanowires directly participates in the catalytic process for favoring the OER...

By integration of oxocarbenium activation and Lewis acid coordination activation via conformational proximity-driven, Pd(II)- or Cu(I)-catalyzed intramolecular ketone haloacylation, regio- and stereoselective heterolytic ring-opening 1,5-haloacylation of cyclopropyl ketones, including those with weak single alkyl donors, has been developed for the synthesis of valuable α-quaternary halo-γ-butenolides. The vicinal carboxylic acid and ketone acceptors are no longer just spectator activators. Further, this reaction delivers a constant regioselectivity regardless of the electronic nature of substituents, even the malonate...

Using the density functional theory, we conducted a study on the electrification upon contact between hydrophobic liquid molecules and water molecules, revealing localized characteristics of contact-electrification. These "localized features" refer to the specific microscale characteristics where electron transfer predominantly occurs at the contact regions, influenced by factors such as atomic distances and molecular orientations. Although the electrostatic potential and the highest occupied molecular orbital-lowest unoccupied molecular orbital gap offer substantial predictive insights for electron transfer across polymer interfaces, they fall short in capturing the complexities associated with the interaction between hydrophobic liquids and water molecules...

METHODS: Five electronic databases (PubMed (Medline), Web of Science, Embase, Sport Discus, and Cochrane Library) were searched for controlled trials that assessed the MPS response to RE in healthy, adult humans, postabsorptive state. Individual study and random-effects meta-analysis arewere used to inform the effects of RE and covariates on MPS. Results from 79 controlled trials with 237 participants were analysed. RESULTS: Analysis of the pooled effects revealed robust increases in MPS following RE (weighted mean difference (WMD): 0...

DNA double-strand breaks occur in all human cells on a daily basis and must be repaired with high fidelity to minimize genomic instability 1 . Deficiencies in high-fidelity DNA repair by homologous recombination lead to dependence on DNA polymerase theta, which identifies DNA microhomologies in 3' single-stranded DNA overhangs and anneals them to initiate error-prone double-strand break repair. The resulting genomic instability is associated with numerous cancers, thereby making this polymerase an attractive therapeutic target 2,3 ...

BACKGROUND: Midwives may be key stakeholders to improve perinatal mental healthcare (PMHC). Three systematic reviews considered midwives' educational needs in perinatal mental health (PMH) or related interventions with a focus on depression or anxiety. This systematic review aims to review: 1) midwives' educational/training needs in PMH; 2) the training programs in PMH and their effectiveness in improving PMHC. METHODS: We searched six electronic databases using a search strategy designed by a biomedical information specialist...

Direct interspecies electron transfer (DIET) is essential for maintaining the function and stability of anaerobic microbial consortia. However, only limited natural DIET modes have been identified and DIET engineering remains highly challenging. Here, an unnatural DIET between Shewanella oneidensis MR-1 (SO, electron donating partner) and Rhodopseudomonas palustris (RP, electron accepting partner) was artificially established by a facile living cell-cell click chemistry strategy. By introducing alkyne- or azide-modified monosaccharides onto the cell outer surface of the target species, precise covalent connections between different species in high proximity were realized via a fast click chemistry reaction...

ConspectusNature has established a sustainable way to maintain aerobic life on earth by inventing one of the most sophisticated biological processes, namely, natural photosynthesis, which delivers us with organic matter and molecular oxygen derived from the two abundant resources sunlight and water. The thermodynamically demanding photosynthetic water splitting is catalyzed by the oxygen-evolving complex in photosystem II (OEC-PSII), which comprises a distorted tetramanganese-calcium cluster (CaMn4 O5 ) as catalytic core...

BACKGROUND: Influenza vaccination is recommended for Australians 18+ years old with medical risk factors, but coverage is suboptimal. We aimed to examine whether automatic, opportunistic patient reminders (SMS and/or printed) before appointments with a general practitioner increased influenza vaccination uptake. METHODS: This clustered non-randomised feasibility study in Australian general practice included patients aged 18-64 years with at least one medical risk factor attending participating practices between May and September 2021...

We studied the electronic properties of a high-temperature superconductor in proximity to a ferromagnetic material in a bilayer film of La0.67 Sr0.33 MnO3 (LSMO)/YBa2 Cu3 O7 (YBCO). High-quality single-crystalline films of YBCO and LSMO/YBCO were grown epitaxially on an SrTiO3 (001) surface. Magnetization data of the LSMO/YBCO bilayer exhibit ferromagnetic transition at about 255 K, which is much smaller than the Curie temperature of bulk LSMO. Experimental data show the emergence of magnetic anisotropy with cooling, which becomes significantly stronger in the superconducting phase...

Metabolic homeostasis within cells and tissues requires engagement of catabolic and anabolic pathways consuming nutrients needed to generate energy to drive these and other subcellular processes. However, the current understanding of cell homeostasis and metabolism, including how cells utilize nutrients, comes largely from tissue and cell models analyzed after fractionation. These bulk strategies do not reveal the spatial characteristics of cell metabolism at the single cell level, and how these aspects relate to the location of cells and organelles within the complexity of the tissue they reside within...

In the last decade, graphene has become an exciting platform for electron optical experiments, in some aspects superior to conventional two-dimensional electron gases (2DEGs). A major advantage, besides the ultra-large mobilities, is the fine control over the electrostatics,
which gives the possibility of realising gap-less and compact p-n interfaces with high precision. The latter host non-trivial states, \eg, snake states in moderate magnetic fields, and serve as building blocks of complex electron interferometers...

We report an improved and efficient method to prepare well-defined, structurally complex truxinate cyclobutane polymers via a thioxanthone sensitized solution state [2 + 2] photopolymerization. Monomers with varying electron density and structure polymerize in good to excellent yields to afford a library of 42 polyesters. Monomers with internal olefin separation distances of greater than 5 Å undergo polymerization via intermolecular [2 + 2] photocycloaddition readily, as opposed to the intramolecular [2 + 2] photocycloaddition observed in monomers with olefins in closer proximity...

The emergence and rapid spread of Mpox (formerly monkeypox) have caused significant societal challenges. Adequate and appropriate diagnostics procedures are an urgent necessity. Herein, we discover a pair of aptamers through the systematic evolution of ligands by exponential enrichment (SELEX) that exhibit high affinity and bind to different sites towards the A29 protein of the Mpox virus. Subsequently, we propose a facile, sensitive, convenient CRISPR/Cas12a-mediated aptasensor for detecting the A29 antigen...

Polythiophene (PT) is an important conducting polymer for its outstanding optoelectronic properties. Here, we delineate the self-assembly-driven optoelectronic properties of PT-peptide and PT-polymer conjugates, taking examples from recent literature reports. PT-peptide conjugates made by both covalent and noncovalent approaches are discussed. Poly(3-thiophene acetic acid) (P3TAA) covalently coupled with Gly-Gly-His tripeptide, C-protected and deprotected tripeptide H2 N-F-F-V-OMe, etc. exhibits self-assembly-driven absorbance, fluorescence, photocurrent, and electronic properties...

Solar-driven upgrading of biomass-derived 5-hydroxylmethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) holds great promise for sustainable production of bio-plastics and resins. However, the process is limited by poor selectivity and sluggish kinetics due to the vertical coordination of HMF at relatively strong metal sites. Here, we purposely developed a Cu(II) porphyrin framework featuring side-chain incorporated urea linkages, denoted as TBUPP-Cu MOF, to render HMF a weak hydrogen bond at the urea site and flat adsorption via π-π stacking with the benzyl moiety...