bluuebunny/crossref_metadata_2025_split huggingface dataset:
Highly Efficient Red Thermally Activated Delayed Fluorescence Nanoparticles for Real‐Time in Vivo Time‐Resolved Luminescence Imaging
Authors: Zhu Zece , Luo Zihan , Xie Yu‐Qing , Sun Yiting , Xu Li , Wu Qi 
Published: December 2023

AbstractThermally activated delayed fluorescence (TADF) nanoparticles are used importantly in time‐resolved luminescence imaging for eliminating the background signals from scattering and short‐lived autofluorescence. However, TADF nanoparticles are seldom used for real‐time time‐resolved luminescence imaging, due to their limited luminescence efficiency and lifetimes. To detect delayed fluorescence, multiple excitation cycles with adequate delay times are usually required, leading to long detecting durations and low imaging speed. Herein, highly efficient red TADF nanoparticles are developed through doping a guest molecule, TPAAQ (2,6‐bis[4‐(diphenylamino) phenyl] anthraquinone), in a host (4,4′‐bis(carbazol‐9‐yl)biphenyl, CBP) matrix. With a low doping concentration, the nanoparticles can exhibit obvious TADF with luminescence lifetimes over 0.1 ms and photoluminescence quantum yield up to 35%. A cell‐penetrating peptide is used together with the amphiphilic compound for assembling nanoparticles, which can easily penetrate cells and greatly increase the TADF signals for luminescence lifetime imaging. Thanks to the long‐lived and highly efficient TADF, real‐time in vivo time‐gated luminescence imaging of zebrafish is realized on a chopper‐based wide‐field microscope. This low‐cost time‐resolved luminescence imaging method showed a great potential for real‐time detection of life activities in many organisms with high autofluorescence.
3D Printing of Covalent Organic Frameworks: A Microfluidic‐Based System to Manufacture Binder‐Free Macroscopic Monoliths
Authors: Royuela Sergio , Sevim Semih , Hernanz Guillermo , Rodríguez‐San‐Miguel David , Fischer Peter , Franco Carlos , Pané Salvador , Puigmartí‐Luis Josep , Zamora Félix 
Published: December 2023

AbstractCovalent organic frameworks (COFs) have witnessed outstanding developments in the past 15 years, particularly in optimizing their pore structures, linkages, and variety of monomers used in their synthesis. Yet, a significant challenge remains unaddressed: the processability of COFs into macroscopic architectures with arbitrary shapes, as they are typically obtained as unprocessable powders. This study presents a novel strategy to address this issue by developing a 3D printable ink comprising a colloidal water suspension of COF nanoparticles. A microfluidic device is engineered that provides precise control over the gelation process of the COF‐based ink, allowing for a layer‐by‐layer fabrication. As a result, the direct production of large‐scale binder‐free COF architectures from digital designs is achieved at room temperature and atmospheric pressure while eliminating the use of toxic organic solvents.
Frank Partial Dislocations in Coplanar Ir/C Ultrathin Nanosheets Boost Hydrogen Evolution Reaction
Authors: Liu Pengfei , Zhang Xin , Fei Jiawei , Shi Yue , Zhu Jiawei , Zhang Dan , Zhao Liang , Wang Lei , Lai Jianping 
Published: December 2023

AbstractDeveloping highly active and stable acidic hydrogen evolution catalysts is of great significance and challenge for the long‐term operation of commercial proton exchange membrane (PEM) electrolyzers. In this work, coplanar ultrathin nanosheets composed of rich‐Frank partial dislocations (FPDs) are first synthesized. Ir nanoparticles and carbon (Dr‐Ir/C NSs) use a nonequilibrium high‐temperature thermal shock method (>1200 °C) and KBr template‐assisted techniques. Dr‐Ir/C NSs exhibit excellent hydrogen evolution reaction (HER) performance with a remarkably high mass activity of 6.64 A mg−1 at 50 mV, which is among the best Ir‐based catalysts.In addition, Dr‐Ir/C NSs are able to operate stably at 1.0 A cm−2 for 200 h as a cathode in a PEM electrolyser, and the original coplanar ultrathin nanosheets structure are maintained after the test, demonstrating excellent stability against stacking and agglomeration. Geometrical phase analysis and theoretical calculations show that the FPDs produce a 4% compressive strain in the Dr‐Ir/C NSs, and the compressive strain weaken the adsorption of H* by Ir, thus increasing the intrinsic activity of the catalyst.
A Green and Fluorine‐Free Fabrication of 3D Self‐Supporting MXene by Combining Anodic Electrochemical In Situ Etching with Cathodic Electrophoretic Deposition for Electrocatalytic Hydrogen Evolution
Authors: Sheng Minhao , Bin Xiaoqing , Yang Yawei , Chen Zhong , Que Wenxiu 
Published: December 2023

AbstractThe work presents a green and fluorine‐free environmentally friendly two‐electrode system, which enables the direct fabrication of the corresponding 3D MXene electrodes by the synergistic combination of anodic electrochemical in situ Al etching from Mo2TiAlC2 MAX and cathodic electrophoretic deposition. In just several minutes, the Mo2TiC2 MXene can be deposited on the cathode plate (Pt foil or carbon cloth) without the need for organic large‐molecule intercalation agents or ultrasound treatment. This approach allows an efficient separation of MXene from the electrolyte, leading to a significant reduction in the quantity of waste acid generated by conventional acid etching processes. The electrochemically etched‐MXene can be uniformly and stably deposited onto carbon cloth (E‐MXene@CC), enabling its direct utilization as a 3D electrocatalyst for hydrogen evolution reaction (HER). This unique 3D E‐MXene@CC exhibits a moderate HER performance and outperforms most of the reported pure non‐precious MXene‐based catalysts in 0.5 m H2SO4. In order to clarify the catalytic mechanism, in situ Raman spectroscopy of 3D E‐MXene@CC reveals a significant down‐shift without observing any new bands when the HER potential shifts negatively, which can be attributed to H+ intercalation.
Nitrogen and Sulfur Rich Covalent Organic Framework‐Chitosan Triboelectric Nanogenerator for Disposable Urination Evaluation Tool
Authors: Sathiyanathan Ponnan , Saatchi Daniel , Boo Yeonju , Mahato Manmatha , Wicklein Bernd , Kim Ji‐Seok , Yoo Hyunjoon , Song Tae‐Eun , Taseer Ashhad Kamal , Kim Won Jong , Oh Il‐Kwon 
Published: December 2023

AbstractRegular health checkups are crucial for the identification of problems in connection with acute and chronic diseases. Early detection helps patients prevent disease progression, receive more effective treatment, and improve their overall prognosis and quality of life. In this context, the introduction of cost‐effective, advanced sensor technology for the monitoring of healthcare is an essential and unavoidable approach. The present study proposes a disposable triboelectric nanogenerator (TENG) based sensor for a novel urination condition evaluation methodology that is integrated with an artificial intelligence (AI) algorithm. The disposable TENG sensor is fabricated using chitosan‐covalent organic framework (CS‐NSCoF). The optimized CS‐NSCoF (4%) composite, in contact with fluorinated ethylene propylene (FEP), yields remarkable output performance metrics: a peak‐to‐peak voltage of 132 V, a short‐circuit current of ≈2.38 µA, and an average power density of 10.89 mW m−2 at a load resistance of 200 MΩ. Notably, biocompatibility assessments confirm the non‐toxic nature of the CS‐NSCoF sample in this investigation.
Surface Defect Engineered Nano‐Cu/TiO2 Photocatalysts for Hydrogen Production
Authors: Liccardo Letizia , Moras Paolo , Sheverdyaeva Polina M. , Vomiero Alberto , Caballero Alfonso , Colón Gerardo , Moretti Elisa 
Published: December 2023

AbstractSurface defects engineered nano‐Cu/TiO2 photocatalysts are synthesized through an easy and cost‐effective microwave‐assisted hydrothermal synthesis, mixing commercial P25 titania (TiO2) and oxalic acid (Ox), followed by 2.0 wt% Cu co‐catalyst (labeled as Cu2.0) loading through in situ photodeposition during reaction. The hydrothermal treatment does not affect the catalyst crystalline structure, morphology, nor the surface area. However, depending on the Ox/TiO2 molar ratio used an influence on the optical properties and on the reactivity of the system is detected. The presence of surface defects leads to intraband states formation between valence band and conduction band of bare titania, inducing an important enhancement in the photoactivity. Thus, Cu2.0/gOx/P25 200 (where g is the weight of Ox and 200 the temperature in Celsius degrees used during the synthesis) have been successfully tested as efficient photocatalysts for hydrogen production through methanol (MeOH) reforming under UV light in a MeOH/ H2O solution (10% v/v) by fluxing the system with N2, showing an increased reactivity compared to the bare Cu2.0/P25 system.
Chemical Evolution and Biological Evaluation of Natural Products for Efficient Therapy of Acute Lung Injury
Authors: Fan Chengcheng , Zhang Zeyi , Lai Zhencheng , Yang Yanzi , Li Jiaming , Liu Lei , Chen Siyu , Hu Xueping , Zhao Huajun , Cui Sunliang 
Published: December 2023

AbstractAcute lung injury (ALI) is one of the most common complications in COVID‐19 and also a syndrome of acute respiratory failure with high mortality rates, but lacks effective therapeutic drugs. Natural products provide inspiration and have proven to be the most valuable source for bioactive molecule discovery. In this study, the chemical evolution of the natural product Tanshinone IIA (Tan‐IIA) to achieve a piperidine‐fused scaffold through a synthetic route of pre‐activation, multi‐component reaction, and post‐modification is presented. Through biological evaluation, it is pinpointed that compound 8b is a standout candidate with remarkable anti‐inflammation and anti‐oxidative stress properties, coupled with low toxicity. The mechanistic study unveils a multifaceted biological profile of 8b and shows that 8b is highly efficient in vivo for the treatment of ALI. Therefore, this work not only provides an effective strategy for the treatment of ALI, but also offers a distinctive natural product‐inspired drug discovery.
Aquatic Functional Liquid Crystals: Design, Functionalization, and Molecular Simulation
Authors: Kato Takashi , Uchida Junya , Ishii Yoshiki , Watanabe Go 
Published: December 2023

AbstractAquatic functional liquid crystals, which are ordered molecular assemblies that work in water environment, are described in this review. Aquatic functional liquid crystals are liquid‐crystalline (LC) materials interacting water molecules or aquatic environment. They include aquatic lyotropic liquid crystals and LC based materials that have aquatic interfaces, for example, nanoporous water treatment membranes that are solids preserving LC order. They can remove ions and viruses with nano‐ and subnano‐porous structures. Columnar, smectic, bicontinuous LC structures are used for fabrication of these 1D, 2D, 3D materials. Design and functionalization of aquatic LC sensors based on aqueous/LC interfaces are also described. The ordering transitions of liquid crystals induced by molecular recognition at the aqueous interfaces provide distinct optical responses. Molecular orientation and dynamic behavior of these aquatic functional LC materials are studied by molecular dynamics simulations. The molecular interactions of LC materials and water are key of these investigations. New insights into aquatic functional LC materials contribute to the fields of environment, healthcare, and biotechnology.
Fully Integrated Microfluidic Platform for Multiplexed Detection of Hunov by a Dynamic Confined‐Space‐Implemented One‐Pot Rpa‐Lamp System
Authors: Chen Fumin , Lyu Chenang , Li Zhao , Xiu Leshan , Li Huimin , Xie Yi , Cao Runzhen , Hu Qinqin , Yin Kun 
Published: December 2023

AbstractHuman norovirus (HuNoV) is the leading cause of nonbacterial acute gastroenteritis, which is highly infectious, rapidly evolving, and easily transmitted through feces. The accurate and early detection of HuNoV subtypes is essential for effective treatment, early surveillance, risk assessment, and disease prevention. In this study, a portable multiplex HuNoV detection platform that combines integrated microfluidics and cascade isothermal amplification, using a streamlined protocol for clinical fecal‐based diagnosis is presented. To overcome the problems of carryover contamination and the incompatibility between recombinase polymerase amplification (RPA) and loop‐mediated isothermal amplification (LAMP), a Dynamic confined‐space‐implemented One‐pot RPA‐LAMP colorimetric detection system (DORLA) is developed by creating a hydrogen bond network. The DORLA system exhibits excellent sensitivity, with detection limits of 10 copies µL−1 and 1 copy µL−1 for HuNoV GI and GII, respectively. In addition, a portable diagnostic platform consisting of a thermostatic control module and an integrated 3D‐printed microfluidic chip for specific HuNoV capture, nucleic acid pretreatment, and DORLA detection, which enables simultaneous diagnosis of HuNoV GI and GII is developed. A DORLA‐based microfluidic platform exhibits satisfactory performance with high sensitivity and portability, and has high potential for the rapid point‐of‐care detection of HuNoV in clinical fecal samples, particularly in resource‐limited settings.
Construction of 1,3‐Nonadjacent Stereogenic Centers Through Enantioselective Addition of α‐Thioacetamides to α‐Substituted Vinyl Sulfones Catalyzed by Chiral Strong Brønsted Base
Authors: Kondoh Azusa , Ojima Rihaku , Ishikawa Sho , Terada Masahiro 
Published: December 2023

AbstractAn enantioselective addition reaction for the construction of 1,3‐nonadjacent stereogenic centers is developed by means of a chiral strong Brønsted base catalyst. The chiral sodium ureate catalyst efficiently promoted the reaction of α‐thioacetamides as less acidic pronucleophiles with vinyl sulfones having a variety of α‐substituents including aryl, alkyl and halo groups, and α‐phenylacrylates, accomplishing the construction of various 1,3‐nonadjacent stereogenic centers in highly diastereo‐ and enantioselective manners. This is a rare example of the construction of 1,3‐nonadjacent stereogenic centers with less acidic pronucleophiles. In addition, the application of Michael acceptors having various types of α‐substituents in a single catalyst system is achieved for the first time, demonstrating the utility of the present catalyst system for the construction of 1,3‐nonadjacent stereogenic centers.
Synthetic Gene Circuits for Regulation of Next‐Generation Cell‐Based Therapeutics
Authors: Teixeira Ana P. , Fussenegger Martin 
Published: December 2023

AbstractArming human cells with synthetic gene circuits enables to expand their capacity to execute superior sensing and response actions, offering tremendous potential for innovative cellular therapeutics. This can be achieved by assembling components from an ever‐expanding molecular toolkit, incorporating switches based on transcriptional, translational, or post‐translational control mechanisms. This review provides examples from the three classes of switches, and discusses their advantages and limitations to regulate the activity of therapeutic cells in vivo. Genetic switches designed to recognize internal disease‐associated signals often encode intricate actuation programs that orchestrate a reduction in the sensed signal, establishing a closed‐loop architecture. Conversely, switches engineered to detect external molecular or physical cues operate in an open‐loop fashion, switching on or off upon signal exposure. The integration of such synthetic gene circuits into the next generation of chimeric antigen receptor T‐cells is already enabling precise calibration of immune responses in terms of magnitude and timing, thereby improving the potency and safety of therapeutic cells. Furthermore, pre‐clinical engineered cells targeting other chronic diseases are gathering increasing attention, and this review discusses the path forward for achieving clinical success. With synthetic biology at the forefront, cellular therapeutics holds great promise for groundbreaking treatments.
Beyond Imperfections: Exploring Defects for Breakthroughs in Perovskite Solar Cell Research
Authors: Min Jihyun , Choi Yelim , Kim Dohyun , Park Taiho 
Published: December 2023

AbstractThe field of solar systems has undergone rapid development with the emergence of the special material, perovskite. Perovskite's unique mechanism, defect tolerance, has enabled perovskite solar cells (PSCs) to achieve high power conversion efficiencies (PCEs), and many studies on this subject have been conducted. “Defect tolerance” indicates that the defects in perovskite are primarily generated at the shallow‐energy level and do not occur through nonradiative recombination. However, this also indicates that defects are well formed in perovskite films and that the shallow defects can transform into deep traps, leading to long‐term stability issues. Therefore, controlling defects in perovskite is essential for developing PSCs with high PCEs. The causes of defects in perovskite are diverse, and the defect patterns differ considerably, particularly depending on the location of the PSCs. In this review, the defects generated in perovskite will be discussed and review several methods for passivating them at different.
Solvent‐Mediated Synthesis of Functional Powder Materials from Deep Eutectic Solvents for Energy Storage and Conversion: A Review
Authors: Deng Rongrong , Gao Mingyuan , Zhang Bo , Zhang Qibo 
Published: December 2023

AbstractDeveloping advanced electrochemical energy storage and conversion (ESC) technologies based on renewable clean energy can alleviate severe global environmental pollution and energy crisis. The efficient preparation of functional electrode materials via a simple, green, and safe synthesis process is the key to the commercial feasibility of these ESC systems. Deep eutectic solvents (DESs) with easy‐tunable solvent properties and recyclable features have emerged as novel solvent systems for designing and synthesizing various functional powder materials for ESC devices. In this paper, the application of DESs in the synthesis of energy‐related functional powder materials is systematically reviewed. After briefly introducing the classification and synthesis of DESs, their critical roles in synthesizing powder materials are discussed. Then, the recent advances of DES‐derived powder materials in ESC, including batteries, fuel cells, supercapacitors, and water splitting, are described in detail from the perspective of preparation‐structure‐activity. Finally, some challenges and development directions of the DESs‐mediated synthesis of powder materials with high electrochemical performance for ESC applications are outlined.
Among‐individual variation in flowering phenology affects flowering synchrony and mating opportunity
Authors: Shelton Wendy R. , Mitchell Randall J. , Christopher Dorothy A. , Jack Loretha P. , Karron Jeffrey D. 
Published: December 2023

AbstractPremiseThe timing and pattern of a plant's flowering can have important consequences for reproductive success. Variation in flowering phenology may influence the number of prospective mates, the risk of mating with lower quality individuals, and the likelihood of self‐pollination. Here we use a common garden experiment to explore within‐ and among‐population variation in phenology. Our work provides new insights into how flowering phenology shapes mating opportunity and flowering synchrony in a self‐compatible perennial.MethodsTo quantify variation in flowering phenology we raised progeny from nine populations of Mimulus ringens in a common garden. For each individual, we measured phenological traits including age at flowering onset, daily floral display size, total flower number, and flowering synchrony with other members of the population, and related these traits to mating opportunity. We also tested how individual flowering schedules influence the magnitude of synchrony.ResultsFlowering phenology and synchrony varied substantially within and among populations. From day to day, plants often oscillated between large and small daily floral displays. Additionally, flowering schedules of individual plants strongly influenced flowering synchrony and, along with the number of flowering days, markedly affected plants' mating opportunity.ConclusionsPhenological traits such as flowering synchrony can affect the quantity of mating opportunities and may be important targets of natural selection. Our results highlight the need for studies that quantify flowering patterns of individuals as well as populations.
Facial dysmorphology in children exposed in pregnancy to anticonvulsant medications correlates with deficits in IQ
Authors: Holmes Lewis B. , Hunt Anne‐Therese , Will Leslie A. , Dhillon Ruby , Deutsch Curtis , Adams Jane 
Published: December 2023

AbstractSome children exposed at conception to the antiepileptic drugs (AEDs) phenytoin (PHT), phenobarbital (PB), and carbamazepine (CBZ) have changes in their midface and fingers. It has been suggested that the anticonvulsant‐exposed child with these subtle changes in facial features (the “anticonvulsant face”) has a greater likelihood of having deficits in IQ in comparison with children exposed to the same anticonvulsants who do not have these features. 115 AED‐exposed children (40, PHT; 34, PB; and 41, CBZ) between 6.5 and 16 years of age and 111 unexposed children matched by sex, race, and year in school were evaluated. The evaluations were (WISC‐III), physical examination with measurements of facial features and digits and photographs. The AED‐exposed children had cephalometric radiographs, but not the unexposed. Each parent had a similar examination of face and hands plus tests of intelligence. These AED‐exposed children showed an increased frequency of a short nose and anteverted nares, features of the “anticonvulsant face.” Lateral skull radiographs showed a decrease in the angle between the anterior cranial base and nasal bone, which produces anteverted nares. Mean IQs were significantly lower on one or more IQ measures for the children with these facial features. Shortening of the distal phalanges and small fingernails correlated with the presence of a short nose in that child. The findings in 115 children exposed at conception to either phenytoin, phenobarbital, or carbamazepine, as monotherapy, confirmed the hypothesis that those with a short nose and anteverted nares had a lower IQ than exposed children without those features.
Electrohydrogenation of Nitriles with Amines by Cobalt Catalysis
Authors: Wang Tiantian , He Fangfang , Jiang Wei , Liu Jie 
Published: December 2023

AbstractCatalytic hydrogenation of nitriles represents an efficient and sustainable one‐step synthesis of valuable bulk and fine chemicals. We report herein a molecular cobalt electrocatalyst for selective hydrogenative coupling of nitriles with amines using protons as the hydrogen source. The key to success for this reductive reaction is the use of an electrocatalytic approach for efficient cobalt‐hydride generation through a sequence of cathodic reduction and protonation. As only electrons (e−) and protons (H+) as the redox equivalent and hydrogen source, this general electrohydrogenation protocol is showcased by highly selective and straightforward synthesis of various functionalized and structurally diverse amines, as well as deuterium isotope labeling applications. Mechanistic studies reveal that the electrogenerated cobalt‐hydride transfer to nitrile process is the rate‐determining step.