bluuebunny/crossref_metadata_2025_split huggingface dataset:
Unexpected Molecular Sieving of Xylene Isomer Using Tethered Ligand in Polymer‐Metal–Organic Frameworks (polyMOFs)
Authors: Hyun Taehoon , Park Junkil , So Jungseob , Kim Jihan , Koh Dong‐Yeun 
Published: July 2024

AbstractPromising advances in adsorption technology can lead to energy‐efficient solutions in industrial sectors. This work presents precise molecular sieving of xylene isomers in the polymer‐metal‐oragnic framework (polyMOF), a hybrid porous material derived from the parent isoreticular MOF‐1 (IRMOF‐1). PolyMOFs are synthesized by polymeric ligands bridged by evenly spaced alkyl chains, showing reduced pore sizes and enhanced stabilities compared to its parent material due to tethered polymer bridge within the pores while maintaining the original rigid crystal lattice. However, the exact configuration of the ligands within the crystals remain unclear, posing hurdles to predicting the adsorption performances of the polyMOFs. This work reveals that the unique pore structure of polyIRMOF‐1‐7a can discriminate xylene isomers with sub‐angstrom size differences, leading to highly selective adsorption of p‐xylene over other isomers and alkylbenzenes in complex liquid mixtures (αpX/OM = 15 and αpX/OME = 9). The structural details of the polyIRMOF‐1‐7a are elucidated through computational studies, suggesting a plausible configuration of alkyl chains within the polyMOF crystal, which enable a record‐high p‐xylene selectivity and stability in liquid hydrocarbon. With this unprecedented molecular selectivity in MOFs, “polymer‐MOF” hybridization is expected to meet rigorous requirements for high‐standard molecular sieving through precisely tunable and highly stable pores.
Construction of H‐Doped PdB Nanocrystals as Electrocatalysts to Modulate Formic Acid Oxidation
Authors: Li Huiling , Zhou Shangqi , Liu Jiewen , Wang Weibin , Chen Ankang , Sheng LiBo , Zhao Jingxiang , Li Yan , Sui Yongming , Zou Bo 
Published: July 2024

AbstractThe strong ligand effect in B‐doped Pd‐based (PdB) catalysts renders them a promising anode for constructing formic acid fuel cells (FAFCs) exhibiting high power density and outstanding stability. However, the enhancement of the oxidation barrier is unavoidable in this alloy system owing to the electron transfer (ET) from B to Pd. In this study, a hydrogen doping strategy is employed to open charge freedom in PdB compounds and boost their formic acid oxidation reaction (FAOR) activity by suppressing the ET process. The resulting hydrogen‐doped PdB (PdBH) exhibits an ultrahigh mass activity of up to 1.2A mg−1Pd, which is 3.23 times that of the PdB catalyst and 9.55 times that of Pd black. Detailed experimental and theoretical studies show that the interstitial hydrogen leads to enhanced orbital hybridization and reduced electron density around Pd. This optimized ligand effect weakens the carbon monoxide adsorption and increases the direct pathway preference of PdBH, resulting in its outstanding catalytic activity for the FAOR. The development of this high‐performance hydrogen‐doped PdB catalyst is an important step toward the construction of advanced light element co‐doped metal catalysts.
Rationally Improved Surface Charge Density of Triboelectric Nanogenerator with TiO2‐MXene/Polystyrene Nanofiber Charge Trapping Layer for Biomechanical Sensing and Wound Healing Application
Authors: Venkatesan Manikandan , Chandrasekar Jayashree , Hsu Yung‐Chi , Sun Ting‐Wang , Li Po‐Yu , King Xuan‐Ting , Chung Ming‐An , Chung Ren‐Jei , Lee Wen‐Ya , Zhou Ye , Lin Ja‐Hon , Kuo Chi‐Ching 
Published: July 2024

AbstractTriboelectric nanogenerators (TENGs) have become reliable green energy harvesters by converting biomechanical motions into electricity. However, the inevitable charge leakage and poor electric field (EF) of conventional TENG result in inferior tribo‐charge density on the active layer. In this paper, TiO2‐MXene incorporated polystyrene (PS) nanofiber membrane (PTMx NFM) charge trapping interlayer is introduced into single electrode mode TENG (S‐TENG) to prevent electron loss at the electrode interface. Surprisingly, this charge‐trapping mechanism augments the surface charge density and electric output performance of TENGs. Polyvinylidene difluoride (PVDF) mixed polyurethane (PU) NFM is used as tribo‐active layer, which improves the crystallinity and mechanical property of PVDF to prevent delamination during long cycle tests. Herein, the effect of this double‐layer capacitive model is explained experimentally and theoretically. With optimization of the PTMx interlayer thickness, S‐TENG exhibits a maximum open‐circuit voltage of (280 V), short‐circuit current of (20 µA) transfer charge of (120 nC), and power density of (25.2 µW cm−2). Then, this energy is utilized to charge electrical appliances. In addition, the influence of AC/DC EF simulation in wound healing management (vitro L929 cell migration, vivo tissue regeneration) is also investigated by changing the polarity of trans‐epithelial potential (TEP) distribution in the wounded area.
Selective CO2 Photoreduction into CH4 Triggered by the Synergy between Oxygen Vacancy and Ru Substitution under Near‐Infrared Light Irradiation
Authors: Li Jun , Liu Xinglong , Wu Xi , Liu Zhongyi , Zhao Zaiwang , Liu Yifeng , Dou Shixue , Xiao Yao 
Published: July 2024

AbstractNear‐infrared (NIR) light powdered CO2 photoreduction reaction is generally restricted to the separation efficiency of photogenerated carriers and the supply of active hydrogen (*H). Herein, the study reports a retrofitting hydrogenated MoO3‐x (H‐MoO3‐x) nanosheet photocatalysts with Ru single atom substitution (Ru@H‐MoO3‐x) fabricated by one‐step solvothermal method. Experiments together with theoretical calculations demonstrate that the synergistic effect of Ru substitution and oxygen vacancy can not only inhibit the recombination of photogenerated carriers, but also facilitate the CO2 adsorption/activation as well as the supply of *H. Compared with H‐MoO3‐x, the Ru@H‐MoO3‐x exhibit more favorable formation of *CHO in the process of *CO conversion due to the fast *H generation on electron‐rich Ru sites and transfer to *CO intermediates, leading to the preferential photoreduction of CO2 to CH4 with high selectivity. The optimized Ru@H‐MoO3‐x exhibits a superior CO2 photoreduction activity with CH4 evolution rate of 111.6 and 39.0 µmol gcatalyst−1 under full spectrum and NIR light irradiation, respectively, which is 8.8 and 15.0 times much higher than that of H‐MoO3‐x. This work provides an in‐depth understanding at the atomic level on the design of NIR responsive photocatalyst for achieving the goal of carbon neutrality.
Solar‐Driven Photoelectrochemical Upcycling of Polyimide Plastic Waste with Safe Green Hydrogen Generation
Authors: Zhao Hu , Zhao Xin , Zhang Jiajia , Anandita Shafira , Liu Wen , Koh See Wee , Yu Shuyan , Li Congju , Chen Zhong , Xu Rong , Zou Zhigang , Tu Wenguang , Li Hong 
Published: July 2024

AbstractArbitrary disposal of plastic waste into landfills and oceans can disturb the ecological system and even challenge human survival. Centralized plastic recycling process only works for selected types of plastics (e.g., polyethylene) with limited contribution (<10%), because of high infrastructure requirement. Comparatively, photoreforming of plastic waste for commodity and fuels production is much more facile and decentralizable, and thus holds great potential to mitigate the plastic waste challenge. To this end, a fully solar powered photoelectrochemical system is developed to selectively upgrade polyimide waste (often appears in electronic waste) into valuable commodity chemicals, including succinic acid, acetic acid, and formic acid, and cogenerating green hydrogen fuels. It is also demonstrated that one of the key monomer, pyromellitic acid, and the precious metals (in electronic waste) can be fully recycled. This proof‐of‐concept demonstration provides a new viewpoint for designing decentralized photoelectrochemical system for simultaneous plastic waste upcycling and renewable fuel synthesis, critical for a sustainable plastic economy. Selective cleavage of benzene ring also opens a green route for other benzene ring‐containing waste upgrading.
The careful selection of zwitterionic nanoparticle coating results in rapid and efficient cell labeling for imaging‐based cell tracking
Authors: Calvert Nicholas D. , Yu Luciana , Sehl Olivia C. , Gevaert Julia J. , Knier Natasha N. , Rivera‐Rodriguez Angelie , Goulet Clara S. , Fernando Nitara , Flood Samantha , Rinaldi‐Ramos Carlos M. , Foster Paula J. , Shuhendler Adam J. 
Published: July 2024

AbstractThe increased clinical application of cell‐based therapies has resulted in a parallel increase in the need for non‐invasive imaging‐based approaches for cell tracking, often through labeling with nanoparticles. An ideal nanoparticle for such applications must be biologically compatible as well as readily internalized by cells to ensure adequate and stable cell loading. Surface coatings have been used to make nanoparticle trackers suitable for these purposes, but those currently employed tend to have cytotoxic effects. Zwitterionic ligands are known to be biocompatible and antifouling; however, head‐to‐head evaluation of specific zwitterionic ligands for cell loading has not yet been explored. Magnetic particle imaging (MPI) detects superparamagnetic iron oxide nanoparticles (SPIONs) using time‐varying magnetic fields. Because MPI can produce high‐contrast, real‐time images with no tissue depth limitation, it is an ideal candidate for in vivo cell tracking. In this work, we have conjugated hard (permanently charged) and soft (pKa‐dependently charged) biomimetic zwitterionic ligands to SPIONs and characterized how these ligands changed SPION physicochemical properties. We have evaluated cellular uptake and subcellular localization between zwitterions, how the improvement in cell uptake generated stronger MPI signal for smaller numbers of cells, and how these cells can be tracked in an animal model with greater sensitivity for longer periods of time. Our best‐performing surface coating afforded high cell loading within 4 h, with full signal retention in vivo over 7 days.
What is known about cardiovascular diseases among seafarers: A systematic scoping review and quality assessment
Authors: Dohrmann Solveig Boeggild , Heiberg Regina Fromsejer , Krenzen Line Wang , Petersen Sofie Ronja , Adams Jordan Thomas , Skov Jane 
Published: July 2024

AbstractBackgroundSeafarers are at an increased risk of developing cardiovascular diseases (CVDs), potentially due to a stressful working environment and behavioral risk factors. To develop better prevention strategies, it is important to elucidate the extent of this risk. Therefore, we conducted a systematic literature review on CVD in seafarers.MethodWe conducted systematic searches in five databases. All studies investigating CVDs among occupational seafarers, published in articles or conference papers, were eligible for inclusion. The identified records were screened and reviewed by two independent researchers, who also evaluated the methodological quality of the included studies.ResultsThree thousand nine hundred and seventeen records qualified for screening, and 55 were eligible for inclusion. Most of the studies were observational, including cohort, frequency, incidence or prevalence studies, and review of case records. Around half were assessed at risk of biased findings. Participants in the studies were primarily from North America or the European continent and work onboard transportation vessels. Many studies investigated CVDs as a cause of death, focusing on conditions such as CVD, ischemic heart disease, and myocardial infarction. Frequency of CVD conditions varied but indicate that seafarers face a greater risk compared to the reference populations or control groups. Environmental factors were mainly investigated as risk factors.ConclusionOur results indicate a higher risk of CVDs among seafarers compared to reference or control groups. However, due to the variable quality of the evidence, well‐designed studies are needed to establish the causes of cardiovascular mortality and morbidity in seafarers and to investigate behavioral aspects of cardiovascular risk.
Intramolecular Electrostatic Interactions Regulate Reactivity of Zwitterionic Functionalities in Amphiphilic Assemblies
Authors: Das Ritam , Dutta Ranit , Yi Jun , Qiu Jingyi , Krishna Jithu , Tzafriri Gideon , Lin Zhou , Thayumanavan S. 
Published: July 2024

AbstractThe consequences of intramolecular ionic interactions in determining the reactivity of functional groups are of interest because they provide insights into how nature deploys seemingly reactive functionalities to be rather ubiquitous. Of specific interest are the quaternary ammonium ions in lipids. In this work, we investigate the effect of intramolecular electrostatic interactions in zwitterionic functionalities by judiciously incorporating them as leaving groups at the α‐position of α,β‐unsaturated ester‐based lipid head groups. We find that electrostatic stabilization indeed plays a critical role in both the reaction kinetics with nucleophiles and the thermodynamics of lipid formation. We further leverage these findings to fabricate both triggerable assembly and disassembly of liposomal supramolecular assemblies in the presence of nucleophiles.
Revisiting the Electrochemical Impedance Spectroscopy of Porous Electrodes in Li‐ion Batteries by Employing Reference Electrode
Authors: Xu Lei , Xiao Ye , Yu Zhi‐Xian , Yang Yi , Yan Chong , Huang Jia‐Qi 
Published: July 2024

AbstractElectrochemical impedance spectroscopy (EIS), characterized by its non‐destructive and in situ nature, plays a crucial role in comprehending the thermodynamic and kinetic processes occurring within Li‐ion batteries. However, there is a lack of consistent and coherent physical interpretations for the EIS of porous electrodes. Therefore, it is imperative to conduct thorough investigations into the underlying physical mechanisms of EIS. Herein, by employing reference electrode in batteries, we revisit the associated physical interpretation of EIS at different frequencies. Combining different battery configurations, temperature‐dependent experiments, and elaborated distribution of relaxation time analysis, we find that the ion transport in porous electrode channels and pseudo‐capacitance behavior dominate the high‐frequency and mid‐frequency impedance arcs, respectively. This work offers a perspective for the physical interpretation of EIS and also sheds light on the understanding of EIS characteristics in other advanced energy storage systems.
Dissoziative Elektronenanlagerungsdynamik eines vielversprechenden Krebsmedikaments zeigt sein Potential als Radiosensitizer
Authors: Izadi Farhad , Luxford Thomas F. M. , Sedmidubská Barbora , Arthur‐Baidoo Eugene , Kočišek Jaroslav , Ončák Milan , Denifl Stephan 
Published: July 2024

Abstract2‐Bromo‐1‐(3,3‐dinitroazetidin‐1‐yl)ethan‐1‐on (RRx‐001) ist ein Chemotherapeutikum für sauerstoffarme Tumore und zeigte bereits Synergieeffekte in Kombination mit Strahlentherapie. Die Wechselwirkung des Moleküls mit niederenergetischen Sekundärelektronen, die in großer Zahl in der physikalisch‐chemischen Phase der Bestrahlung gebildet werden, könnten für diesen Synergieeffekt verantwortlich sein. Die vorliegende Studie konzentriert sich auf die ersten Schritte in der Wechselwirkung von RRx‐001 mit niederenergetischen Elektronen, in denen das temporäre negative Ion gebildet wird und rasch fragmentiert. Die Kombination von Resultaten zweier Versuchsaufbauten erlaubt es uns, den Zerfall des RRx‐001 Anions auf verschiedenen Zeitskalen zu entflechten. Die alleinige Anwesenheit des eingefangenen Elektrons führt zu einer raschen Abspaltung von NO2 und HNO2, während NO2− und Br− Anionen direkt beziehungsweise über andere Zwischenprodukte gebildet werden. Auf Basis quantenchemischer Rechnungen schlagen wir einen bidirektionalen Wechsel zwischen π*(NO2) und σ*(C−Br) Zuständen vor, welcher die experimentellen Spektren erklärt. Die beobachtete schnelle Dynamik lässt auch Schlussfolgerungen für die Chemie des Anions in der kondensierten Phase zu.
Polyacrylate epoxide oligomers with robust photo‐crosslinked and thermomechanical properties enabled by controlling copolymerizing molecular weight distribution
Authors: Lian Keyu , Yang Shengdu , Tang Wei , Zhang Junhua 
Published: July 2024

AbstractPhoto‐triggering curing coatings have advantages of improving production efficiency, reducing pollution emissions, and contributing to green environmental protection. However, making the trade‐off between appropriate viscosity and UV‐curing properties in a high‐performing polymer system remains a formidable challenge. In this paper, firstly, a series of acrylate copolymer oligomers (named as PAAR) were synthesized using methyl methacrylate (MMA), butyl acrylate (BA), and glycidyl methacrylate (GMA), then methacrylic acid (MAA) was grafted utilizing the reaction between carboxyl group in MAA with epoxy group in oligomer to introduce double bonds. By adjusting the oligomer molecular weight to control the viscosity and changing the GMA ratio to obtain suitable double bonds content. As a result, the number molecular weight (Mn) of the thus‐obtained PAAR oligomers were less than 3000 Da, and the polymer dispersity indexes (PDI) were lower than 1.8. Photo‐polymerization kinetics revealed that the coating prepared using the oligomers could be fully cross‐linked by UV light triggering within 60 s, achieving a high transparency of 90% along with favorable thermal and mechanical properties. Furthermore, it was confirmed that the water resistance on the surface of the cured films and hydrophobicity were more influenced by the presence of hydroxyl groups.
Fine and combinatorial regulation of key metabolic pathway for enhanced β‐alanine biosynthesis with non‐inducible Escherichia coli
Authors: Zhou Hai‐Yan , Ding Wen‐Qing , Zhang Xi , Zhang Hong‐Yu , Hu Zhong‐Ce , Liu Zhi‐Qiang , Zheng Yu‐Guo 
Published: July 2024

Abstractβ‐Alanine is the only β‐amino acid in nature and one of the most important three‐carbon chemicals. This work was aimed to construct a non‐inducible β‐alanine producer with enhanced metabolic flux towards β‐alanine biosynthesis in Escherichia coli. First of all, the assembled E. coli endogenous promoters and 5′‐untranslated regions (PUTR) were screened to finely regulate the combinatorial expression of genes panDBS and aspBCG for an optimal flux match between two key pathways. Subsequently, additional copies of key genes (panDBSK104S and ppc) were chromosomally introduced into the host A1. On these bases, dynamical regulation of the gene thrA was performed to reduce the carbon flux directed in the competitive pathway. Finally, the β‐alanine titer reached 10.25 g/L by strain A14‐R15, 361.7% higher than that of the original strain. Under fed‐batch fermentation in a 5‐L fermentor, a titer of 57.13 g/L β‐alanine was achieved at 80 h. This is the highest titer of β‐alanine production ever reported using non‐inducible engineered E. coli. This metabolic modification strategy for optimal carbon flux distribution developed in this work could also be used for the production of various metabolic products.
Trametinib restores the central conducting lymphatic flow in a premature infant with Noonan syndrome
Authors: Leenders Erika K. S. M. , Kleimeier Lotte E. R. , Weeke Lauren C. , Coppens Catelijne H. , Klein Willemijn M. , Draaisma Jos M.T. 
Published: July 2024

Key Clinical MessageWe describe a premature hydropic infant with Noonan syndrome and a therapy refractory chylothorax. This was shown to be due to a central conducting lymphatic anomaly. After therapy with a MEK‐inhibitor the infant recovered clinically and radiologically completely, possibly by restoring lymphatic valve function.
A Heterogeneous Acid‐Base Organocatalyst For Cascade Deacetalisation‐Knoevenagel Condensations
Authors: Chhetri Ashis , Maibam Ashakiran , Maniam Subashani , Babarao Ravichandar , Wilson Karen , Lee Adam F. , Mitra Joyee 
Published: July 2024

AbstractMultifunctional heterogeneous catalysts are an effective strategy to drive chemical cascades, with attendant time, resource and cost efficiencies by eliminating unit operations arising in normal multistep processes. Despite advances in the design of such catalysts, the fabrication of proximate, chemically antagonistic active sites remains a challenge for inorganic materials science. Hydrogen‐bonded organocatalysts offer new opportunities for the molecular level design of multifunctional structures capable of stabilising antagonistic active sites. We report the catalytic application of a charge‐assisted, hydrogen‐bonded crystalline material, bis(melaminium)adipate (BMA), synthesised from melamine and adipic acid, which possesses proximate acid‐base sites. BMA exhibits high activity for the cascade deacetalisation‐Knoevenagel condensation of dimethyl acetals to form benzylidenemalononitriles under mild conditions in water; BMA is amenable to large‐scale manufacture and recycling with minimal deactivation. Computational modelling of the melaminium cation in protonated BMA explains the observed catalytic reactivity, and identifies the first demethoxylation step as rate‐limiting, which is in good agreement with time‐dependent 1H NMR and kinetic experiments. A broad substrate scope for the cascade transformation of aromatic dimethyl acetals is demonstrated.
Deep learning for predicting rehospitalization in acute heart failure: Model foundation and external validation
Authors: Kim Mi‐Na , Lee Yong Seok , Park Youngmin , Jung Ayoung , So Hanjee , Park Joonwoong , Park Jin‐Joo , Choi Dong‐Joo , Kim So‐Ree , Park Seong‐Mi 
Published: July 2024

AbstractAimsAssessing the risk for HF rehospitalization is important for managing and treating patients with HF. To address this need, various risk prediction models have been developed. However, none of them used deep learning methods with real‐world data. This study aimed to develop a deep learning‐based prediction model for HF rehospitalization within 30, 90, and 365 days after acute HF (AHF) discharge.Methods and resultsWe analysed the data of patients admitted due to AHF between January 2014 and January 2019 in a tertiary hospital. In performing deep learning‐based predictive algorithms for HF rehospitalization, we use hyperbolic tangent activation layers followed by recurrent layers with gated recurrent units. To assess the readmission prediction, we used the AUC, precision, recall, specificity, and F1 measure. We applied the Shapley value to identify which features contributed to HF readmission. Twenty‐two prognostic features exhibiting statistically significant associations with HF rehospitalization were identified, consisting of 6 time‐independent and 16 time‐dependent features. The AUC value shows moderate discrimination for predicting readmission within 30, 90, and 365 days of follow‐up (FU) (AUC:0.63, 0.74, and 0.76, respectively). The features during the FU have a relatively higher contribution to HF rehospitalization than features from other time points.ConclusionsOur deep learning‐based model using real‐world data could provide valid predictions of HF rehospitalization in 1 year follow‐up. It can be easily utilized to guide appropriate interventions or care strategies for patients with HF. The closed monitoring and blood test in daily clinics are important for assessing the risk of HF rehospitalization.