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The role and regulatory mechanism of USP25 in pancreatic microcirculatory disturbance in severe acute pancreatitis
Spatiotemporal photon distribution control on active sites enables bio-inspired methane-to-methanol conversion
Highly Efficient Deep‐Blue Room‐Temperature Phosphorescence With Tunable Long‐Lived Afterglow and Reversible Photoactivation Behavior
ABSTRACT Wide band gap organic molecule with ultralong room‐temperature phosphorescence (RTP) remains a big challenge in optoelectronic field due to the intrinsic large Stokes shift of phosphorescence relative to fluorescence, and complexity of filling and stabilizing high‐energy triplet excited states. In this work, three organic small molecules, MSPA , BSPA , and TSPA , based on succinimide and triphenylamine groups are designed and synthesized, and deep‐blue RTP with reversible photoactivation properties is successfully realized by physically doping them into polyvinyl alcohol (PVA) matrix. Notably, MSPA ‐doped film exhibits RTP at 440 nm with ultralong lifetime of 1403 ms and phosphorescence quantum yield as high as 14.32%. Theoretical calculations reveal that the efficient intersystem crossing and strong intermolecular hydrogen‐bonding interactions leads to the ultralong RTP in MSPA /PVA doping system. Taking advantages of the wide band gaps, tunable organic afterglow, and reversible photoactivation behaviors of MSPA , BSPA , and TSPA , the amorphous and flexible films are prepared and show potential applications in photoactivated information encryption, advanced anti‐counterfeiting, and multicolored displays through triplet‐to‐singlet Förster energy transfer. This work provides a reliable strategy to realize high‐performance wide band gap RTP materials and further broadening practical applications in organic optoelectronic information.
Nonalcoholic fatty liver disease assessed by multiple tools are correlated to periodontal conditions
The key role of nanoparticle concentration gradient in aerosol initial growth
Abstract New particle formation has been estimated to produce more than half of the global cloud condensation nuclei and profoundly impacts clouds, climate, and air quality. The initial growth from the cluster size ( ~ 1 nm) to a few nanometers, for which the underlying mechanisms can be very different from the subsequent growth, is the most critical stage for new particles to become climate-relevant. However, initial growth mechanisms evidenced by controlled laboratory experiments can rarely explain observations from the real atmosphere. Here we show that a large nanoparticle concentration gradient in the size space can drive unexpected rapid initial growth based on measurements across the globe. It accelerates the condensation of globally abundant oxygenated organic molecules onto a population of new particles compared to a single particle, and substantially increases the fraction of new particles that survive to climate- and air-quality-relevant sizes. Our findings provide insights into explaining the puzzle of the frequent new particle formation events in polluted urban environments and indicate an even more important role of new particle formation in climate predictions.
Iridium‐Catalyzed Enantioselective Allylation of Alkynylboronates to Access Chiral 1,4‐Dienes
ABSTRACT Skipped dienes, particularly 1,4‐dienes, play significant roles in pharmaceuticals and organic synthesis as they serve as key intermediates for the construction of complex structures and also bioactive molecules. However, the catalytic assembly of this motif with high stereoselectivity from readily available starting materials remains a substantial synthetic challenge. Herein, we reported a direct iridium‐catalyzed enantioselective allylation reaction with allylic electrophiles and alkynyl boronates, resulting in various 1,4‐dienes with excellent Z/E ratios and enantioselectivity. The reaction proceeds through a concerted mechanism that involves an allylation‐induced 1,2‐migration of the alkynyl boronate, followed by a syn ‐addition of the migrating group and Ir( π ‐allyl) complex across the alkynyl fragment to selectively deliver the more challenging Z‐alkenes. DFT calculations clarify the origins of the observed high chemo‐ and stereoselectivity. Furthermore, this method demonstrates a broad substrate scope, and the resulting enantiomerically enriched 1,4‐diene products can be readily derivatized.
Green synthesis of silver nanoparticles from Eichhornia crassipes and evaluates their antimicrobial properties against multidrug-resistant UTI pathogens
Reversible surface modifications of functional proteins for accelerated cytosolic delivery via cell-penetrating peptide clusters
Abstract A long-standing goal in biomedical research is to label and manipulate intracellular targets, which could be achieved through the cytosolic delivery of exogenous functional proteins. The development of Tat clusters has advanced the nontoxic intracellular delivery of functional antibodies at low concentrations, but the variety of proteins that can be successfully delivered remains limited. Here, we find that by simply reversibly modifying the surface of functional proteins with anionic peptide patches, various protein cargoes (which are normally difficult to deliver) can be delivered into living cells by synergetic electrostatic interactions with the cationic cell-penetrating peptide clusters TAT 3 . To demonstrate the applicability of this approach, we successfully deliver functional proteins with widely varying molecular weights (∼1.5 kDa to 430 kDa) and isoelectric points (less than 5 to greater than 9) into the cytosol of cells. By exploiting this method, we also achieve protein delivery in plant tissues, which is more challenging due to the presence of intact plant cell walls. This strategy is further applied for the cytosolic delivery of synthetic protein probes carrying posttranslational modifications (PTMs), which can aid in in situ mapping of the intracellular PTM-mediated interactome. Overall, this strategy is expected to enrich cytosolic protein delivery technology and help to repurpose a wide range of customized and therapeutic proteins for emerging intracellular applications.
Enzyme‐Mimicking Metal–Phosphide Tandem Catalytic Centers for Efficient Electrochemical Nitrate‐to‐Ammonia Conversion and Zinc–Nitrate Battery
ABSTRACT Achieving spatially coupled and functionally complementary active sites in synthetic catalysts remains a significant challenge. Inspired by the enzymatic cascade involving nitrate reductase and nitrite reductase, we report a nanozyme comprising iron clusters and iron‐doped nickel phosphide nanoparticles on CeO 2 nanorods (Fe–Fe x Ni 2−x P/CeO 2 ) in proximity for efficient electrocatalytic nitrate‐to‐ammonia conversion and Zn–NO 3 − battery. The Fe clusters serve as nitrate reductase mimics, promoting the deoxygenation step of NO 3 − to NO 2 − , while the adjacent Fe x Ni 2−x P nanoparticles serve as nitrite reductase mimics, accelerating the subsequent hydrogenation steps to NH 3 . The CeO 2 nanorods stabilize the dual active sites and function as proton reservoirs to suppress the hydrogen evolution reaction. Thus, the nanozyme delivers exceptional performance in NH 3 electrosynthesis, achieving a high yield rate of 43.5 mg h −1 cm −2 with a Faradaic efficiency (FE) of 91.2% at –0.7 V versus RHE in an H‐type cell and an industrial‐level current density of 800 mA cm −2 for over 100 h under flow‐cell conditions (FE NH3 > 90%) at the same potential. When employed Fe–Fe x Ni 2−x P/CeO 2 as a cathode in a rechargeable Zn–NO 3 − battery, it enables simultaneous NH 3 production and power generation, delivering a peak power density of 21.1 mW cm −2 and an NH 3 yield rate of 1.9 mg h −1 cm −2 .
Evolutionary reinforcement learning framework for energy-efficient fault resilience and topological stability in WSNs
One-pot co-upcycling of mixed polyolefin waste
Resolving the Efficiency–Mechanical Trade‐off in Organic Solar Cells: 20.4% Enabled by Hydrogen‐Bonding Engineering
ABSTRACT Organic solar cells (OSCs) face a trade‐off between power conversion efficiency (PCE) and mechanical robustness: high toughness requires low‐crystallinity amorphous polymers, which impair photovoltaic performance. Herein, we propose a strategy combining random copolymerization and hydrogen‐bonding modulation to resolve this conflict. First, the incorporation of an ester‐substituted thiophene yields PM6‐H, exhibiting improved toughness (high crack‐onset strain, COS ) but lower PCE. Subsequently, introducing ─OH and ─OOCNHC 6 H 13 groups at the terminals of alkyl chains forms PM6‐OH and PM6‐UR. The hydrogen bonding serves dual functions: acting as dynamic cross‐linking sites to further enhance mechanical properties while restoring optimal lamellar stacking for efficient charge transport. As a result, these copolymers simultaneously achieve a COS exceeding 46%, a high PCE of up to 20.4%, and superior storage, thermal, and light stability (with T 80 being twice that of the PM6 benchmark). Flexible OSCs fabricated using these donor polymers deliver a PCE of 18.22% while maintaining outstanding flexibility, with ∼90% PCE retention after 2200 bending cycles (vs. 78% for controls). This work demonstrates that copolymerization with controlled hydrogen‐bonding interactions overcomes the efficiency‐robustness trade‐off in OSCs through precise structural modulation, paving the way for high‐performance, mechanically durable, and stable OSCs suitable for practical applications.
Food insecurity and associated factors among adult cancer patients in south Ethiopia: a cross-sectional study
Embryo metabolite analysis and implantation potential prediction using chemiluminescent microfluidic chips with dielectric wetting valves
Engineering Fluoroacetate Dehalogenase by Growth‐Based Selections on Non‐Natural Organofluorides
ABSTRACT The widespread use of organofluorides in modern society has inadvertently led to the bioaccumulation of harmful pollutants, most prominently per‐ and polyfluorinated alkyl substances (PFAS). In principle, tailored biocatalysts able to cleave C─F bonds represent an attractive strategy to combat this (emerging) environmental crisis. However, Nature is largely impartial to C─F bonds, with fluoroacetate dehalogenases (FAcDs) standing out by catalyzing the hydrolysis of single C─F bonds in fluoroacetate at high turnover rates. To harness its catalytic prowess for non‐natural organofluorides, we designed and applied a robust growth‐based selection strategy for large‐scale FAcD engineering. Specifically, we demonstrate that FAcD‐catalyzed C─F bond cleavage of (natural and) synthetic organofluorides generates metabolizable carbon sources for bacteria, enabling in vivo enrichment of active FAcD variants. By forcing populations expressing diverse FAcD‐libraries to utilize various organofluorides as sole carbon source, we elicited a panel of FAcD variants with improved activities and altered substrate profiles for fluoroacetate, 2‐fluoropropionate, and 2,2‐difluoroacetate. In these efforts, we also identified a previously overlooked inhibition pathway, which impedes the conversion of gem‐difluoride compounds. Overall, our study presents the first large‐scale engineering campaign of FAcDs and introduces an operationally simple selection platform to adapt these enzymes for the sustainable degradation of contaminating organofluorides.
Preliminary reference range for B cell subpopulations in peripheral blood of healthy Malaysian children aged 2–15 years
Abstract Physicians rely on reference values from healthy populations to guide clinical decisions regarding B-cell subpopulations in primary immunodeficiency. While age-dependent reference ranges have been reported in several populations, no study has established these values for Malaysian children. Given that B-cell subpopulation distributions may vary between populations, we aimed to define reference ranges for total B cells, transitional B cells, naïve B cells, total memory B cells, switched and non-switched memory B cells, and plasmablasts in Malaysian children aged 2 to 15 years. Blood samples taken from 85 children aged 2 to 15 years were evaluated for the distribution of B cell subsets. Absolute numbers and percentages were determined for total B cells (CD19 + ), transitional B cells (CD19 + CD27 − CD24 + bright CD38 +bright ), naïve B cells (CD19 + CD27 − IgD + ), total memory B cells (CD19 + CD27 + ), class-switched memory B cells (CD19 + CD27 + IgM − IgD − ), non-classical switched memory B cells(CD19 + CD27 − IgM − IgD − ), non-switched memory B cells (CD19 + CD27 + IgM + IgD + ), and plasmablasts (CD19 + CD27 + CD38 + bright ). We observed age-dependent variations in most B-cell subpopulations, with naïve B cells being predominant, followed by memory B cells, while plasmablasts were present in trace amounts across all ages. Additionally, certain of B-cell subpopulations (total memory B cells and class-switched memory B cells) were observed at higher frequencies in female children compared to males. This study provides age-specific reference values for B cell subsets in a paediatric population, which may serve as a valuable guideline for diagnosing children with suspected immunodeficiency.
Persistent semiquinone radicals enable efficient near-infrared-driven H2O2 photosynthesis
Modulation of Local Hydrogen Bonding for Highly Efficient Bi‐MOFs Photocatalyzed Fixation of N <sub>2</sub> in Aqueous Solution
ABSTRACT For photocatalytic reduction of dinitrogen in aqueous solution, water plays an important role as not only a reactant to supply protons via the water oxidation reaction, but also a solvent, which cannot be neglected. At the interface between the catalyst surface and local water molecules, modulation of the hydrogen bonds (HBs) is critical for improving the production rate of ammonia. Herein, both roles (i.e., reactant and solvent) were balanced through the formation of an interfacial HB network between organic ligands of Bi‐MOFs and water with the aim of accelerating water oxidation to produce more protons and facilitating the adsorption of N 2 as well as the release of free water molecules. With this approach, the ammonia synthesis rate reached 258.86 µmol·g −1 ·h −1 at ambient conditions. As demonstrated, the empty 6p orbitals present in Bi 3+ (6s 2 6p 0 ), can accept electrons from the ligands due to the ligand‐to‐metal charge transfer (LMCT) effect. These electrons are then transferred to the π* antibonding orbitals of N 2 , thus significantly weakening the N≡N bond. The photogenerated holes on the ligands oxidize hydrogen‐bonded water molecules, producing more protons, which can further promote the critical process, namely the proton‐coupled electron transfer (PCET), for the multi‐step hydrogenation of N 2 . Therefore, the dynamic balance among N 2 adsorption and activation, proton supply capacity, and proton transfer was achieved through a local microenvironment modulation strategy on MOFs. As a further proof, a phototactically produced NH 4 + solution with a concentration of approx. 200 mg·L −1 was concentrated and used as a fertilizer. Overall, this work provided a new design strategy for the photocatalytic reduction of N 2 to produce ammonia on MOFs by elucidating the key role of the HB network.
Study on inter-segment interference mechanisms and patterns between horizontal well sections in a combined well pattern of horizontal and vertical wells in offshore oilfields
Abstract In the development of heavy oil fields in the Bohai Sea, the “horizontal + directional” well pattern has significantly improved recovery rates. However, as the oilfield enters the ultra-high water cut stage, changes in waterflooding behavior and production characteristics lead to a more complex distribution of remaining oil, posing challenges for subsequent development. This study introduces a dynamic interference analysis method that integrates three-dimensional (3D) physical modeling with numerical simulation. The method optimizes the interference prediction model under the “horizontal + directional” well pattern, aiding in well placement optimization and enhancing development efficiency during the ultra-high water cut period. Additionally, a phenomenon was observed where remaining oil concentrates in the central segment during the displacement process. Through numerical simulations under varying permeability rhythms, the impact of the injection-production relationship on the distribution of remaining oil was revealed, providing a theoretical foundation for well pattern optimization. The findings offer technical support for the continued development of Bohai Oilfields under ultra-high water cut conditions and provide valuable guidance for other offshore heavy oil fields. The new methods proposed in this study can improve recovery rates in complex waterflood environments.