bluuebunny/crossref_metadata_2025_split huggingface dataset:
Hydrocarbon‐Based Ionomer/PTFE‐Reinforced Composite Membrane Through Multibar Coating Technique for Durable Fuel Cells
Authors: Lee Sanghyeok , Sul Taejun , Kim Unsoo , Kim Sohee , Chae Ji Eon , Kim Junsoo , Kim Sang Moon , Jang Segeun 
Published: September 2024

AbstractFor cost reduction and environmental‐friendly manufacturing, it is highly demanded to replace the current perfluorinated sulfonic acid‐based membrane in polymer electrolyte membrane fuel cells (PEMFCs) with inexpensive and readily available hydrocarbon‐based (HC) membranes. However, HC membranes suffer from profound dimensional changes caused by swelling and shrinking during operation, especially in automotive applications. These changes lead to severe mechanical degradation and shorten the service life of PEMFC. Herein, a multibar coating system is developed to manufacture HC/polytetrafluoroethylene (PTFE) composite membrane. This system facilitates capillary‐rise infiltration with the aid of an optimal amount of residual alcohol solvent on the PTFE. To address compatibility issues between PTFE and HC‐ionomer solutions, the effects of residual alcohol solvent on tuning the PTFE surface are investigated by controlling systemic parameters and performing diverse mechanical, optical, and electrochemical measurements. Based on its enhanced mechanical toughness (≈30.04%) and superior impregnation properties, the constructed HC/PTFE composite membrane exhibited more than seven‐fold improvement in mechanical durability under repeated accelerated wet–dry conditions compared with an unsupported pristine HC membrane while also mitigating performance loss (≈5.84%).
Synthesis of Aza‐S(VI) Fluorides and Primary Sulfonimidamides from Sulfinylamines
Authors: Andresini Michael , Marraffa Laura , Şerbetçi Defne , Natho Philipp , Colella Marco , Degennaro Leonardo , Luisi Renzo 
Published: September 2024

AbstractAza‐S(VI) fluorides are crucial compounds in the synthesis of various S(VI) derivatives, which find broad applications in drug discovery. However, the synthesis of sulfonimidoyl and sulfondiimidoyl fluorides have been relatively underexplored, often requiring lengthy reaction sequences and/or the use of hazardous gaseous reagents. In this study, we present a rapid one‐pot method for producing sulfonimidoyl fluorides from sulfinylamines via a nucleophilic addition/electrophilic fluorination sequence. Similarly, sulfondiimidoyl fluorides can be synthesized using the same sequence, preceded by the formation of unsymmetrical sulfurdiimides readily generated in situ from sulfinylamines. Whereas isolation of sulfondiimidoyl fluorides was not feasible, they could be efficiently converted into primary sulfonimidamides by base hydrolysis in a one‐pot process. Furthermore, we explored the reactivity of aza‐S(VI) fluorides with various nucleophiles, demonstrating a versatile synthetic platform for the synthesis of aza‐S(VI) compounds.
Integrated Ultrasound‐Enrichment and Machine Learning in Colorimetric Lateral Flow Assay for Accurate and Sensitive Clinical Alzheimer's Biomarker Diagnosis
Authors: Wang Shuqing , Zhu Yan , Zhou Zhongzeng , Luo Yong , Huang Yan , Liu Yibiao , Xu Tailin 
Published: September 2024

AbstractThe colloidal gold nanoparticle (AuNP)‐based colorimetric lateral flow assay (LFA) is one of the most promising analytical tools for point‐of‐care disease diagnosis. However, the low sensitivity and insufficient accuracy still limit its clinical application. In this work, a machine learning (ML)‐optimized colorimetric LFA with ultrasound enrichment is developed to achieve the sensitive and accurate detection of tau proteins for early screening of Alzheimer's disease (AD). The LFA device is integrated with a portable ultrasonic actuator to rapidly enrich microparticles using ultrasound, which is essential for sample pre‐enrichment to improve the sensitivity, followed by ML algorithms to classify and predict the enhanced colorimetric signals. The results of the undiluted serum sample testing show that the protocol enables efficient classification and accurate quantification of the AD biomarker tau protein concentration with an average classification accuracy of 98.11% and an average prediction accuracy of 99.99%, achieving a limit of detection (LOD) as sensitive as 10.30 pg mL−1. Further point‐of‐care testing (POCT) of human plasma samples demonstrates the potential use of LFA in clinical trials. Such a reliable lateral flow immunosensor with high precision and superb sensing performance is expected to put LFA in perspective as an AD clinical diagnostic platform.
Functional Zwitterionic Polyurethanes as Gate Dielectrics for Organic Field‐Effect Transistors
Authors: Sun Qian , Hu Jinkang , Chen Chi , Wan Xiaobo , Mu Youbing 
Published: September 2024

AbstractThe development of polymeric dielectrics with a high dielectric constant is of great significance for flexible low‐voltage organic field‐effect transistors (OFETs). Herein, functional polyurethanes (PUs) with nitro and sulfobetaine zwitterionic groups are synthesized, and their electrical properties, mechanical properties, and the performances of OFET devices using these zwitterionic PUs as gate dielectrics are studied. Compared with sulfobetaine zwitterion‐containing PUs, nitro‐containing PUs (NO2‐PUs) show higher dielectric constant up to 6.5. Both zwitterionic PUs enhance the OFET performances, while the effect of NO2‐PU is more significant. Devices using NO2‐PU‐15 that contains 15 moL% nitro groups as the dielectric layer show the best performance and a threshold voltage (Vth) of as low as −0.02 V together with two orders’ increase of the mobility is observed, compared with the devices using PU without nitro groups. This study provides a new method to improve the dielectric constant of polymeric dielectrics, which is valuable for flexible/stretchable and wearable electronic devices.
A machine learning‐based exploration of resilience and food security
Authors: Villacis Alexis H. , Badruddoza Syed , Mishra Ashok K. 
Published: September 2024

AbstractLeveraging advancements in remote data collection and using the Food Insecurity Experience Scale (FIES) as a proxy measure of resilience, we show that machine learning models (such as Gradient Boosting Classifier, eXtreme Gradient Boosting, and Artificial Neural Networks), can predict resilience with relatively high accuracy (up to 81%). Key household‐level predictors include access to financial institutions, asset ownership, the adoption of agricultural mechanization as evidenced by the use of tractors, the number of crops cultivated, and ownership of nonfarm enterprises. Our analysis offers insights to researchers and policymakers interested in the development of targeted interventions to bolster household resilience.
Sulfonated Hydroxyaryl‐Tetrazines with Increased pKa for Accelerated Bioorthogonal Click‐to‐Release Reactions in Cells
Authors: Rahm Michal , Keppel Patrick , Šlachtová Veronika , Dzijak Rastislav , Dračínský Martin , Bellová Simona , Reyes‐Gutiérrez Paul E. , Štěpánová Sille , Raffler Jakob , Tloušťová Eva , Mertlíková‐Kaiserová Helena , Mikula Hannes , Vrabel Milan 
Published: September 2024

AbstractBioorthogonal reactions that enable switching molecular functions by breaking chemical bonds have gained prominence, with the tetrazine‐mediated cleavage of trans‐cyclooctene caged compounds (click‐to‐release) being particularly noteworthy for its high versatility, biocompatibility, and fast reaction rates. Despite several recent advances, the development of highly reactive tetrazines enabling quantitative elimination from trans‐cyclooctene linkers remains challenging. In this study, we present the synthesis and application of sulfo‐tetrazines, a class of derivatives featuring phenolic hydroxyl groups with increased acidity constants (pKa). This unique property leads to accelerated elimination and complete release of the caged molecules within minutes. Moreover, the inclusion of sulfonate groups provides a valuable synthetic handle, enabling further derivatization into sulfonamides, modified with diverse substituents. Significantly, we demonstrate the utility of sulfo‐tetrazines in efficiently activating fluorogenic compounds and prodrugs in living cells, offering exciting prospects for their application in bioorthogonal chemistry.
Magnetic Excitations in Ferromagnetically Coupled Spin‐1 Nanographenes
Authors: Turco Elia , Wu Fupeng , Catarina Gonçalo , Krane Nils , Ma Ji , Fasel Roman , Feng Xinliang , Ruffieux Pascal 
Published: September 2024

AbstractIn the pursuit of high‐spin building blocks for the formation of covalently bonded 1D or 2D materials with controlled magnetic interactions,
‐electron magnetism offers an ideal framework to engineer ferromagnetic interactions between nanographenes. As a first step in this direction, we explore the spin properties of ferromagnetically coupled triangulenes—triangular nanographenes with spin
. By combining in‐solution synthesis of rationally designed molecular precursors with on‐surface synthesis, we successfully achieve covalently bonded
triangulene dimers and
trimers on Au(111). Starting with the triangulene dimer, we meticulously characterize its low‐energy magnetic excitations using inelastic electron tunneling spectroscopy (IETS). IETS reveals conductance steps corresponding to a quintet‐to‐triplet excitation, and a zero‐bias peak resulting from higher‐order spin‐spin scattering of the five‐fold degenerate ferromagnetic ground state. The Heisenberg model captures the key parameters of inter‐triangulene ferromagnetic exchange, and its successful extension to the larger
system validates the model's accuracy. We anticipate that incorporating ferromagnetically coupled building blocks into the repertoire of magnetic nanographenes will unlock new possibilities for designing carbon nanomaterials with complex magnetic ground states.
Stepwise One‐Shot Borylation Reactions for Intersecting DABNA Substructures Exhibiting Bright Yellow‐Green Electroluminescence with EQE Beyond 40 % and Mild Roll‐Off
Authors: Xiong Xin , Chen Ting‐Feng , Walia Rajat , Fan Xiao‐Chun , Cheng Ying‐Chun , Wang Hui , Wu Hao , Chen Xian‐Kai , Yu Jia , Wang Kai , Zhang Xiao‐Hong 
Published: September 2024

AbstractBoron/nitrogen (B/N)‐doped polycyclic aromatic hydrocarbons (PAHs) with the multiple resonance (MR) effect are promising for organic light‐emitting diodes (OLEDs) because of their narrowband emission and thermally activated delayed fluorescence (TADF) characteristics. Nevertheless, exploring the variety of such emitters is challenging because of the tricky and limited synthetic protocols. Herein, we designed a novel B/N‐doped PAH, L–DABNA‐1, whose backbone (L–DABNA) could not be achieved via conventional routes (e.g., one‐pot borylation or one‐shot borylation). We successfully synthesized it through stepwise one‐shot borylations with precisely introducing decorations. The unique MR backbone with intersecting DABNA substructures sharing an aniline group, avoiding any para‐N‐π‐B motif, allows L–DABNA‐1 to maintain narrowband TADF emission while significantly redshifting to the yellow‐green region with a reverse intersystem crossing rate (kRISC) of 1.28×105 s−1. An L–DABNA‐1‐based OLED device achieved a maximum external quantum efficiency (EQE) of over 40 % and maintained a high EQE of 36.3 % at 1000 cd m−2, with a current efficiency reaching ~170 cd A−1. This work not only demonstrated the great potential of stepwise borylations in synthesizing B/N‐doped PAH backbones, expanding their chemical space, but also provided a promising pathway for exploring MR‐TADF emitters at longer wavelengths.
Luminescent Terbium Probe for Time‐Resolved FRET and NSET Binding Assays with Quantum Dots and Gold Nanoparticles
Authors: Iyanu Diriwari P. , Connor Payne N. , Mazitschek Ralph , Gallavardin Thibault , Hildebrandt Niko 
Published: September 2024

AbstractTime‐gated or time‐resolved FRET (TR‐FRET) assays are important tools in biosensing, bioimaging, drug screening, and molecular diagnostics. Efficient TR‐FRET assays require stable lanthanide complexes with high absorption cross sections, high quantum yields, and long photoluminescence lifetimes. Owing to their challenging synthesis, such complexes are relatively rare and new components are of potential interest when developing TR‐FRET probes. Here, we evaluate the recently developed Tb complex CoraFluor‐1 concerning its analytical performance in terbium‐to‐quantum dot FRET and terbium‐to‐gold nanoparticle NSET assays using the prototypical biological recognition system of streptavidin and biotin. Biological binding was quantifiable at sub‐picomolar concentrations in small sample volumes, with broad applicability demonstrated across three commercial fluorescence plate readers used for time‐resolved, spectrally‐resolved, and clinical bioanalysis. Overall, CoraFluor‐1 provided excellent analytical performance as both FRET and NSET donor, validating its potential for developing new TR‐FRET probes for biosensing and bioimaging.
A high‐temperature resistant benzimidazole‐based porous polymer for efficient adsorption of trinitrotoluene in aqueous solution
Authors: Yang Chunyan , Mo Shijie , Chen Xirui , Yuan Qianqian , Zhu Jiali , Wang Ting , Zheng Min , Zhou Mingru , Chang Guanjun , Xu Yewei 
Published: September 2024

AbstractA novel benzimidazole‐based porous polymer, denoted as PTBI, was synthesized utilizing self‐synthesized 1,3,5‐tris(1H‐benzo[d]imidazol‐2‐yl)benzene (TBI) and 4,4′‐difluorobenzophenone as primary materials via a CN coupling reaction, followed by a freeze‐drying process. PTBI displayed commendable thermal stability, as evidenced by a temperature of 475°C at which a 5% weight loss occurred and a char yield of up to 65% at 800°C. Trinitrotoluene (TNT) was effectively adsorbed by PTBI in aqueous solutions, thanks to the combined effects of three π–π interactions and one dipole–π interaction. At 25°C, PTBI achieved a maximum adsorption capacity as high as 280.8 mg/g, with approximately 60% of this capacity attained within just 1 h. Furthermore, a thermodynamic analysis showed that the adsorption of TNT by PTBI was a spontaneous, exothermic process that was followed by a decrease in entropy. It is noteworthy that following five adsorption and desorption cycles, the adsorption efficiency held steady at a relatively high level using acetone as the eluent. These promising results underscore PTBI's significant potential in the realm of TNT wastewater treatment, positioning it as a compelling candidate for further research and application under extreme condition in this field.
Preparation and study on electrical/thermal properties of epoxy/polyacrylate rubber composite dielectric
Authors: Zhang Wenchao , Wen Ming , Chen Qingguo , Yue Dong , Feng Yu 
Published: September 2024

AbstractWith the development of power systems and electronic devices, epoxy resin (EP) is facing increasingly severe operating environments, and its performance may not meet expectations. In order to broaden the application of EP, the DE/EP composite films were prepared with EP as matrix, polyacrylic rubber dielectric elastomer (DE) as reinforcement materials. The structure of DE/EP composite films was characterized by XRD, SEM, and other methods, and the electrical and thermal properties of the materials were tested and studied. The study found that with appropriate dissolution and stirring treatment, DE can be evenly dispersed in the EP matrix, and the introduction of DE does not significantly affect the structure of the EP molecular chain, also found the introduction of DE improve the electrical and thermal properties of EP. The breakdown strength of the 4% DE/EP composite film surpasses that of the pure EP film by 15.58%. Additionally, the thermal conductivity of the 8% DE/EP composite film is elevated by 41.6% compared to the pure EP film, while its dielectric constant is also enhanced by 8.2%. This work may provide a theoretical basis for studying the application of EP modified system in electrical engineering, integrated circuit packaging and other fields.
Dorsal venous complex ligation‐free and parietal endopelvic fascia preserving in laparoscopic radical prostatectomy: A prospective study of single centre
Authors: Yang Zhong‐Hua , Wang Yong‐Zhi , Liu Tao , Zheng Hang , Wang Xing‐Huan 
Published: September 2024

AbstractObjectivesThis study aims to describe a novel dorsal venous complex (DVC) ligation‐free and parietal endopelvic fascia preserving technique for laparoscopic radical prostatectomy and to evaluate its post‐operative outcomes.MethodsFrom April 2020 to May 2021, a total of 125 patients with localized prostate cancer received laparoscopic radical prostatectomy by a single surgeon. In the procedure, a novel technique of DVC ligation‐free and parietal endopelvic fascia preserving was used. Preoperative characteristics of patients and perioperative results were recorded. In this study, continence was defined as zero to one pad per day. Oncological outcomes were evaluated based on positive surgical margin.ResultsFive patients required a blood transfusion. Mean post‐operative hospital stay was 3.9 days (2–5), and the catheter could be removed on post‐operative day 7 to 9. Final pathologic evaluations were 87 stage pT2, 22 stage pT3a, and 7 pT3b, 9 stage pT4, respectively. The positive surgical margin rate was 10.4% in total. Ninety‐three patients (74.4%) returned to urinary continence 2 months post‐operatively, and 11 patients (11/125) developed biochemical recurrence 6 months post‐operatively.ConclusionsThe DVC ligation‐free and parietal endopelvic fascia preserving technique provides early recovery from incontinence without adversely affecting the oncological outcome.
Overexpression of SLC2A1, ALDOC, and PFKFB4 in the glycolysis pathway drives strong drug resistance in 3D HeLa tumor cell spheroids
Authors: Wang Tong , Wang Xueting , Zheng Xuli , Guo Zhongfang , Mohsin Ali , Zhuang Yingping , Wang Guan 
Published: September 2024

AbstractThe 3D multicellular tumor spheroid (MTS) model exhibits enhanced fidelity in replicating the tumor microenvironment and demonstrates exceptional resistance to clinical drugs compared to the 2D monolayer model. In this study, we used multiomics (transcriptome, proteomics, and metabolomics) tools to explore the molecular mechanisms and metabolic differences of the two culture models. Analysis of Gene Ontology (GO) and Kyoto Encyclopedia of Genes and Genomes (KEGG) enrichment pathways revealed that the differentially expressed genes between the two culture models were mainly enriched in cellular components and biological processes associated with extracellular matrix, extracellular structural organization, and mitochondrial function. An integrated analysis of three omics data revealed 11 possible drug resistance targets. Among these targets, seven genes, AKR1B1, ALDOC, GFPT2, GYS1, LAMB2, PFKFB4, and SLC2A1, exhibited significant upregulation. Conversely, four genes, COA7, DLD, IFNGR1, and QRSL1, were significantly downregulated. Clinical prognostic analysis using the TCGA survival database indicated that high‐expression groups of SLC2A1, ALDOC, and PFKFB4 exhibited a significant negative correlation with patient survival. We further validated their involvement in chemotherapy drug resistance, indicating their potential significance in improving prognosis and chemotherapy outcomes. These results provide valuable insights into potential therapeutic targets that can potentially enhance treatment efficacy and patient outcomes.
Enhancing the expression of terminal deoxynucleotidyl transferases by N‐terminal truncation
Authors: Li An‐Na , Shi Kun , Zeng Bu‐Bing , Xu Jian‐He , Yu Hui‐Lei 
Published: September 2024

AbstractTerminal deoxynucleotidyl transferase (TdT), a unique DNA polymerase that catalyzes the template‐free incorporation of nucleotides into single‐stranded DNA, has facilitated the development of various oligonucleotide‐based tools and methods, especially in the field of template‐free enzymatic DNA synthesis. However, expressing vertebrate‐derived TdTs in Escherichia coli complicates purification and increases production costs. In this study, N‐terminal truncation of TdTs was performed to improve their expression and stability. The results revealed that N‐terminal truncation could enhance the expression level of six TdTs. Among the truncated mutants, N‐140‐ZaTdT and N‐140‐CpTdT, with 140 amino acids removed, exhibited an increase in protein expression, which was 9.5‐ and 23‐fold higher than their wild‐types, respectively. Importantly, the truncation preserves the catalytic function of TdT. Additionally, the Tm values of N‐140‐ZaTdT increased by 4.9°C. The improved expression of the truncated mutants makes them more suitable for reducing production costs and advancing enzyme engineering.
Physiological Metabolic Analysis of VB12 Accumulation in Ensifer adhaerens Casida A Enhanced by Oxygen Limitation
Authors: Li Bo , Chen Xinyi , Zhao Dujuan , Liu Zebo , Li Junming , Siddique Muhammad Safwan , Wu Jiequn , Zhuang Yingping , Wang Zejian 
Published: September 2024

ABSTRACTCobalamin (VB12) is in enormous demand across the fields of medicine, food, and feed additives. However, the oxygen supply plays a critical role in VB12 biosynthesis by Ensifer adhaerens Casida A and has been identified as a bottleneck for economical substrate consumption. This study elucidates the relationship between oxygen limitation and VB12 accumulation with transcriptomic and metabolomic analyses. Under oxygen limitation, E. adhaerens enhances oxygen transport and storage by increasing expression of flavin hemoglobin (Hmp), which was up‐regulated 6‐fold at 24 h of oxygen restriction compared to the oxygen restriction of 4 h (p < 0.01). Because of the cofactor of Hmp is heme, the demand for heme increases, leading to the upregulation of genes in the heme biosynthesis pathway. Similarly, genes involved in biosynthesis of its precursor, 5‐ALA, were upregulated as well. 5‐ALA is also a direct precursor of VB12, further leading to the upregulation of genes in the VB12 biosynthesis pathway. This process initiates biosynthesis and accumulation of VB12. As VB12 and heme biosynthesis progresses, genes associated with the biosynthesis and transportation pathways of compounds related to their biosynthesis were likewise upregulated, including genes involved in S‐adenosyl methionine (SAM) biosynthesis, and the transport of Fe2+ and Co2+. Additionally, amino acids and organic acids associated with biosynthesis were also extensively consumed, such as methionine, which is used for synthesizing SAM, decreased by 310% after 24 h of oxygen limitation compared to 20% dissolved oxygen (p < 0.05). At the same time, genes related to growth‐associated metabolic pathways, such as pentose phosphate pathway (PPP), were significantly downregulated. Therefore, the potential mechanism by which E. adhaerens accumulates VB12 under oxygen‐limited conditions by enhancing Hmp expression, which facilitates the porphyrin metabolic pathway and promotes VB12 biosynthesis. This research provides valuable insights for increasing VB12 production through metabolic engineering and process optimization.