bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Tag‐Free Platform for Synthesis and Screening of Cyclic Peptide Libraries
Authors: Bruce Angele , Adebomi Victor , Czabala Patrick , Palmer Jonathan , McFadden William M. , Lorson Zachary C. , Slack Ryan L. , Bhardwaj Gaurav , Sarafianos Stefan G. , Raj Monika 
Published: March 2024

AbstractIn the realm of high‐throughput screening (HTS), macrocyclic peptide libraries traditionally necessitate decoding tags, essential for both library synthesis and identifying hit peptide sequences post‐screening. Our innovation introduces a tag‐free technology platform for synthesizing cyclic peptide libraries in solution and facilitates screening against biological targets to identify peptide binders through unconventional intramolecular CyClick and DeClick chemistries (CCDC) discovered through our research. This combination allows for the synthesis of diverse cyclic peptide libraries, the incorporation of various amino acids, and facile linearization and decoding of cyclic peptide binder sequences. Our sensitivity‐enhancing derivatization method, utilized in tandem with nano LC‐MS/MS, enables the sequencing of peptides even at exceedingly low picomolar concentrations. Employing our technology platform, we have successfully unearthed novel cyclic peptide binders against a monoclonal antibody and the first cyclic peptide binder of HIV capsid protein responsible for viral infections as validated by microscale thermal shift assays (TSA), biolayer interferometry (BLI) and functional assays.
Strukturrevision einer weit verbreiteten marinen Sulfonolipidklasse basierend auf deren Isolierung und Totalsynthese
Authors: Roman Dávid , Meisinger Philippe , Guillonneau Richard , Peng Chia‐Chi , Peltner Lukas K. , Jordan Paul M. , Haensch Veit , Götze Sebastian , Werz Oliver , Hertweck Christian , Chen Yin , Beemelmanns Christine 
Published: March 2024

AbstractBakterien der marinen Roseobacter‐Gruppe spielen eine wichtige Rolle in globalen biogeochemischen Prozessen. Prominente Vetreter dieser Gruppe produzieren schwefelhaltige Aminolipide (SAL), die für die Bildung von Biofilmen und die Besiedlung von Meeresoberflächen von entscheidender Bedeutung sind. Obwohl Genome Mining‐Ansätze und massenspektrometrische Studien homotaurinhaltige Strukturen für eine Gruppe von SALs postulierten, blieben deren relative und absolute Strukturen bisher unbekannt, was biochemische und funktionelle Untersuchungen behinderte. In dieser Studie konnten wir die absoluten Strukturen durch eine Kombination von analytischen Techniken, Isolierungs‐ und Abbauexperimenten sowie Totalsynthese bestimmen. Im Gegensatz zu vorherigen Strukturvorschlägen sind die hier untersuchten Aminolipide durch eine ungewöhnliche N,O‐acylierte Cysteinolsäure Kopfgruppe gekennzeichnet, weshalb wir die Substanzklasse Cysteinolide genannt haben. Durch gezielte Netzwerk‐basierende metabolomische Studien konnten wir zudem die Verteilung und strukturelle Vielfalt von Cysteinoliden in verschiedenee Vertretern der bakteriellen Roseobacter‐Gruppe kartieren. Insgesamt konnten in dieser Studie 14 verschiedene Aminolipide, einschließlich der in dieser Studie isolierten Cysteinolide, synthetisiert werden. Der Vergleich der erhaltenen analytischen Daten ermöglichte tiefergehende strukturelle Einblicke in die Charakteristika diese Substanzgruppe, welche für Studien zum bakteriellen Sulfonolipid‐Stoffwechsel und zu biogeochemischen Nährstoffkreislauf in den Ozeanen von großer Bedeutung sein werden.
Two‐Orders‐of‐Magnitude Enhancement of Photoinitiation Activity via a Simple Surface Engineering of Metal Nanoclusters
Authors: Tang Jin , Xu Ning , Ren An , Ma Liang , Xu Wenwu , Han Zhongkang , Chen Zijie , Li Qi 
Published: March 2024

AbstractDevelopment of high‐performance photoinitiator is the key to enhance the printing speed, structure resolution and product quality in 3D laser printing. Here, to improve the printing efficiency of 3D laser nanoprinting, we investigate the underlying photochemistry of gold and silver nanocluster initiators under multiphoton laser excitation. Experimental results and DFT calculations reveal the high cleavage probability of the surface S−C bonds in gold and silver nanoclusters which generate multiple radicals. Based on this understanding, we design several alkyl‐thiolated gold nanoclusters and achieve a more than two‐orders‐of‐magnitude enhancement of photoinitiation activity, as well as a significant improvement in printing resolution and fabrication window. Overall, this work for the first time unveils the detailed radical formation pathways of gold and silver nanoclusters under multiphoton activation and substantially improves their photoinitiation sensitivity via surface engineering, which pushes the limit of the printing efficiency of 3D laser lithography.
Achieving Efficient Dark Blue Room‐Temperature Phosphorescence with Ultra‐Wide Range Tunable‐Lifetime
Authors: Zhou Lei , Song Jinming , He Zhenyi , Liu Yiwei , Jiang Ping , Li Tao , Ma Xiang 
Published: March 2024

AbstractTunable‐lifetime room‐temperature phosphorescence (RTP) materials have been widely studied due to their broad applications. However, only few reports have achieved wide‐range lifetime modulation. In this work, ultra‐wide range tunable‐lifetime efficient dark blue RTP materials were realized by doping methyl benzoate derivatives into polyvinyl alcohol (PVA) matrix. The phosphorescence lifetimes of the doped films can be increased from 32.8 ms to 1925.8 ms. Such wide range of phosphorescence lifetime modulation is extremely rare in current reports. Moreover, the phosphorescence emission of the methyl 4‐hydroxybenzoate‐doped film is located in the dark blue region and the phosphorescence quantum yield reaches as high as 15.4 %, which broadens their applications in organic optoelectronic information. Further studies demonstrated that the reason for the tunable lifetime was that the magnitude of the electron‐donating ability of the substituent group modulates the HOMO–LUMO and singlet‐triplet energy gap of methyl benzoate derivatives, as well as the ability to non‐covalent interactions with PVA. Moreover, the potential applications of luminescent displays and optical anti‐counterfeiting of these high‐performance dark blue RTP materials have been conducted.
A Lipopeptidomimetic of Transcriptional Activation Domains Selectively Disrupts the Coactivator Med25 Protein–Protein Interactions
Authors: Pattelli Olivia N. , Valdivia Estefanía Martínez , Beyersdorf Matthew S. , Regan Clint S. , Rivas Mónica , Hebert Katherine A. , Merajver Sofia D. , Cierpicki Tomasz , Mapp Anna K. 
Published: March 2024

AbstractShort amphipathic peptides are capable of binding to transcriptional coactivators, often targeting the same binding surfaces as native transcriptional activation domains. However, they do so with modest affinity and generally poor selectivity, limiting their utility as synthetic modulators. Here we show that incorporation of a medium‐chain, branched fatty acid to the N‐terminus of one such heptameric lipopeptidomimetic (LPPM‐8) increases the affinity for the coactivator Med25 >20‐fold (Ki >100 μM to 4 μM), rendering it an effective inhibitor of Med25 protein–protein interactions (PPIs). The lipid structure, the peptide sequence, and the C‐terminal functionalization of the lipopeptidomimetic each influence the structural propensity of LPPM‐8 and its effectiveness as an inhibitor. LPPM‐8 engages Med25 through interaction with the H2 face of its activator interaction domain and in doing so stabilizes full‐length protein in the cellular proteome. Further, genes regulated by Med25‐activator PPIs are inhibited in a cell model of triple‐negative breast cancer. Thus, LPPM‐8 is a useful tool for studying Med25 and mediator complex biology and the results indicate that lipopeptidomimetics may be a robust source of inhibitors for activator‐coactivator complexes.
Gold(I)‐Catalyzed Intramolecular 7‐endo‐dig Cyclization of Triene‐Yne Systems: New Access towards Azulenothiophenes
Authors: Eshagh Saatlo Rebeka , Oczlon Julian , Wunsch Jonas F. , Rudolph Matthias , Rominger Frank , Oeser Thomas , Shiri Farshad , Ariafard Alireza , Hashmi A. Stephen K. 
Published: March 2024

AbstractWe report the direct synthesis of new azulene derivatives through gold‐catalyzed cyclization reactions. A five‐membered ring as backbone in the applied triene‐yne substrates turned out to be crucial to induce the 7‐endo‐dig cyclization mode necessary to trigger azulene formation. The obtained targets are of high interest due to their potential applications in different fields, like organic materials, medicine or cosmetics. UV/Vis spectra and cyclic voltammetry were measured, based on these the electronic properties were determined. Short two or three step sequences towards the applied starting materials make this approach synthetically highly attractive.
A novel method for the synthesis of solvent‐free and high‐solid‐content waterborne polyurethanes by introducing a small amount of polyethylene glycol
Authors: Hsu Kuei Ting , You Jhu‐Lin 
Published: March 2024

AbstractIn the study, the synthesis process involved the reaction of dimethylolbutyric acid and polytetramethylene ether glycol 1000 (PTMG1000) with hexamethylene diisocyanate (H12MDI), taking advantage of their mutual dissolution at high temperatures. The chain‐extension reaction with 1,4‐butanediol (BDO) was successfully conducted without the use of organic solvents. The emulsification reaction was carried out using the polyurethane prepolymer at 60% solids content, along with aqueous dispersions of polyethylene glycol (PEG) with varying molecular weights and amounts as interfacially active agents. Fourier transform infrared spectroscopy analysis suggested potential hydrogen bonding interactions between the PEG molecular chain and the polyurethane chain. Rheometer analysis demonstrated a significant reduction in viscosity with the addition of 1–5 wt.% PEG, accompanied by an increase in average particle size. This phenomenon was attributed to the formation of a hydrophilic lubrication layer of PEG around the water‐based polyurethane (WPU) microcells. Among them, WPU films containing 4 wt.% PEG4000 not only exhibited soft properties with a mechanical elongation rate exceeding 2000% but also showed excellent storage stability. The addition of long‐chain PEG facilitated the formation of a lubrication layer between the microcells, contributing to spatial stabilization and reducing particle aggregation at high solids content. It is noteworthy that this solvent‐free process, without any organic solvents, together with the adjusted PEG content, successfully synthesized waterborne polyurethanes with low viscosity and high solids content. This provides a new sustainable and environmentally friendly method for the future production of waterborne polyurethanes.
Optimization of synthesis parameters of PUF/ENB microcapsules for self‐healing applications using factorial design methodology
Authors: de Carvalho Freire Maria Paula , da Silva Gabriel Agostinho , Pereira de Paula Ygor Matheus , Marini Juliano , Melo José Daniel Diniz , Costa Maria Carolina Burgos 
Published: March 2024

AbstractThis study introduces a systematic experimental approach aimed at enhancing the production process of poly(urea‐formaldehyde) (PUF) microcapsules filled with 5‐ethylidene‐2‐norbonene (ENB) using in situ emulsion polymerization. Essential parameters were identified through a prior Plackett Burman (PB) design, leading to the implementation of a 24‐1 fractional factorial design. The key parameters selected encompassed stirring speed, poly(ethylene‐alt‐maleic anhydride) (EMA) emulsifier content, pH of the reaction, and the quantity of 1‐octanol. Optimal conditions for polymeric microcapsule synthesis were determined using a statistical analysis of the complete factorial design, facilitating the development of representative mathematical models for the process. A comprehensive evaluation of response variables including microcapsule diameter, yield, encapsulated content, stability, and thermal degradation was conducted. Utilizing response surface analysis (RSM), it was determined that the PUF/ENB(2C) condition (stirring at 700 rpm, a reaction pH of 3.0, and EMA content of 0.425 g) resides within the optimized synthesis region, producing microcapsules exhibiting favorable morphological characteristics, yield of 52% and encapsulated content of 80%.
Complexities and opportunities: A review of the trajectory of fish farming in Zimbabwe
Authors: Mabika Nyasha , Utete Beaven 
Published: March 2024

AbstractZimbabwe is currently rated as one of the top 10 fish producers in Sub‐Saharan Africa. Fish farming in Zimbabwe is dominated by the culture of Nile tilapia (Oreochromis niloticus) followed by rainbow trout (Oncorhynchus mykiss). Over 90% of the cultured fish isO. niloticus,which comes from Lake Kariba. Since the first decade of the 21stcentury, there has been a significant increase in fish production from two tons to eight tons annually. The increase in fish production has been attributed to the government and donor‐funded fishery programs. In this review, current practices, opportunities, and challenges for aquaculture in Zimbabwe are highlighted. The current practices include intensive, semi‐intensive, and extensive aquaculture systems. Consistent high market demand for fish and numerous water bodies with potential for cage culture are some of the drivers for aquaculture. Despite the industry's significant growth, there are still a number of management and production issues that need to be resolved. Weaknesses in structural issues and operational frameworks in Non‐Governmental Organizations, lack of credit facilities, subsidies, limited technology, obfuscated governance, weak fish disease surveillance mechanisms and legal frameworks, and constrained human resources capacity are some of the challenges plaguing fish culture in Zimbabwe. Cogent aquaculture policies, sustainable subsidies, intensive training of human resources and fisheries experts, strengthened disease surveillance, cheaper alternative fish feeds, reliable viable fingerling production, concerted value chain efforts, and exploration of lucrative export markets is a panacea for the fledgling aquaculture industry in Zimbabwe.
An underlying factor of increasing early winter precipitation in the Hokuriku region of Japan in recent decades
Authors: Takemura Kazuto , Maeda Shuhei , Kawamura Ryuichi 
Published: March 2024

AbstractUsing a reanalysis dataset and large‐ensemble simulation results, this study examines a possible factor of increasing trend in early winter precipitation in recent decades in the Hokuriku region of Japan. Monthly precipitation in December has a significant increasing trend after the early 1990s, which is different from those in January and February. The increasing precipitation in December is related to that in the sea surface upward latent heat flux due to intensified winter monsoon circulation and warming sea surface temperatures (SSTs) over the Sea of Japan. December averaged SSTs show a trend pattern in recent decades that is similar to the negative phase of the interdecadal Pacific oscillation (IPO), accompanied by positive trends from the eastern Indian Ocean to the western tropical Pacific. The enhanced trend of convection over the Bay of Bengal is seen; suggesting a combined effect of climatologically high SSTs and IPO‐related warmed SSTs over the region. Trends in recent decades of an upper‐level wavy pattern from South Asia to near Japan along the subtropical jet associated with enhanced convection near the Bay of Bengal and the related pressure drop from Japan to the north are seen, which contribute to intensified winter monsoon circulation.
May the Intentional Candidate Win: The Effect of Global Performance Information on Intentionality Attributions and Managerial Hot‐Hand Predictions
Authors: Braga João Niza , Jacinto Sofia 
Published: March 2024

ABSTRACTIn organizational contexts, managers often have to judge and predict others' performance. Previous research has consistently shown that when predicting someone's performance, people expect that a local sequence of successful outcomes will continue—the hot‐hand. The present work proposes that hot‐hand predictions occur when local streaks are dispositionally attributed to the agents' intentionality and explores how the inclusion of global performance success rates may guide intentionality inferences and moderate predictions of success after a streak. Three studies, using within‐ and between‐subjects' designs, manipulate agent's global success rate and show that after a local streak, intentionality attributions and predictions of success are lower when success rates are low (vs. high or unknown); intentionality attributions mediate the effect of success rate on predictions; hot‐hand predictions are lower for low success rate agents (vs. high or unknown) as they are not perceived as more responsible for streaky than for alternated performances.
Development of synthetic small regulatory RNA for Rhodococcus erythropolis
Authors: Wang Lijuan , Hou Jie , Yang Kun , Yu Haonan , Zhang Bo , Liu Zhiqiang , Zheng Yuguo 
Published: March 2024

AbstractRhodococci have been regarded as ideal chassis for biotransformation, biodegradation, and biosynthesis for their unique environmental persistence and robustness. However, most species of Rhodococcus are still difficult to metabolically engineer due to the lack of genetic tools and techniques. In this study, synthetic sRNA strategy was exploited for gene repression in R. erythropolis XP. The synthetic sRNA based on the RhlS scaffold from Pseudomonas aeruginosa functions better in repressing sfgfp expression than those based on E. coli MicC, SgrS, and P. aeruginosa PrrF1‐2 scaffold. The RhlS‐based sRNAs were applied to study the influence of sulfur metabolism on biodesulfurization (BDS) efficiency in R. erythropolis XP and successfully identified two genes involved in sulfur metabolism that affect the BDS efficiency significantly. The RhlS‐based synthetic sRNAs show promise in the metabolic engineering of Rhodococcus and promote the industrial applications of Rhodococcus in environmental remediation and biosynthesis.
Characterization of cellular responses and cell lysis to elevated hydrodynamic stress from benchtop perfusion bioreactors
Authors: Zhang Weijian , Ran Qingyuan , Zhao Liang , Ye Qian , Tan Wen‐Song 
Published: March 2024

AbstractThe effective design of perfusion cell culture is currently challenging regarding balancing the operating parameters associated with the hydrodynamic conditions due to increased system complexity. To address this issue, cellular responses of an industrial CHO cell line to different types of hydrodynamic stress in benchtop perfusion bioreactors originating from agitation, sparging, and hollow fibers (HF) in the cell retention devices were systematically investigated here with the analysis of cell lysis. It was found that cell lysis was very common and most associated with the sparging stress, followed by the HF and lastly the agitation, consequently heavily impacting the estimation of process descriptors related to biomass. The results indicated that the agitation stress led to a reduced cell growth with a shift toward a more productive phenotype, suggesting an energy redirection from biomass formation to product synthesis, whereas the sparging stress had a small impact on the intracellular metabolic flux distribution but increased the cell death rate drastically. For HF stress, a similar cell maintenance profile was found as the sparging while the activity of glycolysis and the TCA cycle was significantly impeded, potentially leading to the lack of energy and thus a substantial decrease in cell‐specific productivity. Moreover, a novel concept of volume average shear stress was developed to further understand the relations of different types of stress and the observed responses for an improved insight for the perfusion cell culture.
One‐Pot Reactions in Different Sites: A New Approach in Hydroformylation‐Based Processes
Authors: Delolo Fábio G. , dos Santos Eduardo N. , Gusevskaya Elena V. 
Published: March 2024

AbstractOne‐pot synthetic procedures allow multiple chemical transformations circumventing the isolation of intermediates and thus saving time, energy and feedstocks. Within the scope of one‐pot processes, cascade, domino, or tandem procedures are even more efficient, as multiple reactions can occur in parallel. Hydroformylation is an industrially relevant reaction particularly suitable for this kind of methodology, as the primary products (aldehydes) are usually converted into compounds containing other functionalities. In addition to examples of transformations of the substrate before the hydroformylation step or the transformation of the aldehyde into other functionalities, we highlight a novel approach, in which an additional functionalization takes place in a remote site of the substrate molecule, along with the hydroformylation of the carbon‐carbon double bond.
Atomically Dispersed Metal‐Nitrogen‐Carbon Electrocatalysts for the Oxygen Reduction Reaction
Authors: Lu Jiajia , Deng Peng‐Jun , Fu Gaoliang , Meng Xiangyu , Zhang Shouren , Yang Baocheng 
Published: March 2024

AbstractThe quest for alternatives to Pt as an oxygen reduction electrocatalyst, possessing high activity, stability, and abundant reserves, holds great significance for H2/O2 fuel cells. Recently, metal‐nitrogen‐carbon (M‐N‐C) electrocatalysts have garnered substantial attention as promising substitutes. These electrocatalysts not only exhibit well‐defined structures but also offer the flexibility to adjust the central metal atoms and coordination atoms. It is beneficial in elucidating the active sites during the catalytic process and in the design of highly active electrocatalysts. In this review, the real active site of M‐N‐C electrocatalyst‐driven ORR is investigated in depth by in situ characterization techniques such as X‐ray absorption spectroscopy, Raman spectroscopy, Fourier‐transform infrared spectroscopy. It′s worth noting that the catalytic activity of M‐N‐C electrocatalysts originates from the dynamic evolution of electrocatalyst structure. Subsequently, we review various synthetic strategies, including the wet chemistry method, spatial confinement, and template‐assisted method, aimed at the rational design of M‐N‐C electrocatalysts. Moreover, recent progresses of M‐N‐C electrocatalysts with varying configurations, encompassing single‐atom, and double‐atom electrocatalysts are discussed, Finally, summary and perspectives on the development of M‐N‐C are provided.
Surface‐Enhanced Raman Scattering Using 2D Materials
Authors: Pinto de Sousa Beatriz , Fateixa Sara , Trindade Tito 
Published: March 2024

AbstractThe use of surface‐enhanced Raman scattering (SERS) as a technique for detecting small amounts of (bio)chemical analytes has become increasingly popular in various fields. While gold and silver nanostructures have been extensively studied as SERS substrates, the availability of other types of substrates is currently expanding the applications of this spectroscopic method. Recently, researchers have begun exploring two‐dimensional (2D) materials (e. g., graphene‐like nanostructures) as substrates for SERS analysis. These materials offer unique optical properties, a well‐defined structure, and the ability to modify their surface chemistry. As a contribution to advance this field, this concept article highlights the significance of understanding the chemical mechanism that underlies the experimental Raman spectra of chemisorbed molecules onto 2D materials’ surfaces. Therefore, the article discusses recent advancements in fabricating substrates using 2D layered materials and the synergic effects of using their metallic composites for SERS applications. Additionally, it provides a new perspective on using Raman imaging in developing 2D materials as analytical platforms for Raman spectroscopy, an exciting emerging research area with significant potential.