bluuebunny/crossref_metadata_2025_split huggingface dataset:
Brønsted Acid‐Catalyzed Intramolecular 7‐endo Hydroarylation Reaction of 1,5‐Diaryl‐1‐pentynes
Authors: Makino Kosho , Sueki Shunsuke , Anada Masahiro 
Published: April 2023

AbstractA Brønsted acid‐catalyzed, transition metal‐free intramolecular 7‐endo hydroarylation reaction of 1,5‐diaryl‐1‐pentynes has been developed. The use of 1,1,1,3,3,3‐hexafluoro‐2‐propanol (HFIP) as a solvent was found to be critical for this process. Using the present methodology, we have accomplished the synthesis of KGP‐18, an analogue of the anticancer natural product combretastatin A4.magnified image
Ionic Flexible Mechanical Sensors: Mechanisms, Structural Engineering, Applications, and Challenges
Authors: Ren Ziqi , Liu Nishuang , Zhang Qixiang , Yin Jianyu , Jia Peixue , Lu Wenzhong , Yao Qianqian , Deng Mingfang , Gao Yihua 
Published: April 2023

AbstractThis review covers the evolution of flexible mechanical sensors from an “electronic” language to an “ionic” language, which provides key reference information for the development of next‐generation bio‐intelligent sensing devices. Unlike sensors that rely solely on electron modulation, the core feature of the ionic flexible mechanical sensor (IFMS) is the ability of mechanical deformation to induce ion transport and compensation, thus demonstrating their conceptual similarity to biomechanical strain systems. Here, the basic design principles of flexible mechanical sensors modulated by ion transport are highlighted. This review provides a detailed description of the mechanotransduction mechanisms of IFMS devices based on ion transport modulation. First, although with similar mechanisms to conventional flexible mechanical sensors via piezoresistive, piezoelectric, and triboelectric transduction mechanisms, the core driver for IFMS devices is ions (not electrons). In addition, the transduction models and principles of action of novel transduction mechanisms that have been explored in the last decade are described in detail, which include interfacial iontronic sensing and potentiometric and electrokinetic energy conversion. According to the characteristics of the device, the relevant structural engineering is further highlighted. A comprehensive review of important IFMS application approaches (human–machine interfaces, life and health applications) is presented. Importantly, future challenges and possible solutions for IFMS devices are presented based on the existing research.
Requirement of Cholesterol for Calcium‐Dependent Vesicle Fusion by Strengthening Synaptotagmin‐1‐Induced Membrane Bending
Authors: Ali Moussa Houda Yasmine , Shin Kyung Chul , Ponraj Janarthanan , Kim Soo Jin , Ryu Je‐Kyung , Mansour Said , Park Yongsoo 
Published: April 2023

AbstractCholesterol is essential for neuronal activity and function. Cholesterol depletion in the plasma membrane impairs synaptic transmission. However, the molecular mechanisms by which cholesterol deficiency leads to defects in vesicle fusion remain poorly understood. Here, it is shown that cholesterol is required for Ca2+‐dependent native vesicle fusion using the in vitro reconstitution of fusion and amperometry to monitor exocytosis in chromaffin cells. Purified native vesicles are crucial for the reconstitution of physiological Ca2+‐dependent fusion, because vesicle‐mimicking liposomes fail to reproduce the cholesterol effect. Intriguingly, cholesterol has no effect on the membrane binding of synaptotagmin‐1, a Ca2+ sensor for ultrafast fusion. Cholesterol strengthens local membrane deformation and bending induced by synaptotagmin‐1, thereby lowering the energy barrier for Ca2+‐dependent fusion to occur. The data provide evidence that cholesterol depletion abolishes Ca2+‐dependent vesicle fusion by disrupting synaptotagmin‐1‐induced membrane bending, and suggests that cholesterol is an essential lipid regulator for Ca2+‐dependent fusion.
Cryogenic Storage Memory with High‐Speed, Low‐Power, and Long‐Retention Performance
Authors: Hur Jae , Kang Dongsuk , Moon Dong‐Il , Yu Ji‐Man , Choi Yang‐Kyu , Yu Shimeng 
Published: April 2023

AbstractCryogenic‐computing draws attention due to its variety of applications such as cloud‐computing, aerospace electronics, and quantum computing. Low temperature (e.g., 77 K) enables higher switching speed, improved reliability, and suppressed noise. Although cryogenic dynamic random‐access memory is studied, the cryogenic NAND flash is not explored intensively. Herein, a cryogenic storage memory based on the charge‐trap mechanism is reported. By removing the tunneling oxide from the conventional silicon/oxide/nitride/oxide/silicon (SONOS)‐type flash memory (therefore becoming silicon/oxide/nitride/silicon (SONS)), high‐speed and low‐power operation is aimed to be achieved while relieved from poor retention issue thanks to the cryogenic environment. The FinFET‐structured SONS memory device is demonstrated experimentally with gate length of 20–30 nm, which can achieve the retention issue (>10 years) with low voltage (≈6.5 V) and high speed (≈5 µs) operation at 77 K. To have a holistic system‐level evaluation, benchmark simulation of an interface between a host microprocessor and solid‐state‐drive is conducted, considering the refrigerator cooling cost and the heat loss via cables across two temperatures (300 and 77 K). The results show that the SONS‐type cryogenic storage system shows over 81% improvement in both latency and power, compared to the SONOS counterpart located at cryogenics.
Epithelial innate immune response to Pseudomonas aeruginosa–derived flagellin in chronic rhinosinusitis
Authors: Li Ping , Sheng Quanhu , Huang Li‐Ching , Turner Justin H. 
Published: April 2023

AbstractBackgroundPseudomonas aeruginosa is a common colonizing pathogen in the upper respiratory tract and is associated with recalcitrant chronic rhinosinusitis (CRS). Herein we sought to characterize the effect of P. aeruginosa–derived flagellin on human sinonasal epithelial cell (HSNEC) immune responses and determine whether these pathways are disrupted in CRS.MethodsAir‐liquid interface cultures were established from CRS and healthy control donors. Cells were incubated with P. aeruginosa–derived flagellin for 24 hours and transcriptional changes were assessed using whole transcriptome RNA sequencing. Apical and basolateral secretion of the pro‐inflammatory cytokines in interleukin (IL)‐1β, tumor necrosis factor (TNF)‐α, and IL‐6 were measured after stimulation by lipopolysaccharide or flagellin and responses were compared between CRS and healthy control patients.ResultsHSNECs were weakly responsive to lipopolysaccharide, whereas flagellin stimulated a profound innate immune response dominated by TNF‐α, IL‐1β, and IL‐17 signaling and activation of the IL‐17C/IL‐23 axis. CRS‐derived HNSECs showed an altered innate immune response to flagellin, characterized by a profound increase in TNF‐α secretion coupled with reduced IL‐6 secretion.ConclusionsFlagellin activates a potent innate immune response in HSNECs characterized by pro‐inflammatory mediators and cytokines/chemokines associated with neutrophilic inflammation. HSNECs from CRS patients have a dysregulated innate immune response to flagellin characterized by an imbalance between IL‐6 and TNF‐α secretion.
Quantitative Point of Care Tests for Timely Diagnosis of Early‐Onset Preeclampsia with High Sensitivity and Specificity
Authors: Masoumeh Ghorbanpour Sahar , Wen Shihui , Kaitu'u‐Lino Tu'uhevaha J , Hannan Natalie J. , Jin Dayong , McClements Lana 
Published: April 2023

AbstractPreeclampsia is a heterogeneous and multiorgan cardiovascular disorder of pregnancy. Here, we report the development of a novel strip‐based lateral flow assay (LFA) using lanthanide‐doped upconversion nanoparticles conjugated to antibodies targeting two different biomarkers for detection of preeclampsia. We first measured circulating plasma FKBPL and CD44 protein concentrations from individuals with early‐onset preeclampsia (EOPE), using ELISA. We confirmed that the CD44/FKBPL ratio is reduced in EOPE with a good diagnostic potential. Using our rapid LFA prototypes, we achieved an improved lower limit of detection: 10 pg ml−1 for FKBPL and 15 pg ml−1 for CD44, which is more than one order lower than the standard ELISA method. Using clinical samples, a cut‐off value of 1.24 for CD44/FKBPL ratio provided positive predictive value of 100 % and the negative predictive value of 91 %. Our LFA shows promise as a rapid and highly sensitive point‐of‐care test for preeclampsia.
Efficient Transformation of Polymer Main Chain Catalyzed by Macrocycle Metal Complexes via Pseudorotaxane Intermediate
Authors: Takata Toshikazu , Yamamoto Koji , Higuchi Kazuki , Ogawa Masahiro , Kawasaki Ayumi , Mizuno Shunya , Iwasaki Hikaru , Nagashima Masaki , Hayashi Yoshihiro , Kawauchi Susumu , Nakazono Kazuko , Koyama Yasuhito 
Published: April 2023

AbstractPost‐synthesis modification of polymers streamlines the synthesis of functionalized polymers, but is often incomplete due to the negative polymer effects. Developing efficient polymer reactions in artificial systems thus represents a long‐standing objective in the fields of polymer and material science. Here, we show unprecedented macrocycle‐metal‐complex‐catalyzed systems for efficient polymer reaction that result in 100 % transformation of the main chain functional groups presumably via a processive mode reaction. The complete polymer reactions were confirmed in not only intramolecular reaction (hydroamination) but also intermolecular reaction (hydrosilylation) by using Pd‐ and Pt‐macrocycle‐catalyzed systems. The most fascinating feature of the both reactions is that higher‐molecular‐weight polymers reach completion faster. Various studies suggested that the reactions occur in the catalyst cavity via the formation of a supramolecular complex between the macrocycle catalyst and polymer substrate like pseudorotaxane, which should be of characteristic of the efficient polymer reactions progressing in a processive mode.
Photocatalytic Oxidation of NO2 on TiO2: Evidence of a New Source of N2O5
Authors: Chu Biwu , Liu Yuan , Li Hao , Jia Yongcheng , Liu Jun , Cao Qing , Chen Tianzeng , Zhang Peng , Ma Qingxin , Zeng Xiao Cheng , Francisco Joseph S. , He Hong 
Published: April 2023

AbstractN2O5 is an important intermediate in the atmospheric nitrogen cycle. Using a flow tube reactor, N2O5 was found to be released from the TiO2 surface during the photocatalytic oxidation of NO2, revealing a previously unreported source of N2O5. The rate of N2O5 release from TiO2 was dependent on the initial NO2 concentration, relative humidity, O2/N2 ratio, and irradiation intensity. Experimental evidence and quantum chemical calculations showed that NO2 can react with the surface hydroxyl groups and the generated electron holes on the TiO2, followed by combining with another NO2 molecule to form N2O5. The latter was physisorbed on TiO2 and had a low adsorption energy of −0.13 eV. Box model simulations indicated that the new source of N2O5 released from TiO2 can increase the daytime N2O5 concentration by up to 20 % in urban areas if abundant TiO2‐containing materials and high NOx concentrations were present. This joint experimental/theoretical study not only demonstrates a new chemical mechanism for N2O5 formation but also has important implications for air quality in urban areas.
Intermolecular Enantioselective Benzylic C(sp3)−H Amination by Cationic Copper Catalysis**
Authors: Dai Ling , Chen Ying‐Ying , Xiao Li‐Jun , Zhou Qi‐Lin 
Published: April 2023

AbstractChiral benzylic amines are privileged motifs in pharmacologically active molecules. Intramolecular enantioselective radical C(sp3)−H functionalization by hydrogen‐atom transfer has emerged as a straightforward, powerful tool for the synthesis of chiral amines, but methods for intermolecular enantioselective C(sp3)−H amination remain elusive. Herein, we report a cationic copper catalytic system for intermolecular enantioselective benzylic C(sp3)−H amination with peroxide as an oxidant. This mild, straightforward method can be used to transform an array of feedstock alkylarenes and amides into chiral amines with high enantioselectivities, and it has good functional group tolerance and broad substrate scope. More importantly, it can be used to synthesize bioactive molecules, including chiral drugs. Preliminary mechanistic studies indicate that the amination reaction involves benzylic radicals generated by hydrogen‐atom transfer.
Manganese spinel ferrites‐composite nanotubes impregnated thermally endured cellulose acetate membranes for superior desalination application
Authors: Afzal Amina , Shahid Fiza , Rafique Muhammad , Nazir Iqra 
Published: April 2023

AbstractManganese nanoferrites are decorated over single‐wall carbon nanotubes using in situ co‐precipitation technique to incorporate into cellulose acetate (CA) polymer in order to prepare nanocomposite membranes for salt rejection and desalination purpose. The microstructural study reveals the pore size of the synthesized membranes from 5 nm to 0.20 μm depending upon the loading concentration of the impregnated nanocomposite tubes. Fourier transform infrared (FTIR) and X‐ray diffraction (XRD) patterns of the synthesized membranes delineate the presence of decorated nanotubes in the host polymer matrix. Thermal degradation study proclaims the thermal endurance enhancement with increasing nanotubes concentration in the polymer matrix. Flux rate of the deionized (DI) water through the prepared membranes decreases with increasing nano‐filler concentration while this impact is observed inverse in salt rejection study of the aluminum sulphate (Al2(SO4)3) and zinc sulphate (ZnSO4) solutions due to the transformation of microporosity to nanoporosity with increasing composite tubes dosing into the host CA polymer.
Coordinate System Invariant Formulation of Fractional‐Dimensional Child‐Langmuir Law for a Rough Cathode
Authors: Zubair Muhammad , Fatima Adeela , Raheem Noreen , Ang Yee Sin , Mehmood Muhammad Qasim , Massoud Yehia 
Published: April 2023

AbstractThis work presents an exact closed‐form analytical model of the space charge limited (SCL) current density for planar, cylindrical, and spherical geometries in fractional dimensional spaces (Fα) where α represents the fractional dimensions having a range 0 < α ⩽ 1. Decreasing value of α shows an increasing degree of surface roughness. This analytical model approaches Langmuir–Blodgett equations for sufficiently close anode (Ra) and cathode (Rc) radii for integer dimensions (α = 1). To calculate SCL current density for any geometry, variational calculus (VC) is used to derive the differential equations in fractional (α) dimensions. The effect of electrode radius ratios on space charge limited current is investigated here considering the surface roughness.
Characteristics of near‐surface soil freeze–thaw status using high resolution CLM5.0 simulations on the Tibetan Plateau
Authors: Peng Qing , Jia Binghao , Lai Xin , Wang Longhuan , Huang Qifeng 
Published: April 2023

AbstractSoil freeze–thaw alternation is a natural characteristic of the Tibetan Plateau (TP), and plays an important role in surface energy balance and eco‐hydrological processes. The soil freeze–thaw process on the TP has changed significantly owing to global warming, affecting the alpine ecosystem structure and function. This study used high‐resolution atmospheric forcing datasets to drive the Community Land Model version 5.0 (CLM5.0) to simulate the near‐surface soil freeze–thaw status between 1979 and 2020. The simulated results were compared with in situ observations, and then the spatiotemporal distribution of the freeze start‐date (FSD), freeze end‐date (FED), freeze duration (FD), and thaw duration (TD) at a depth of 0.1 m were analyzed. The Nash–Sutcliffe efficiency coefficients (NSEs) of FSD, FED, FD, and TD between simulations and in situ observations were 0.77, 0.90, 0.98 and 0.92, and the correlation coefficients of FSD, FED, FD, TD were 0.97, 0.99, 0.99 and 0.98, respectively. The spatial distribution of FSD and TD was characterized by gradually increasing from northwest to southeast while FED and FD exhibited the opposite characteristics. FSD, FED, FD, and TD changed at an area‐mean rate of 1.1, −1.4, −2.5, and 2.5 days decade−1, respectively. This study provides an important reference for analyzing and predicting the changes in near surface soil freeze–thaw status on the TP under the warming climate.
Visualizing stimulus‐responsive dual‐ligand fluorescent probes for hypochlorite: A novel strategy for real application in tap water
Authors: Han Jianhong , Wang Yuting , Ren Zehua , Zhang Lianke , Hu Shuting , Li Yumei , Liu Pai 
Published: April 2023

AbstractAs an effective ingredient of disinfectants, ClO− inevitably remains in water, which induces potential health hazards such as lung damage and kidney disease. In this study, we synthesized stimulus‐responsive dual‐ligand luminol‐Tb‐GMP coordination polymer nanoparticles (luminol‐Tb‐GMP CPNPs) as highly selective fluorescent probes for the real‐time and visual detection of ClO−. CPNPs consist of Tb3+, a nuclear metal, that coordinates with GMP and luminol, an auxiliary ligand. GMP can be oxidized by ClO− and damage its structure, resulting in fluorescence quenching of CPNPs. The two‐ligand CPNPs sensor has a rapid fluorescent response, significant fluorescent color change, and high sensitivity, with a linear range of 2–18 μM and a detection limit of 0.14 μM. It has been successfully used to detect ClO− in tap water, fountain water, and drinking water. Simultaneously, the portable filter paper strip was prepared to expand the range of applications outside the laboratory, which will provide a promising application for the real‐time and semiquantitative analysis of ClO−.
Fluorescence imaging approaches for eco‐friendly determination of perampanel in human plasma and application for therapeutic drug monitoring
Authors: Hassan Said A. , Helmy Aya H. , Youssef Nadia F. , Weshahy Soheir A. , El‐zeany Badr A. 
Published: April 2023

AbstractAntiepileptic drugs are among the most common medications that require therapeutic drug monitoring (TDM). Indeed, TDM provides a realistic approach to adjust drug doses for epilepsy based on plasma concentrations to optimize its clinical outcome. The most common technique for TDM is high‐performance liquid chromatography, which has a very low green profile among analytical techniques. Perampanel (PER) is an inherently fluorescent compound that its fluorophore readily allows sensitive and quantitative measurements. This paper describes the development and validation of a sensitive, specific, and eco‐friendly spectrofluorimetric method for the determination of PER. Experimental parameters affecting fluorescence intensity of the compound, including solvent dilution, temperature, and excitation wavelength, were studied and optimized. The developed spectrofluorimetric method was established in acetonitrile at λex = 295 nm and λem = 431 nm over a concentration range of 5–60 ng/ml. The adopted method was applied for the determination of PER in human plasma; it was effective in the range of 15–50 ng/ml. The proposed method was found to be sensitive and specific for PER and can be applied successfully in TDM of PER and in quality control laboratories.
The experience of having a partner in prison—A systematic review and meta‐ethnography
Authors: McDonnell Darren , Lambert Sharon , Farrell Aoife 
Published: April 2023

AbstractThe number of individuals in prison is increasing worldwide. More and more family members are impacted by the imprisonment of a loved one. They face a variety of difficulties, such as social exclusion, mental health difficulties, stigma, and isolation. A systematic review and meta‐ethnography were carried out using Noblit & Hare's seven‐step approach to bring together the qualitative research in this area and support policy recommendations. Key databases were searched systematically and 12 studies, with varying aims, sample, and location, were included. The synthesis produced six core themes, reflecting the experiences of partners (mainly female): Role Transitions; Loss and Isolation; Shame and Secrecy; Encounters with the Prison Systems; Silver Linings; New Ways of Coping. The overarching narrative that integrates the findings suggests that the experience of having a partner in prison is a process of resocialisation. Partners not only conform to new circumstances and adjust their behaviour, but also adjust to changes in their roles and responsibilities, relationships, positions in society, and their futures. The findings, notwithstanding limitations and recommendations for future research, highlight the need for healthcare professionals, community and prison services, and policymakers to work together to support this population in their resocialisation process. Please refer to the Supplementary Material section to find this article'sCommunity and Social Impact Statement.
Rapid, Label‐Free Screening of Diverse Biotransformations by Flow‐Injection Mass Spectrometry
Authors: Berger Sarah A. , Grimm Christopher , Nyenhuis Jonathan , Payer Stefan E. , Oroz‐Guinea Isabel , Schrittwieser Joerg H. , Kroutil Wolfgang 
Published: April 2023

AbstractMass spectrometry‐based high‐throughput screening methods combine the advantages of photometric or fluorometric assays and analytical chromatography, as they are reasonably fast (throughput ≥1 sample/min) and broadly applicable, with no need for labelled substrates or products. However, the established MS‐based screening approaches require specialised and expensive hardware, which limits their broad use throughout the research community. We show that a more common instrumental platform, a single‐quadrupole HPLC‐MS, can be used to rapidly analyse diverse biotransformations by flow‐injection mass spectrometry (FIA‐MS), that is, by automated infusion of samples to the ESI‐MS detector without prior chromatographic separation. Common organic buffers can be employed as internal standard for quantification, and the method provides readily validated activity and selectivity information with an analytical run time of one minute per sample. We report four application examples that cover a broad range of analyte structures and concentrations (0.1–50 mM before dilution) and diverse biocatalyst preparations (crude cell lysates and whole microbial cells). Our results establish FIA‐MS as a versatile and reliable alternative to more traditional methods for screening enzymatic reactions.
Construction of Ternary PtRuPd Alloy Supported on Carbon Nanotubes for Concentrated Methanol Oxidation
Authors: Zhang Quan , Xie Yuhua , Zhang Xia , Zhao Mengxiao , Chen Qian , Wu Yiman , Yu Jiangfeng , Pan Qiyun , Yang Fangqi , Lin Huihui 
Published: April 2023

AbstractDue to the complex reaction process involving six‐electron transfer, high overpotential and slow kinetic rate of methanol oxidation, the development process of direct methanol fuel cells (DMFC) has been hampered. Herein, a simple one‐step solvent reduction approach was employed to simultaneously reduce metal ions supported on carbon nanotubes and prepared ternary metal alloy nanoparticles supported on carbon nanotubes electrocatalyst (PtRuPd@CNT). Compared with PtRu@CNT binary metal catalyst, the as‐prepared PtRuPd@CNT ternary metal catalyst displayed more outstanding methanol oxidation reaction (MOR) catalytic performance and good CO anti‐poisoning ability. In the case of using 8 M methanol, the MOR performance of PtRuPd@CNT was 1.8 times better than the PtRu@CNT electrocatalyst. The addition of the Pd atom regulates the surface electronic structure of PtRu alloy, and the strong electronic interaction enhances the MOR activity of the PtRu@CNT catalyst. Furthermore, the addition of the Pd atom in the PtRuPd@CNT electrocatalyst also diminishes adsorption of CO intermediate species on the Pt surface, boosting the CO anti‐poisoning ability of the catalyst and improving the stability. Therefore, the PtRuPd@CNT electrocatalyst incorporating the Pd atoms could actualize the practical application prospect as an efficient concentrated DMFC anode catalyst.