bluuebunny/crossref_metadata_2025_split huggingface dataset:
Advancing Insights into Electrochemical Pre‐Treatments of Supported Nanoparticle Electrocatalysts by Combining a Design of Experiments Strategy with In Situ Characterization
Authors: Mule Aniket S. , Tran Kevin , Aleman Ashton M. , Cornejo‐Carrillo Yamile E. , Kamat Gaurav A. , Stevens Michaela Burke , Jaramillo Thomas F. 
Published: August 2024

AbstractActivation, break‐in, and/or pre‐treatment protocols are generally applied to energy conversion devices before regular operation to reach stable performance. There remains much to understand about the relationships among physical properties, performance, and electrochemical pre‐treatments. Here, a design‐of‐experiments (DoE) strategy is employed to address this gap by demonstrating the influence of five pre‐treatment parameters for carbon‐supported Pt‐nanoparticle catalysts on the electrocatalytic oxygen reduction reaction (ORR). A subset of pre‐treatments, developed using a central composite design, are tested in a flow cell combined with an inductively‐coupled plasma mass spectrometer (on‐line ICP‐MS). The DoE‐based approach facilitates comprehensive insights from two orders of magnitude fewer experiments than a conventional grid search. The coupled on‐line ICP‐MS setup enables effective catalysis and real‐time catalyst dissolution data. Leveraging insights from DoE for on‐line ICP‐MS and additional characterization, a model is built between the degradation of a multi‐dimensional supported Pt surface, its performance, and applied electrochemical parameters. These investigations identify surface modifications, such as oxidation, and subsequent restructuring of Pt during pre‐treatment as a primary cause of performance deterioration during ORR. By combining DoE with advanced characterization techniques, a powerful approach is demonstrated to gain a mechanistic understanding of pre‐treatment protocols that can be broadly adapted to various reaction chemistries.
Sea trout (Salmo trutta) activity and movement patterns in response to environmental cues in a fjord system
Authors: Staveley Thomas A. B. , van der Meijs Felix , Gullström Martin 
Published: August 2024

AbstractAs a predatory fish that migrates between freshwater and marine environments, the sea trout (Salmo trutta) is important in linking these systems. This study investigated movement patterns of sea trout in a coastal fjord at the Swedish Skagerrak region from August 2018 to January 2019, using acoustic telemetry, while assessing these against environmental variables across different spatial and temporal scales. Six acoustic receivers were deployed in the fjord and a river, which flows into the upper reaches of the fjord, with the aim of detecting 20 sea trout that had been tagged with acoustic transmitters. Sea surface temperature and winds (east–west) affected movement patterns of the sea trout the most, while changes in atmospheric pressure were also important, but to a lesser extent. Sea surface temperature and atmospheric pressure both had a positive relationship with the number of detections, whereas stronger winds from the east (i.e. from land) resulted in more detections than stronger winds from the west (i.e. from the ocean). In addition, interesting diel (day–night) movement patterns were observed for some fish. A significant positive correlation was also discovered between the weight of the fish and the number of detections. This study offers insight in movements of sea trout that use coastal habitats and how environmental conditions can affect movement patterns in a fjord system. To further our understanding of sea trout movement patterns and connectivity, tracking from river, through fjord, out to sea and at a longer time scale with more variation in fish size would be valuable to understand more about the complex movement dynamics of this important species.
Divergent lineages in a young species: The case of datilillo (Yucca valida), a broadly distributed plant from the Baja California Peninsula
Authors: Aleman Alberto , Arteaga Maria Clara , Gasca‐Pineda Jaime , Bello‐Bedoy Rafael 
Published: August 2024

AbstractPremiseGlobally, barriers triggered by climatic changes have caused habitat fragmentation and population allopatric divergence. Across North America, oscillations during the Quaternary have played important roles in the distribution of wildlife. Notably, diverse plant species from the Baja California Peninsula in western North America, isolated during the Pleistocene glacial–interglacial cycles, exhibit strong genetic structure and highly concordant divergent lineages across their ranges. A representative plant genus of the peninsula is Yucca, with Y. valida having the widest range. Although a dominant species, it has an extensive distribution discontinuity between 26° N and 27° N, suggesting restricted gene flow. Moreover, historical distribution models indicate the absence of an area with suitable conditions for the species during the Last Interglacial, making it an interesting model for studying genetic divergence.MethodsWe assembled 4411 SNPs from 147 plants of Y. valida throughout its range to examine its phylogeography to identify the number of genetic lineages, quantify their genetic differentiation, reconstruct their demographic history and estimate the age of the species.ResultsThree allopatric lineages were identified based on the SNPs. Our analyses support that genetic drift is the driver of genetic differentiation among these lineages. We estimated an age of less than 1 million years for the common ancestor of Y. valida and its sister species.ConclusionsHabitat fragmentation caused by climatic changes, low dispersal, and an extensive geographical range gap acted as cumulative mechanisms leading to allopatric divergence in Y. valida.
Die Click‐to‐Release‐Aktivierung des Reserveantibiotikums Colistin am Zielort verringert dessen Nierentoxizität
Authors: Charoenpattarapreeda Jiraborrirak , Tegge Werner , Xu Chunfa , Harmrolfs Kirsten , Hinkelmann Bettina , Wullenkord Hannah , Hotop Sven‐Kevin , Beutling Ulrike , Rox Katharina , Brönstrup Mark 
Published: August 2024

AbstractDer Einsatz hochwirksamer, aber zugleich toxischer Antibiotika wie Colistin ist aufgrund der Zunahme antimikrobieller Resistenzen unvermeidlich geworden. Wir berichten hier, wie geschütztes Colistin chemisch am Ort der Infektion kontrolliert mithilfe von click‐to‐release‐Reaktionen freigesetzt werden kann, um seine systemische Toxizität zu verringern. Kinetische Experimente mit neun Tetrazinen und drei Dienophilen zeigten eine besonders schnelle Wirkstoff‐Freisetzung über eine Diels–Alder‐Reaktion mit inversem Elektronenbedarf zwischen einem trans‐Cycloocten (TCO) und dem aminfunktionalisierten Tetrazin Tz7. Die antibiotische Aktivität von Colistin gegen Escherichia coli wurde durch TCO‐Einheiten maskiert, aber durch die Reaktion mit d‐Ubi−Tz, einem Tetrazin, das mit dem an Bakterien bindenden Peptid D‐Ubi29–41 funktionalisiert ist, wiederhergestellt. Während neutral geladenes TCO die Toxizität gegenüber der humanen proximalen Tubulus‐Nierenzelllinie HK‐2 nicht verbesserte, verringerte mit Asparaginsäure modifiziertes TCO die Gesamtladung des Peptids und den Eintritt in die Nierenzellen, wodurch seine Toxizität drastisch verringert wurde. Das Analogon Col−(TCO‐Asp)1 zeigte bei Mäusen günstige pharmakokinetische Eigenschaften und wurde in einem in vivo Infektionsmodell durch d‐Ubi−Tz lokal in der Lunge aktiviert, während es ohne den chemischen Auslöser inaktiv blieb. Diese Studie liefert das erste Beispiel für ein systemisch wirkendes Zweikomponenten‐Antibiotikum mit verbesserter Arzneimittelverträglichkeit.
Highly Selective Production of C2+ Oxygenates from CO2 in Strongly Acidic Condition by Rough Ag‐Cu Electrocatalyst
Authors: Yang Yisen , Zhang Jianling , Tan Zhonghao , Yang Jie , Wang Sha , Li Meiling , Su Zhuizhui 
Published: August 2024

AbstractThe acidic electrocatalytic conversion of CO2 to multi‐carbon (C2+) oxygenates is of great importance in view of enhancing carbon utilization efficiency and generating products with high energy densities, but suffering from low selectivity and activity. Herein, we synthesized Ag−Cu alloy catalyst with highly rough surface, by which the selectivity to C2+ oxygenates can be greatly improved. In a strongly acidic condition (pH=0.75), the maximum C2+ products Faradaic efficiency (FE) and C2+ oxygenates FE reach 80.4 % and 56.5 % at −1.9 V versus reversible hydrogen electrode, respectively, with a ratio of FEC2+ oxygenates to FEethylene up to 2.36. At this condition, the C2+ oxygenates partial current density is as high as 480 mA cm−2. The in situ spectra, control experiments and theoretical calculations indicate that the high generation of C2+ oxygenates over the catalyst originates from its large surface roughness and Ag alloying.
A Bio‐Inspired Multifunctional Hydrogel Network with Toughly Interfacial Chemistry for Dendrite‐Free Flexible Zinc Ion Battery
Authors: Yang Song , Wu Qing , Li Yue , Luo Fusheng , Zhang Jinlong , Chen Kui , You Yang , Huang Jun , Xie Haibo , Chen Yiwang 
Published: August 2024

AbstractFlexible and high‐performance aqueous zinc‐ion batteries (ZIBs), coupled with low cost and safe, are considered as one of the most promising energy storage candidates for wearable electronics. Hydrogel electrolytes present a compelling alternative to liquid electrolytes due to their remarkable flexibility and clear advantages in mitigating parasitic side reactions. However, hydrogel electrolytes suffer from poor mechanical properties and interfacial chemistry, which limits them to suppressed performance levels in flexible ZIBs, especially under harsh mechanical strains. Herein, a bio‐inspired multifunctional hydrogel electrolyte network (polyacrylamide (PAM)/trehalose) with improved mechanical and adhesive properties was developed via a simple trehalose network‐repairing strategy to stabilize the interfacial chemistry for dendrite‐free and long‐life flexible ZIBs. As a result, the trehalose‐modified PAM hydrogel exhibits a superior strength and stretchability up to 100 kPa and 5338 %, respectively, as well as strong adhesive properties to various substrates. Also, the PAM/trehalose hydrogel electrolyte provides superior anti‐corrosion capability for Zn anode and regulates Zn nucleation/growth, resulting in achieving a high Coulombic efficiency of 98.8 %, and long‐term stability over 2400 h. Importantly, the flexible Zn//MnO2 pouch cell exhibits excellent cycling performance under different bending conditions, which offers a great potential in flexible energy‐related applications and beyond.
Chirality and Curvature on Protein Adsorption and Osteogenesis
Authors: Li Meijun , Jiang Shengjie , Wang Xiaowei , Xu Wei , Du Cong , Wei Yan , Deng Xuliang , Liu Minghua 
Published: August 2024

AbstractHere we designed enantiomeric lipid‐mimetic glutamic acid derivatives (L/D‐UG) and investigated their self‐assembled chiral nanostructures’ interaction with the protein adsorption as well as the osteogenesis. It was found that L or D‐UG molecules can self‐assemble into vesicle bilayers and two‐dimensional (2D) nanocrystals via a kinetic and thermodynamic control, respectively. These chiral vesicles and 2D crystals showed differentiated adsorption of proteins, determined by their curvature and chirality. Specifically, fibronectin constituted by L‐amino acids adsorbed preferentially on L‐UG 2D crystal in a semi‐random pattern and L‐2D nanocrystal show as the most effective structures to promote bone regeneration. The controlled vesicle and 2D crystal assemblies with different chirality and curvature helps to clarify their determine roles in protein adsorption and osteogenesis.
Arginine Accelerates Sulfur Fluoride Exchange and Phosphorus Fluoride Exchange Reactions between Proteins
Authors: Cao Li , Yu Bingchen , Klauser Paul C. , Zhang Pan , Li Shanshan , Wang Lei 
Published: August 2024

AbstractSulfur fluoride exchange (SuFEx) and phosphorus fluoride exchange (PFEx) click chemistries are advancing research across multiple disciplines. By genetically incorporating latent bioreactive unnatural amino acids (Uaas), these chemistries have been integrated into proteins, enabling precise covalent linkages with biological macromolecules and paving the way for new applications. However, their suboptimal reaction rates in proteins limit effectiveness, and traditional catalytic methods for small molecules are often incompatible with biological systems or in vivo applications. We demonstrated that introducing an arginine adjacent to the latent bioreactive Uaa significantly boosts SuFEx and PFEx reaction rates between proteins. This method is effective across various Uaas, target residues, and protein environments. Notably, it also enables efficient SuFEx reactions in acidic conditions, common in certain cellular compartments and tumor microenvironments, which typically hinder SuFEx reactions. Furthermore, we developed the first covalent cell engager that substantially enhances natural killer cell activation through improved covalent interaction facilitated by arginine. These findings provide mechanistic insights and offer a biocompatible strategy to harness these robust chemistries for advancing biological research and developing new biotherapeutics.
Light‐Controlled Bioorthogonal Chemistry Altered Natural Killer Cell Activity for Boosted Adoptive Immunotherapy
Authors: Liu Zhengwei , Zhang Wenting , Zhao Huisi , Sun Mengyu , Zhao Chuanqi , Ren Jinsong , Qu Xiaogang 
Published: August 2024

AbstractNatural killer (NK) cell‐based immunotherapy has received much attention in recent years. However, its practical application is still suffering from the decreased function and inadequate infiltration of NK cells in the immunosuppressive microenvironment of solid tumors. Herein, we construct light‐responsive porphyrin Fe array‐armed NK cells (denoted as NK@p‐Fe) for cell behavior modulation via bioorthogonal catalysis. By installing cholesterol‐modified porphyrin Fe molecules on the NK cell surface, a catalytic array with light‐harvesting capabilities is formed. This functionality transforms NK cells into cellular factories capable of catalyzing the production of active agents in a light‐controlled manner. NK@p‐Fe can generate the active antineoplastic drug doxorubicin through bioorthogonal reactions to enhance the cytotoxic function of NK cells. Beyond drug synthesis, NK@p‐Fe can also bioorthogonally catalyze the production of the FDA‐approved immune agonist imiquimod (IMQ). The activated immune agonist plays a dual role, inducing dendritic cell maturation for NK cell activation and reshaping the tumor immunosuppressive microenvironment for NK cell infiltration. This work represents a paradigm for the modulation of adoptive cell behaviors to boost cancer immunotherapy by bioorthogonal catalysis.
Tunable, reagent‐loaded polyurethane nanocapsules cleavable by NIR light
Authors: Avlasevich Yuri , Baluschev Stanislav , Landfester Katharina 
Published: August 2024

AbstractDual response polyurethane nanocapsules consisting of a hydrophilic core are synthesized via interfacial polyaddition of the diisocyanate monomers and different diols (VA‐060 and glycols) in inverse miniemulsion process. The presence of the water‐soluble NIR dye in the core and azo‐bonds in the polymer shell allows the selective release of encapsulated material triggered by temperature or NIR light. The capsules are characterized by transmission electron microscopy (TEM) and dynamic light scattering (DLS). The capsule degradation under external stimuli, like temperature and NIR light, is confirmed microscopically by TEM. Macroscopic evidence of the capsule cleavage was achieved by the incorporation of the chemical into the capsule core, and subsequent treatment of the capsules with NIR laser in the presence of the suitable reagent outside the capsules. A color‐forming chemical reaction occurred after the shell opening. The reactions were easily detected by visual observation of a color change and by UV–Vis spectroscopy.
Reprocessable carbon fiber vitrimer composites: Reclamation and reformatting of carbon fibers for second generation composite materials
Authors: Sharma Harsh , Bender Marcel , Kim Geonwoo , Lee Dongkwan , Caglayan Cigdem , Schlögl Sandra , Yun Gun Jin , Kumar Ajay , Rana Sravendra 
Published: August 2024

AbstractCarbon fibers (CFs) are experiencing a growing demand owing to their low specific weight, exceptional mechanical properties, superior temperature, and corrosion resistance, however, their sustainability and energy consumption during manufacturing is still a challenge. Therefore, reclamation of waste CFs and their reformatting has gained significant attention. Herein, we synthesized a chemically degradable vitrimer matrix by curing bisphenol‐A diglycidyl ether (BADGE) with 2‐aminophenyl disulfide (2‐AFD) and further utilized the matrix for the development of CF reinforced composites (CFRCs) through vacuum‐assisted resin infusion molding (VARIM) process. The obtained vitrimeric system and its composites show excellent mechanical, self‐adhering, shape‐memory, and reprocessing properties. Meanwhile, the developed CFRP vitrimer composites can be rapidly dissolved in thiol solvent (1‐octanethiol), resulting in the efficient recycling of CFs. X‐ray diffraction, scanning electron microscopy, and Raman spectroscopy validate that the chemical structure of the recycled fibers closely resembles the structure of the original CFs. The recycled CFs were further used to prepare second generation composite materials with excellent thermal, dynamic, and mechanical properties for nonstructural applications (e.g., sports, automotive, etc.). Thus, with an effective CF recycling method, this study can assist in preparing reliable, long‐term functional, recyclable, and high‐performance composites.
A phosphorus/fluorine‐containing block copolymer endows epoxy with multifunctionality
Authors: Chen Yongming , Liu Xiaohui , Wu Shunwei , Li Lu , Zeng Birong , Luo Weiang , He Kaibin , Xu Yiting , Yuan Conghui , Dai Lizong 
Published: August 2024

AbstractIn order to achieve flame retardant, hydrophobic, and toughened epoxy resins, phosphorus/fluorine‐containing block copolymer (FBCP) was synthesized by reversible addition‐fragmentation chain transfer polymerization, and then the as‐synthesized PMADOPO‐b‐PHFBA block copolymer was used as additive to modify the epoxy resin, accompanying with a random copolymer (FRCP) serving as control group. It showed that due to the regular arrangement of molecular chains, FBPC formed a fibrous‐like structure at the fracture interface of epoxy/PMADOPO‐b‐PHFBA (EP/FBCP) samples, effectively enhancing the toughness of epoxy composite materials. The fracture energy of EP90/FBCP‐10 was higher than that of EP90/FRCP‐10 and was about twice than that of pure EP. The addition of 3 wt% FBCP could enhance the limited oxygen index (LOI) of EP97/FBCP‐3 to 33.2% and reached a V‐1 UL‐94 rating. As the addition of FBCP increased, the LOI gradually increased. When the addition of FBCP was 10%, the LOI and UL‐94 of EP90/FBCP‐10 was 38.2% and V‐0 grade, respectively. Meanwhile, the presence of fluorine element effectively reduced the surface energy of the composite EP material. Compared with pure EP, the water contact angle of EP90/FBCP‐10 was about 101° with an increasing of 20.8%. Furthermore, the flame‐retardant mechanism of EP/FBCP epoxy composites was discussed.
Breastfeeding patterns in infants are associated with a later diagnosis of autism Spectrum disorder
Authors: Elbedour Leena , Balaum Rewaa , Alhozyel Einav , Meiri Gal , Zigdon Dikla , Michaelovski Analya , Kerub Orly , Menashe Idan 
Published: August 2024

AbstractBreastfeeding is associated with medical and developmental benefits. This study aimed to assess associations between nutritional patterns in the first year of life and the likelihood of autism spectrum disorder (ASD). 270 children diagnosed with ASD (cases) and 500 neurotypical children (controls) matched to cases by sex, ethnicity, and birth date (± 3 months) were included in this retrospective case–control study. Both groups were ascertained from children born between 2014 and 2017 whose development/nutrition were monitored at mother–child health clinics in southern Israel. Conditional logistic regression was used to determine the independent association of nutritional patterns with ASD while adjusting for socio‐demographic and clinical characteristics. Both exclusive and partial breastfeeding modes were associated with decreased odds of ASD diagnosis (aOR = 0.221, 95%CI = 0.136–0.360; aOR = 0.494, 95%CI = 0.328–0.743, respectively). A breastfeeding duration of >12 months was associated with lower ASD odds (aOR = 0.418, 95%CI = 0.204–0.855), while the introduction of solids after 6 months of age was associated with higher ASD odds than the introduction of solids at 6 months (aOR = 2.455, 95%CI = 1.116–4.201). These findings suggest that a longer period of exclusive breastfeeding is associated with a subsequent reduced likelihood of ASD diagnosis, thus reiterating the importance of proper post‐natal nutrition for infant neurodevelopment.
Development of an amperometric biosensor that can determine the amount of glucose in the blood using the glucose oxidase enzyme: Preparation of polyaniline–polypyrrole–poly(sodium‐4‐styrenesulfonate) film
Authors: Uzumer Tugce Yagmur , Cete Servet , Tekeli Yener , Altuner Elif Esra 
Published: August 2024

AbstractIn this study, a new amperometric biosensor was developed for glucose determination. For this purpose, polyaniline–polypyrrole–poly(sodium‐4‐styrenesulfonate) film was prepared by electropolymerization of aniline and pyrrole with poly(sodium‐4‐styrenesulfonate) on a platinum plate. The best working conditions of the polyaniline–polypyrrole–poly(sodium‐4‐styrenesulfonate) film were determined. The glucose oxidase enzyme was immobilized by the entrapment method in polyaniline–polypyrrole–poly(sodium‐4‐styrenesulfonate) film. Glucose determination was made based on the oxidation of hydrogen peroxide, which is formed as a result of the enzymatic reaction on the surface of the prepared biosensor at +0.40 V. The working range for the glucose determination of the biosensor was determined. The effects of pH and temperature on the response of the glucose biosensor were investigated. The reusability and shelf life of the biosensor were determined. The effects of interference in biological environments on the response of the biosensor were investigated. Glucose determination was made in the biological fluid (blood) with the prepared biosensor. This study has a feature that sheds light on biosensor studies to be developed for the detection of substances in the human body, such as glucose, uric acid, and urea. This article will set an example for future scientific research on the development of a sensor for other biological fluids in the human body, such as the sensor developed for blood samples. In addition, this developed sensor provides an innovation that improves the quality of life of patients by allowing them to constantly monitor their glucose levels and intervene when necessary.